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The characteristic feature of a biofunctional system is that components with various functions work together. These multi-components are not simply mixed together, but are rationally arranged. The fundamental technologies to do this in an artificial system include the synthetic chemistry of the substances that make the component unit, the science and techniques for assembling them, and the technology for analyzing their nanoostructures. A new concept, nanoarchitectonics, can play this role. Nanoarchitectonics is a post-nanotechnology concept that involves building functional materials that reflect the nanostructures. In particular, the approach of combining and building multiple types of components to create composite materials is an area where nanoarchitectonics can be a powerful tool. This review summarizes such examples and related composite studies. In particular, examples are presented in the areas of catalyst & photocatalyst, energy, sensing & environment, bio & medical, and various other functions and applications to illustrate the potential for a wide range of applications. In order to show the various stages of development, the examples are not only state-of-the-art, but also include those that are successful developments of existing research. Finally, a summary of the examples and a brief discussion of future challenges in nanoarchitectonics will be given. Nanoarchitectonics is applicable to all materials and aims to establish the ultimate methodology of materials science.
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REVIEW
Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
https://doi.org/10.1007/s10904-024-03065-9
vectorially. This is a highly evolved form of functional
material system. It can also regarded as a highly organized
composite system. The goal of material chemistry for func-
tional materials is to construct such material systems.
Highly functional composites should not be merely
mixed with ingredients. It is organized with extreme preci-
sion. The fundamental technologies to do this in an articial
system include the synthetic chemistry of the substances
that make the component units, the science and techniques
for assembling them, and the technology for analysing their
nanostructures. Humanity has developed those elemental
technologies. Organic chemistry [48], inorganic chemistry
[913], coordination chemistry [1418], polymer chemistry
[1923], material chemistry [2428], and biochemistry [29
33] are still being developed as creating units or substances.
Methodologies such as self-assembly by supramolecular
chemistry [3437] are used to bring them in organization.
Thin lm technologies such as self-assembled monolayer
(SAM) [3842], Langmuir-Blodgett (LB) method [4347],
layer-by-layer (LbL) assembly [4852] are also used. Syn-
thesis of ordered porous materials such as metal-organic
1 Introduction
Biological systems that has a highly sophisticated structures
and perform ecient and highly selective functions can be
said to be the ultimate forms of functional material systems.
The characteristic feature of a bio-functional system is that
components with various functions work together [13].
These multi-components are not simply mixed together, but
are rationally arranged. Their organizational structures are
hierarchical and asymmetrical. Accordingly, material and
information transformations are performed continuously
and sequentially. Energies are integrated and electrons ow
Katsuhiko Ariga
ARIGA.Katsuhiko@nims.go.jp
1 Research Center for Materials Nanoarchitectonics (MANA),
National Institute for Materials Science (NIMS), 1-1 Namiki,
Tsukuba 305-0044, Ibaraki, Japan
2 Graduate School of Frontier Sciences, The University of
Tokyo, 5-1-5 Kashiwanoha, Kashiwa 277-8561, Chiba, Japan
Abstract
The characteristic feature of a biofunctional system is that components with various functions work together. These
multi-components are not simply mixed together, but are rationally arranged. The fundamental technologies to do this in
an articial system include the synthetic chemistry of the substances that make the component unit, the science and tech-
niques for assembling them, and the technology for analyzing their nanoostructures. A new concept, nanoarchitectonics,
can play this role. Nanoarchitectonics is a post-nanotechnology concept that involves building functional materials that
reect the nanostructures. In particular, the approach of combining and building multiple types of components to create
composite materials is an area where nanoarchitectonics can be a powerful tool. This review summarizes such examples
and related composite studies. In particular, examples are presented in the areas of catalyst & photocatalyst, energy,
sensing & environment, bio & medical, and various other functions and applications to illustrate the potential for a wide
range of applications. In order to show the various stages of development, the examples are not only state-of-the-art, but
also include those that are successful developments of existing research. Finally, a summary of the examples and a brief
discussion of future challenges in nanoarchitectonics will be given. Nanoarchitectonics is applicable to all materials and
aims to establish the ultimate methodology of materials science.
Keywords Nanoarchitectonics · Composite · Energy · Environmental · Biomedical
Received: 4 March 2024 / Accepted: 6 March 2024 / Published online: 16 April 2024
© The Author(s) 2024
Composite Nanoarchitectonics Towards Method for Everything in
Materials Science
KatsuhikoAriga1,2
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
frameworks (MOFs) [5357], covalent organic frameworks
(COFs) [5862], mesoporous materials [6367] is also
useful. Not limited to these typical materials forms, vari-
ous integrated structures are used for advanced functions
including sensors [6872], devices [7377], batteries [78
82], fuel cells [8387], solar cells [8892], supercapaci-
tors [9397], and so on. Engineering fabrication techniques
such as lithography also have a wide range of applications
[98102]. Even more important is the technology to anal-
yse nanostructures. An important contribution is made by
a series of technologies featured in nanotechnology [103
105]. These include structural observation at the atomic and
molecular level [106109], manipulation [110113], and
evaluation [114117] of physical properties at the nano-
scopic level. Integrating all of these technologies to create
materials is essential for constructing advanced functional
material systems.
A new concept, nanoarchitectonics, can play this role
(Fig. 1) [116121]. Nanoarchitectonics can be considered as
post-nanotechnology [122, 123]. Just as Richard Feynman
initiated nanotechnology in the mid-20th century [124, 125],
Masakazu Aono proposed nanoarchitectonics in the early
21st century [126, 127]. Nanoarchitectonics is an interdis-
ciplinary concept rather than an entirely new concept. It has
the role of developing a group of functional materials that
rationally reect the nanostructure by integrating the exist-
ing material science with the nanoscale science/technology
of nanotechnology. The functional material system will be
built from units such as atoms, molecules, and nanomateri-
als, taking advantage of the characteristics of nanostructures
[128, 129]. The process uses elements such as atomic and
molecular manipulation, physical and chemical material
transformation, self-assembly/self-organization, alignment
and organization by external elds and actions, biochemical
processes, and nano and micro fabrication techniques [130].
These elemental technologies are selected and combined to
architect materials from nano.
This methodology is widely applied regardless of the
material used or its intended application. For example,
recent papers advocating nanoarchitectonics can be found
in a wide range of elds. In addition to application-oriented
areas such as catalysis [131135], sensors [136140],
devices [141145], energy production [146150], energy
storage [151155], environmental response [156160],
drug delivery [161165], and biomedical applications
[166170], there are also fundamental areas such as mate-
rial synthesis [171176], structural control [177181], the
exploration of physical phenomena [182186], relatively
basic biochemical studies [187191], and research on cel-
lular interactions [192196]. Since all matter is principally
composed of atoms and molecules, the methodology of
building matter from atoms and molecules is applicable to
all material synthesis. It could be likened to the ultimate the-
ory of everything in physics [197], and nanoarchitectonics
could be called a method for everything in materials science
[198, 199]. This concept of nanoarchitectonics, which is
applicable to all materials, is more suitable for the construc-
tion of multi-component functional material systems such
as composites.
Now, the ideal functional material is to create complex
composites like biological systems. To achieve advanced
functionality, the components must be rationally organized,
rather than simply a collection of functional molecular units.
Their structure is asymmetric and hierarchical. The process
ows accordingly in a continuous and directional manner.
In assembling such hierarchical structures, nanoarchitecton-
ics has advantages [200]. In nanoarchitectonics, materials
are built by combining several unit processes. Therefore,
Fig. 1 Outline of nanoarchitec-
tonics concept: meaning and
procedure
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
nanoarchitectonics approaches easily create hierarchical
structures than self-assembly by simple equilibrium pro-
cesses [201]. It also has an aptitude for incorporating mul-
tiple components. Another feature is the harmonization of
actions. It is nano interactions that are the origin of nano-
architectonics. There is a degree of uncertainty involved
[202]. In the nano processes of nanoarchitectonics, uncer-
tainties such as thermal uctuations, stochastic distribu-
tions, and quantum eects can be included. Thus, many
eects will not simply add up, but will work in a jointly har-
monized manner [203]. This is similar to what happens in
bio-functional research, where many eects harmonize with
each other to achieve advanced functionality. If the goal is
to develop highly functionalized composite materials, it is
necessary to incorporate such harmonization of actions.
Combining the concept of nanoarchitectonics with multi-
component composites can lead to the architecture of highly
advanced functional material systems, such as those found
in biological systems. The concept of composite nanoar-
chitectonics is a long way from perfection, but there have
been several reports that provide the beginnings of the con-
cept. This review illustrates the reported nanoarchitectonics
research on composites and some related functional com-
posite materials. To show the wide range of applications and
potential, recent examples are categorized as (i) catalyst &
photocatalyst, (ii) energy, (iii) sensing & environment, (iv)
bio & medical, and (v) various other functions and applica-
tions. In order to show the various stages of development,
the examples are not only state-of-the-art, but also include
those that are successful developments of existing research.
Finally, a summary of the examples and a brief discussion
of future challenges in nanoarchitectonics will be given.
Nanoarchitectonics is applicable to all materials and aims
to establish the ultimate methodology of materials science.
2 Catalyst & Photocatalyst
Various functions require the fullment of several necessary
elements. To satisfy these elements, nanoarchitectonics,
which is a composite of two dierent materials, is eective.
For example, a catalytic function requires two elements: the
ability to promote reactions and the structural selectivity of
substrates and products. As one that satises such properties,
Fujiwara reported on an active catalyst for the production of
aromatic hydrocarbons by CO2 hydrogenation [204]. In this
catalyst, a composite catalyst consisting of Fe-Zn oxide and
a zeolite, H-ZSM-5, was used. This composite catalyst is
very eective for the selective formation of aromatic hydro-
carbons. The narrow pore size of the zeolite H-ZSM-5 pro-
vides excellent geometry selectivity of the reaction, which
was also achieved in the methanol-hydrocarbon reaction of
CO2 hydrogenation. Such catalytic technology will contrib-
ute to carbon recycling. This will be a necessary technology
to realize a sustainable low-carbon society.
Shimakoshi and co-workers nanoarchitectonized high-
performance visible light-driven hybrid catalysts from vita-
min B12 complexes derived from natural vitamin B12, earth
metal ions, and titanium dioxide (Fig. 2) [205]. First, metal
ions (Cu2+, Ni2+, Fe2+, Zn2+, Mn2+, Al3+, Mg2+, etc.) were
modied on the TiO2 surface. This resulted in an eective
response to visible light. Furthermore, vitamin B12 com-
plexes were loaded on the surface. In this way, the nano-
architectonically modied catalyst can promote visible
light-driven reactions without the use of precious rhodium.
In particular, B12-Mg2+/TiO2 showed the highest catalytic
activity among the prepared samples. This is because elec-
tron transfer to the B12 complex occurs eciently because
no electron transfer to the modied magnesium side occurs.
It was also shown that useful chemical products, N,N-
diethyl-3-methylbenzeamide and N,N-diethylformamide,
can be prepared in high yield under visible light irradia-
tion. Such performance is useful for ne chemical synthesis
using sustainable solar energy.
Fig. 2 Hybrid catalysts from
vitamin B12 complexes derived
from natural vitamin B12, earth
metal ions, and titanium dioxide
that can promote visible light-
driven reactions. Reproduced
with permission from Ref. [205].
Copyright 2022 Oxford Univer-
sity Press
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electrostatic energy storage in modern electronic and electri-
cal systems. Although nanoarchitectonics approaches with
polymer nanocomposites have been used to improve per-
formance, they have the drawbacks of reduced energy den-
sity and lower discharge eciency at temperatures above
150 °C. Creating ultra-small inorganic clusters, as in this
study, can introduce richer and deeper traps into composite
dielectrics compared to conventional polymer/nanoparticle
blends. Due to this eect, high-temperature capacitance
performance was achieved up to 200 °C. Such composite
nanoarchitectonics of polymer/inorganic clusters is useful
for high-temperature dielectric energy storage in practi-
cal applications of power devices and electronic devices.
Combined with the synthetic advantages of inexpensive
precursors and one-pot synthesis, this could be a promising
method for tuning the high-temperature capacitance perfor-
mance of polymeric dielectrics.
The development of multifunctional electrode materials
is an important approach for practical applications in energy
storage and conversion devices. For example, the construc-
tion of composite materials based on metal-organic frame
work (MOF) is considered a promising strategy. It is impor-
tant to improve the conductivity of MOF materials through
a rational nanoarchitectonics approach. Jiao, Chen, and co-
workers have created composites of iron-based MOFs and
ultra-thin Co(OH)2 nanosheets by in situ hydrothermal strat-
egies (Fig. 3) [209]. This created a hollow, interconnected
porous network structure. Structural and morphological
analysis conrms that the Co(OH)2 nanosheets are uni-
formly anchored on the Fe-based MOF, forming a hollow
composite. A large specic surface area with a hierarchical
porous structure is provided for electrolyte storage. There-
fore, the diusion of ions is promoted, and the reaction rate
of the active material is greatly improved. The hollow struc-
ture can expose more active surfaces. The enhanced electro-
lyte penetration may improve the utilization of iron-based
MOFs. The composite materials developed in this study
showed excellent performance in both supercapacitors and
oxygen evolution reaction. Such nanoarchitectonized com-
posite materials can be used in electrode materials with
excellent performance. They also have great potential for
development in the eld of electrochemistry. It will provide
inspiration for future energy storage and conversion device
designs.
Wu, Gong, and co-workers have shown how black phos-
phorus quantum dots can be eciently used in lithium bat-
teries under the concept of composite nanoarchitectonics for
ecient lithium storage [210]. In this study, the goal is to
obtain high energy density while improving stability. Black
phosphorus quantum dots were co-precipitated into pores
matching the size of the cobalt/iron Prussian blue analogues
of MOFs. The composite nanoarchitectonics was achieved
Hakamy, Abd-Elnaiem, and co-workers reported on
nanoarchitectonics of nickel dimethylglyoxime/γ-alumina
composites [206]. In this approach, nickel dimethylglyox-
ime is synthesized on γ-alumina, which is used as a catalyst,
using a direct impregnation method. Using this catalyst, the
photocatalytic degradation performance for methylene blue
and methyl orange was investigated. The photodegradation
performance of these dyes was signicantly enhanced by
compositing, and the Ni microcrystals or Ni nanospheres on
the γ-alumina support were analysed as being distributed in
a single phase and/or in a homogeneous manner. This sup-
port structure enhanced thermal stability and photocatalytic
degradation of dyes. In particular, the nanosized form of the
γ-alumina catalyst, with its large surface area, is useful for
a variety of applications. It may also be suitable for degra-
dation of other dyes. Furthermore, the nanoarchitectonized
composite would be suitable for a variety of applications,
such as sensing, in addition to catalytic applications.
Abd-Elnaiem et al. reported on graphene oxide-based
composite photocatalysts under the concept of compos-
ite nanoarchitectonics of graphene oxide [207]. Graphene
oxide-bound Au and ZnO nanocomposites were synthesized
by a modied Hummers method and an ultrasound-assisted
solution method. Photocatalytic degradation of methylene
blue was investigated under simulated visible-ultraviolet
light irradiation. Porous graphene oxide nanoparticles
showed the greatest eciency and performance in photo-
degradation. For example, the photocatalytic eciency for
the removal of methylene blue from wastewater reached
97% for the porous graphene oxide nanoparticle catalyst.
The best t for the photocatalytic degradation mechanism
was adsorption by an intraparticle diusion kinetics model.
The use of such composite catalysts for the purication of
organic dyes is of interest from economic, safety, and envi-
ronmental perspectives.
3 Energy
Exquisite composite nanoarchitectonics of various compo-
nents can improve material performance. This methodology
has also come in handy for energy-related applications. Li
and co-workers have prepared polymer/metal oxide clus-
ter composites based on a site-isolation strategy [208].
This co-polymerization strategy allows the preparation of
polymer/inorganic cluster composites with ultrasmall-sized
inorganic phases. The maximum probable diameter of the
nanoarchitectonized aluminium oxide clusters is 2.2 nm.
This technique does not require an auxiliary dispersion
step. Nevertheless, the clusters are uniformly dispersed in
the polymer matrix. As background, polymer dielectrics
need to operate at high temperatures to meet the demands of
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
composite materials. As a result, this could serve as a guide-
line for developing lithium batteries with higher capacity
density and cycle stability.
Nickel-rich layered oxides are widely used as cathode
materials in energy-dense lithium-ion batteries. However,
these chemistries, based on the parent compound LiNiO2,
are known to be very sensitive to the ambient environ-
ment and react readily with moisture and carbon dioxide.
This characteristic leads to a signicant reduction in per-
formance. To address this issue, Hersam and co-workers
prepared LiNiO2 cathode particles with a uniform coat-
ing of a hydrophobic barrier layer composed of graphene
and ethylcellulose (Fig. 4) [211]. This hydrophobic coat-
ing reduced contact between atmospheric moisture and the
LiNiO2 surface, minimizing the generation of lithium impu-
rities. The obtained results demonstrate the breaking of the
with dierent amounts of black phosphorus quantum dots
encapsulated in the pores of the Co/Fe Prussian blue ana-
logue. The morphology and particle size of the composite
were changed without changing the crystal structure of the
MOF. The stability of the composite with black phosphorus
quantum dots was signicantly improved. Excellent electro-
chemical performance was demonstrated in lithium batter-
ies. The close contact between black phosphorus quantum
dots and Co/Fe catalyst sites promoted rapid transfer of
lithium ions between metal sites. The lithium storage capac-
ity was also increased due to the special molecular struc-
ture of black phosphorus, which forms P-N bonds. The
material developed here with black phosphorus quantum
dots in Prussian blue analogues encapsulated as electrodes
exhibited higher capacity density and longer cycle stabil-
ity than batteries using conventional Prussian blue analogue
Fig. 4 LiNiO2 (LNO) cathode
particles with a uniform coat-
ing of a hydrophobic barrier
layer composed of graphene
and ethylcellulose followed by
pyrolysis process. Reproduced
with permission from Ref.
[211]. Copyright 2023 American
Chemical Society
Fig. 3 Composites of iron-based MOFs and ultra-thin Co(OH)2
nanosheets by in situ hydrothermal strategies having a large specic
surface area with a hierarchical porous structure for electrolyte stor-
age. Reproduced with permission from Ref. [209]. Copyright 2023
Royal Society of Chemistry
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
Zn powder, poor connections due to point contacts between
particles can be avoided. Thereby improving the conductiv-
ity of the electrode. It also provides more nucleation sites
for Zn deposition. As a result, the symmetric cell exhibits
tremendous stability. The application of powder metal-
lurgy in this study provides new ideas for the preparation
of high-performance and low-cost Zn-based aqueous bat-
tery anodes. Potential applications for large-scale practical
preparation and renewable energy storage are suggested.
To achieve sucient photoelectrochemical water split-
ting performance, it is essential to improve charge sepa-
ration/transport eciency. In particular, various interface
engineering strategies to mitigate charge recombination are
essential. Zhang, Du, Lu, and co-workers demonstrated an
eective strategy that can synchronously regulate the simul-
taneous transfer of electrons and holes in dierent directions
on the photoanodes to improve photoelectrochemical per-
formance [213]. Figure 6 shows that monodisperse MXene
quantum dots were obtained by HF etching, exfoliation, and
hydrothermal treatment. Next, ZnIn2S4 nanosheet arrays
were synthesized on FTO by hydrothermal method. Then,
MXene quantum dots and α-Fe2O3 nanodots were modied
Ni-rich limit of the layered lithium transition metal oxide
family. This work establishes a scalable strategy for improv-
ing the environmental stability of Ni-rich cathode materials.
Demonstrating this approach for the ultimate nickel-rich
chemistries is likely to be generalizable to a wide range of
environmentally sensitive battery materials. In addition, it
is expected to be applicable to other related Ni-rich chem-
istries that are widely used in electric vehicles and related
energy storage technologies.
As a promising candidate for grid-scale energy storage,
Zn-based aqueous batteries have shown high potentials
due to their intrinsic safety, outstanding theoretical energy
density, and cost-eectiveness. However, a negative factor
against practical application is the performance degradation
due to dendrite formation, side reactions, and corrosion of
the anode, etc. To address this issue, Zhang, Han, and co-
workers have fabricated a new Zn matrix composite anode
with an implanted 3D carbon network by powder metal-
lurgy (Fig. 5) [212]. The internal carbon network provides a
continuous electron transfer channel. Through optimization
of the surface electric eld distribution, highly reversible
Zn deposition can be achieved. By lling the gaps in the
Fig. 6 Process for photoelectric conversion devices; monodisperse
MXene quantum dots were obtained by HF etching, exfoliation, and
hydrothermal treatment; next, ZnIn2S4 nanosheet arrays were synthe-
sized on FTO by hydrothermal method; then, MXene quantum dots
and α-Fe2O3 nanodots were modied on the ZnIn2S4 nanosheet surface
by spin-coating and solvothermal methods. Reproduced with permis-
sion from Ref. [213]. Copyright 2024 Wiley-VCH.
Fig. 5 Fabrication of a Zn matrix composite anode with an implanted 3D carbon network by powder metallurgy with the surface electric eld
distribution through highly reversible Zn deposition. Reproduced with permission from Ref. [212]. Copyright 2024 Wiley-VCH.
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
chitosan using an in situ polymer oxidation [225]. The
nanocomposites for sensor electrodes were prepared using
the in situ polymer oxidation pathway. Specically, glassy
carbon electrodes modied with polythiophene/multiwalled
carbon nanotubes, chitosan, and CuO were prepared. The
modied electrode prepared exhibited a certain range of
detection linearity and excessively yielding ion detection at
low concentrations. The high Cd(II) detection eciency of
the sensor with this modied glassy carbon electrode can be
regarded as a good success story for electrochemical sensor
applications.
Photocatalytic reduction of Hg2+ under visible light is an
important challenge. This can be improved in performance
by a composite nanoarchitectonics approach. Alotaibi,
under the approach of composite nanoarchitectonics of PtO
decorated mesoporous ZrO2, has synthesized mesoporous
ZrO2 and PtO by a wet chemical method [226]. The PtO@
ZrO2 photocatalyst exhibited high photocatalytic reduction
capacity of Hg2+ ions. Characteristically, the addition of
PtO enhanced the photoactivity of ZrO2 for Hg2+ removal
upon visible light irradiation. Factors such as the reduced
band gap of PtO@ZrO2 photocatalyst, broadening of the
visible light absorption spectrum, and suppression of charge
recombination resulted in superior photoactivity. 1.5% of
PtO added to ZrO2 resulted in complete photoreduction of
Hg2+ within 1 h after visible light irradiation. The newly
developed PtO@ZrO2 photocatalyst in composite nanoar-
chitectonics has the potential to be used as an environmen-
tally friendly photocatalyst for a variety of environmental
transformation phenomena. Moreover, its excellent stabil-
ity, permanence, and ability to be used in a wide variety
of applications make it a potential candidate for industrial
applications.
Approaches to remove pollutants and their models from
the environment are traditional research, but recognition of
their importance remains. Shah and Naglah have developed
a powerful material for the removal of dye molecules under
the approach of nanoarchitectonics of chitosan/glutaralde-
hyde/ZnO [227]. In this study, chitosan was cross-linked
with glutaraldehyde in the presence of zinc oxide nanopar-
ticles. As a result, a novel composite of chitosan/glutaral-
dehyde/zinc oxide was obtained. The nanoarchitectonized
composite showed ecient removal ability of eriochrome
black T dye from aqueous media. The analysis revealed that
the adsorption process of eriochrome black T dye is endo-
thermic and spontaneous. It is expected that this complex
can be used not only for this dye but also for the removal of
various organic and inorganic contaminants.
Photothermal membrane distillation is a promising and
sustainable approach for desalination and wastewater puri-
cation. Wang and co-workers have developed a hydro-
gel composite membrane with improved photothermal
on the ZnIn2S4 nanosheet surface by spin-coating and solvo-
thermal methods to obtain photoelectric conversion devices.
The resulting photoelectric conversion device photoanodes
have a synergistic combination of α-Fe2O3 nanodots and
MXene quantum dots on ZnIn2S4 nanosheets. It has a high
photocurrent density and exhibits benchmark photoelectro-
chemical performance. The above results are mainly due
to the MXene quantum dot capturing and storing electrons
from the conduction band of ZnIn2S4, mitigating electron-
hole pair recombination and S-O interfacial chemical bonds
introduced at the interface between ZnIn2S4 and α-Fe2O3
nanodot eciently promote carrier transfer. These factors
are believed to have led to the photoelectrochemical perfor-
mance. These interfacial nanoarchitectonics strategies will
provide insights for precisely regulating carrier separation
and migration. They will provide a better understanding of
interfacial charge separation and provide valuable guidance
for the rational design and fabrication of high-performance
composite electrode materials.
4 Sensing & Environment
There are many social demands in dealing with environ-
mental problems, such as sensing hazardous substances
[214218], removing pollutants [219223], etc. The targets
are diverse. Materials nanoarchitectonics with multi-com-
ponent components is therefore important for environmen-
tal applications. For example, Supreet, Pal, and co-workers
have developed a highly responsive and selective metha-
nol gas sensor at room temperature under the concept of
composite nanoarchitectonics with reduced-graphene oxide
and polyaniline [224]. The approach is based on camphor
sulde. As an approach, reduced-graphene oxide-polyani-
line nanocomposites were synthesized by a simple chemi-
cal oxidation synthesis process in the presence of camphor
sulfonic acid. The morphology of the prepared material
was observed to be nanoparticles and semi-crystalline in
structure. This gas sensor based on polyaniline doped with
reduced graphene oxide showed selective high response
to methanol vapor. Specically, the highest response was
found at 200 ppm. Furthermore, the sensor showed excel-
lent stability of more than 85% even after 180 days of fabri-
cation. This cost-eective, responsive, stable, reproducible,
and repeatable method may be a good candidate for com-
mercial production of methanol vapor sensors.
Detection of toxic ion species is an important issue for
environmental science. Various composite nanoarchitecton-
ics can be used to construct sensors for hazardous metal
ions. AL-Refai et al. prepared nanocomposites for sensor
electrodes under the concept of composite nanoarchitec-
tonics with polythiophene, carbon nanotubes, CuO and
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activity and antimicrobial properties of the cobalt complex
and chitosan composite were investigated. Spinel cobalt
oxide particles with octahedral shape were synthesized by
pyrolysis of cobalt(III) complex precursors. This synthesis
does not involve the use of harmful solvents, surfactants, or
complicated apparatus. Furthermore, the octahedral-shaped
spinel cobalt oxide particles were xed on a chitosan poly-
mer to form a composite. The performance of this compos-
ite in the photolysis of methylene blue was evaluated. It was
found that the regular morphology of octahedral-shaped
cobalt spinel oxide particles, appropriate band gap energy,
and absorption properties of chitosan are necessary for the
enhanced photocatalytic activity of the composite. Further-
more, the antibacterial eciency against two bacteria (E.
coli and Staphylococcus aureus) was tested using an agar
well diusion assay. The antimicrobial screening results
showed that coating the chitosan polymer with octahedral-
shaped spinel cobalt oxide particles enhanced its inhibitory
activity against both Gram-positive and Gram-negative
bacteria.
Hydroxyapatite-based nanocomposites have potential
for various biological applications. El-Naggar et al. exam-
ined nanocomposites of these three components under the
title nanoarchitectonics of hydroxyapatite/molybdenum
trioxide/graphene oxide composite [230]. Electron micro-
scopic analysis and the roughness characteristics observed
suggest that utilizing the type and amount of additives to
the hydroxyapatite component is a highly eective tactic to
tailor a composite suitable for biomedical applications. The
optimized triple complex exhibited the highest cell viability
against E. coli and Staphylococcus aureus compared to the
other compositions.
Antibiotic-resistant bacteria are one of the most danger-
ous factors causing human disease and endangering public
health and social security. One means of controlling this
conversion capacity as well as the fouling and moisture
resistance required for photothermal membrane distillation
(Fig. 7) [228]. The composite membrane exhibits a syner-
gistic eect of Ti3C2Tx MXene nanosheets with photother-
mal conversion capacity and the tannic acid-Fe3+ network in
the hydrogel. As a result, the lm exhibits excellent surface
self-heating capability. The hydrogel composite membrane
has high water vapor ux and high solar eciency under
solar irradiation. It is also resistant to oil fouling and surfac-
tant wetting. It can signicantly extend the lifetime of mem-
branes in the treatment of contaminated salt water. When
desalinated with actual seawater, the membrane exhibited
stable vapor ux for 100 h, excellent ion rejection, and
superior durability. The lifetime of the membranes in treat-
ing contaminated salt water could be signicantly extended.
The developed photothermal distillation membrane has
great potential for the production of standard-compliant
water.
5 Bio & Medical
The targets of biochemistry and biomedical applications are
complex in many cases. Organisms express their functions
by processing complex interactions in an integrated man-
ner. The materials that can deal with them must also have
a certain level of complexity. Therefore, various composite
nanoarchitectonics will be a force to be reckoned with in
this eld.
For example, antimicrobial function is a matter of uni-
versal importance in the biomedical eld. Bahramian and
co-workers have raised the concept of nanoarchitectonics
of octahedral Co3O4/chitosan composite and investigated
the photocatalytic activity and antimicrobial properties of
cobalt complexes and chitosan [229]. The photocatalytic
Fig. 7 A hydrogel composite
membrane with improved pho-
tothermal conversion capac-
ity as well as the fouling and
moisture resistance required for
photothermal membrane distil-
lation with a synergistic eect
of Ti3C2Tx MXene nanosheets
with photothermal conversion
capacity and the tannic acid-Fe3+
network in the hydrogel. Repro-
duced with permission from Ref.
[228]. Copyright 2024 American
Chemical Society
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
using cytotoxicity, apoptosis, and ow cytometry. The
results showed that the newly developed nanocomposites
had improved anticancer activity against the HeLa cell line.
It also became a better therapeutic agent for cervical cancer.
Spinal cord injury causes permanent loss of sensory and
motion function, but eective clinical treatments are needed.
In particular, synergistic treatments are urgently needed in
clinical practice. Jin, Feng, Wei, and co-workers designed a
composite patch for spinal cord injury repair consisting of
a nanober scaold and hyaluronic acid hydrogel (Fig. 9)
[233]. Compared to traditional invasive treatments, local
cellular drug injection, and tissue scaold implantation,
the patch provides a drug-exosome dual release system and
may oer a noninvasive method for clinical treatment of
spinal cord injury patients. The compound patch suppresses
the inammatory response by polarizing macrophages from
M1 to M2 type. And it increases neuronal survival by inhib-
iting neuronal apoptosis after spinal cord injury. These stud-
ies demonstrate the translation of nanoarchitectonics ideas
into clinical applications.
Living cells and organisms can be regarded as complex
composites composed of numerous biomolecules. They
perform complex biological functions by controlling their
concentration and spatial distribution in space and time.
Against this background, synthetic multi-network hydro-
gels that mimic extracellular matrices have attracted much
attention. Kubota reported their results on supramolecular-
polymer composite hydrogels in their recent review article
[234]. These gels can be regarded as one of a new class of
multi-network hydrogels. These composite hydrogels can
problem is the use of porous cellulose and other materi-
als to inhibit bacterial membranes and metabolism. This
methodology can also be a sustainable strategy for treat-
ing bacteria-contaminated water. Under the strategy com-
posite nanoarchitectonics of cellulose with porphyrin-Zn,
Chen and co-workers have developed a simple, reusable,
and environmentally friendly material for antimicrobial and
adsorption applications [231]. They has developed porous,
light-responsive bers to develop a simple, reusable, and
environmentally friendly material for antimicrobial and
adsorption applications. Specically, photoresponsive
bers were synthesized from covalently bonded compos-
ites of porous cellulose and porphyrin derivatives (Fig. 8).
The composite exhibited excellent inhibition and adsorption
against both Escherichia coli and Staphylococcus aureus. It
showed excellent inhibition against both Gram-negative and
Gram-positive bacteria. It was suggested that the bacterial
membrane is disrupted via porphyrin-zinc nanospheres. The
porous rod-like structural bers are expected to be appli-
cable for bacterial inhibition and ltration.
Saranya et al. developed composites with anticancer
properties using an approach called nanoarchitectonics of
cerium oxide/zinc oxide/graphene oxide composites [232].
Using an ultrasonic approach, they developed a material
based on cerium oxide/zinc oxide/graphene oxide nanocom-
posites. The nanocomposites exhibited smoother sheet-like
micromorphology. Using antiproliferation assay tests, they
evaluated the elimination anticancer ability of these nano-
systems against HeLa cell lines at various doses and vari-
ous culture intervals. Anticancer properties were validated
Fig. 8 Photoresponsive bers synthesized from covalently bonded
composites of porous cellulose and porphyrin derivatives for a simple,
reusable, and environmentally friendly material for antimicrobial and
adsorption applications. Reproduced with permission from Ref. [231].
Copyright 2023 Springer-Nature.
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
were constructed in situ to conne and stabilize the Au-Pt
nanozymes to enhance their mimetic activity. On top of that,
pluronic F127 was modied on the surface to improve the
hydrophilicity and biocompatibility of the composite. After
internalization by tumour cells, the Cu(II)-MOF shell is
degraded by endogenous acidity and glutathione. The nano-
zymes are exposed for cascade catalytic chemodynamic
therapy. Exposed Au-Pt nanozymes interact with intertu-
moral H2O2 to form O2 via catalase-like activity. H2O2 with
glucose oxidase-like properties for ·OH formation was gen-
erated as a mimetic peroxidase for cascade chemodynamic
therapy. Laser irradiation at 808 nm induced local hyper-
thermia and promoted catalytic activity for ·OH formation.
The high photothermal conversion capacity also enhanced
chemodynamic therapy, and Cu2+ ions consumed glutathi-
one to further improve chemodynamic therapy eciency as
an enhancement of cascade catalytic tumour therapy. Three-
in-one nanozyme systems improve the ecacy of tumour
therapy and minimize side eects on normal tissue. This is a
new paradigm with drug-free single nanoteams.
6 Various Other Functions and Applications
The possibilities of materials assembled by composite nano-
architectonics are enormous. The range of applications is
also diverse. From basic research to applications can be
found. The following are examples of some of these studies
in various elds.
rationally integrate the stimulus response of supramolecu-
lar gels with the stiness of polymer gels. Furthermore,
supramolecular-polymer composite hydrogels have poten-
tial applications in controlled release of protein biopharma-
ceuticals. Supramolecular-polymer composite hydrogels
can incorporate functional molecules such as enzymes
or their inhibitors as a matrix. This allows for the release
of protein biopharmaceuticals in response to antibodies.
Supramolecular-polymer composite hydrogels are expected
to be the next generation of smart and responsive soft mate-
rials for biomedical applications including tissue engineer-
ing and regenerative medicine. Thus, the spatiotemporally
controlled fabrication of functional composite soft materi-
als will produce a variety of functions. This includes bio-
medical applications such as 3D controlled release of drugs/
proteins, construction of hierarchical organoids, and devel-
opment of implantable/injectable gel devices.
Natural bio-systems skilfully use cascade reactions.
Mimicking the processes of this cascade is a highly attrac-
tive target. However, orderly assembly of dierent enzyme-
like functions is not always easy. Cheng, Wang, Yin, and
co-workers have developed a composite with three-in-one
functionality (Fig. 10) [235]. In this composite, a single
gold-platinum nanozyme provides oxygen as a mimetic
catalase. It also produces H2O2 through glucose oxidase-
like properties. In addition, it initiates a cascade conversion
for ·OH generation as a mimetic peroxidase for chemody-
namic therapy. Metastable Cu2O nanoparticles were used as
scaolds to immobilize ultrasmall Au-Pt nanozymes. MOF
was used to encapsulate the nanozymes. Porous MOF shells
Fig. 9 A composite patch for
spinal cord injury repair consist-
ing of a nanober scaold and
hyaluronic acid hydrogel. Repro-
duced with permission from Ref.
[233]. Copyright 2023 American
Chemical Society
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
Cu/Wood layers with dierent electro-magnetic proper-
ties induced multiple reections at their interfaces. This
promoted absorption attenuation and enhanced the electro-
magnetic shielding eect. It was veried that this multilayer
composite material can block more than 99.99% of incident
electromagnetic waves.
Lightweight structural materials with various combina-
tions of high stiness, high strength, high toughness, and
high hardness have a wide range of uses. Although the
development of such materials is highly desired, they are
not always easy to fabricate articially. On the other hand,
some biological structural materials have hierarchically
heterogeneous structures bounded by gradient interfaces.
Structures ingeniously integrate multiple mutually exclusive
mechanical properties. Gao, Yu, and co-workers proposed
a simple bottom-up approach to fabricate such materials
by combining continuous nanober-assisted evaporation-
induced self-assembly, stacking, pressure-free sintering,
and resin inltration method (Fig. 11) [238]. They have
produced a large scale ceramic-resin composite inspired by
pearls with a tunable heterogeneous structure. This ceramic-
resin composite has a tough, pearl-like body and a rigid,
hard outer surface. A gradient intermediate layer was intro-
duced between these two parts to provide a gradual tran-
sition between adjacent dissimilar layers. This eectively
mitigated the mismatch of properties between the dierent
layers. As a result, mutually exclusive mechanical proper-
ties were successfully integrated into a single material. The
Takaguchi, Orita, and co-workers investigated photo-
electron transfer reactions in composites of dyes on carbon
nanotubes [236]. Namely, visible light absorbing anthrylene
and ferrocenoyl substituted acetylene dyes were compos-
ited with single-walled carbon nanotubes. Specically,
copper-catalysed dimerization reactions of anthrylene and
ferrocenoyl-substituted terminal ethynes were used. In addi-
tion, composite one-pot nanoarchitectonics was achieved by
subsequent adsorption of butadiyne dye onto single-walled
carbon nanotubes. The dye-nanotube composite was dis-
persed in water using an amphiphilic poly(amidoamine)
dendrimer. In this composite, irradiation with visible light
(> 422 nm) allowed the transfer of electrons from 1-benzyl-
1,4-dihydronicotinamide to methyl viologen dichloride.
This compositing methodology of adsorbing anthrylene and
ferrocenoyl will pave the way to novel visible-light organic
dyes to photocurrent conversion.
In the concept of micro-nanoarchitectonics of electroless
Cu/Ni composite materials based on wood, Pan, Huang,
and co-workers fabricated Cu-Ni multilayer composites by
a simple electroless Cu and Ni method on wood surfaces
[237]. As materials based on wood, Cu-Ni multilayer com-
posites were fabricated by a simple electroless Cu and Ni
method on wood surfaces. Wood was composited by two
times electroless Cu and one time electroless Ni to obtain
an ideal surface roughness prole. The metallic Cu and Ni
were embedded closely together on the surface of the wood,
forming a dense composite layer. The three Ni/Cu Cu/Cu
Fig. 10 A composite with
three-in-one functionality that
improves the ecacy of tumour
therapy and minimize side eects
on normal tissue. Reproduced
with permission from Ref. [235].
Copyright 2024 Wiley-VCH.
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
cellulose showed a reinforcing eect below their melting
temperature and a decreasing eect above the melting tem-
perature. This remarkable temperature response behaviour
occurs because poly(stearyl methacrylate) particles act as
an eective reinforcing ller in the material in the hard state
and have little eect on the mechanical strength of the sup-
port network in the soft state. The responsiveness of the
composite gel can be adjusted simply by varying the amount
of poly(stearyl methacrylate). Increasing the amount of
incorporated poly(stearyl methacrylate) particles wid-
ened the dierence between the hard and soft states of the
methodology presented here paves the way for the design of
advanced bio-inspired heterogeneous materials for diverse
structural and functional applications. It is expected that
advanced materials with diverse functions, not only struc-
tural, will be designed and manufactured on an industrial
scale.
Uyama and co-workers developed a hydrogel that can
switch mechanical strength depending on temperature
by incorporating poly(stearyl methacrylate) as a response
domain in bacterial cellulose as a support hydrogel (Fig. 12)
[239]. Poly(stearyl methacrylate) particles in bacterial
Fig. 12 A hydrogel that can switch mechanical strength depending on temperature by incorporating poly(stearyl methacrylate) as a response
domain in bacterial cellulose as a support hydrogel. Reproduced with permission from Ref. [239]. Copyright 2023 Oxford University Press
Fig. 11 A simple bottom-up approach to fabricate lightweight struc-
tural materials with high stiness, high strength, high toughness, and
high hardness by combining continuous nanober-assisted evapora-
tion-induced self-assembly, stacking, pressure-free sintering, and resin
inltration method. Reproduced with permission from Ref. [238].
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
These multifaceted high functionalities are expected to con-
tribute to the smart materials industry.
Kobayashi and co-workers prepared Eu(III) composite
materials from europium compounds and tetramethylam-
monium acetate using a solvent-free mechanochemical
process [241]. The composite material was found to have
a bimetallic structure that functions as a bridge molecule
between multiple Eu(III) complexes. The composite exhib-
its outstanding photoluminescence performance and excel-
lent circular polarization activity. It also exhibits thermal
stability. Due to the convenience, eciency, and sustain-
ability of green chemistry, the solvent-free nanoarchitecton-
ics of luminescent lanthanide materials is highly promising.
Miyazaki and Yamada prepared praseodymium oxide
particle-embedded composite lms using praseodymium
nitrate and urethane resin as starting materials [242]. By
irradiating the prepared composite lms with ultraviolet
light, composite lms containing Pr6O11 nanoparticles of
various particle sizes can be obtained. This does not require
a heating process at high temperatures, as is common in
the preparation of praseodymium-doped glass, as UV irra-
diation can form praseodymium oxide nanoparticles in the
composite lms. The resulting composite lm exhibited a
composite. The development of such strength-responsive
materials will facilitate the industrial utility of hydrogels as
articial muscles and soft robotic components.
Hydrogel materials show promise for use in a variety of
elds, including exible electronic devices, bio-tissue engi-
neering, and wound dressings. Gao and co-workers have
developed hydrogels with the synergistic eects of hydro-
gen bonding, metal coordination bonding, and electrostatic
interactions (Fig. 13) [240]. Based on these multiple syn-
ergistic eects, composite hydrogels have high mechanical
strength, rapid self-healing, and ecient self-healing capa-
bilities. The hydrogels were prepared by a simple one-pot
method. A homogeneous prepolymer solution containing
branched polyethyleneimine, acrylic acid, glycerol, zirco-
nyl chloride octahydrate, photoinitiator, and water was dis-
persed in a glass container and polymerization was initiated
by UV irradiation. Because of the multiple reversible eects
at work, hydrogels have excellent self-healing capabilities.
For example, a disrupted hydrogel achieved 95% self-heal-
ing within 4 h at room temperature. Composite hydrogels
had programmable and reversible shape transformation
properties. It also exhibited outstanding fatigue resistance
properties. The introduction of glycerol gave the hydro-
gel excellent antifreeze and moisture retention properties.
Fig. 13 Hydrogels with the synergistic eects of hydrogen bonding, metal coordination bonding, and electrostatic interactions. Reproduced with
permission from Ref. [240]. Copyright 2023 Royal Society of Chemistry
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
composed of a biodegradable elastomer, poly(l-lactide-co-
ε-caprolactone), and biocompatible/biodegradable nanopar-
ticles, polytetrauoroethylene and silicon dioxide. The
micro-pattern reduces the diusion area of water molecules.
The embedded nanoparticles block water permeation, which
synergistically enhances the water barrier performance. In
the initial stage of exposure to water, the surface repelled the
wetting of water droplets. Subsequently, the nanoparticles
embedded in the polymer matrix physically inhibited water
penetration. These synergistic eects lengthen the timescale
for water molecules to reach the electronics. The compos-
ite for stretchable bioabsorbable electronics acts as a base
encapsulating lm. It will be able to ensure stable device
functionality over a long period of time.
The development of polydimethylsiloxane elastomers
with high self-healing eciency and excellent mechanical
properties is a very attractive research target. Zhang, He,
and co-workers have created composite elastomers based on
polydimethylsiloxane with ultrafast light-controlled heal-
ing capability and toughness (Fig. 16) [245]. The dynamic
bond breakdown and reconstruction and the strengthening
eect of the carbon nanotubes contained in the composite
elastomer are observed. Therefore, the composite elastomer
exhibited excellent fracture toughness derived from good
yield strength and elongation. Furthermore, with the help
of dynamic polymer/ller interfacial interactions, carbon
nanotubes can quickly and directly heat the damaged part of
the composite and achieve ultra-fast repair. As a result, the
PL property at 605 nm when excited at 444 nm, correspond-
ing to the photoluminescence of the 1D2->3H4 transition of
Pr3+.
Electrochromic devices have a variety of applications,
including energy-saving devices and displays. Under
the policy of facile nanoarchitectonics of electrochromic
devices, Kim, You, and co-workers have created electro-
chromic devices using transparent bioplastic composite
substrates (Fig. 14) [243]. Specically, novel electrochro-
mic devices based on poly(3,4-ethylenedioxythiophene)
(PEDOT)/2,2,6,6-tetramethylpiperidine-1-oxide cellulose
nanober (TEMPO-CNF)/epoxy composite materials were
fabricated by simple solution nanoarchitectonics by simple
solution cast polymerization. The PEDOT layer (PEDOT/
TEMPO-CNF/epoxy) coated on the TEMPO-CNF/epoxy
substrate functions as a conductive electrode. It showed a
reversible colour change between light blue (translucent
state) and dark blue (coloured state) depending on the redox
potential. In other words, a reversible colour switch between
light blue and dark blue could be caused. Such a composite
nanoarchitectonics approach could be a simple fabrication
route for various energy-saving smart windows and high-
contrast displays.
Eective waterproong or encapsulation systems are
essential for reliable and durable operation of electronic
devices, etc. Hwang and co-workers have developed a
stretchable, bioabsorbable encapsulants (Fig. 15) [244]. The
composite has a stretchable biodegradable array of pillars
Fig. 14 Electrochromic devices using transparent bioplastic com-
posite substrates based on poly(3,4-ethylenedioxythiophene)
(PEDOT)/2,2,6,6-tetramethylpiperidine-1-oxide cellulose nanober
(TEMPO-CNF)/epoxy composite materials fabricated by simple solu-
tion nanoarchitectonics by simple solution cast polymerization. Repro-
duced with permission from Ref. [243]. Copyright 2023 Elsevier
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
structures at dierent length scales. The majority of the lm
is made of a polymer matrix and nanoparticle ller. The
pore size of the polymer matrix is designed to be compara-
ble to the wavelength of sunlight (400–2000 nm). Sunlight
is strongly scattered at the interface between the surface and
the interior according to the dierence in refractive index.
Nanoparticle llers are added to adjust the infrared radiation
properties of the lm; ZnO nanoparticles allow for infrared
transparency. SiO2 particles also increase the IR emissivity.
Air lls the tiny valleys on the lm surface, which reduces
solid-liquid adhesion and makes the lm superhydropho-
bic. This design and manufacturing approach will aid in the
long-term operation of passive radiative cooling applica-
tions because of its simplicity and versatility.
Wang and coworkers have developed composite materi-
als with good electromagnetic wave absorption properties
by Nanoarchitectonics of SiC/multilayer graphene com-
posite powders [247]. Specically, SiC/multilayer gra-
phene composite powders were synthesized by a simple
catalyst-assisted carbon thermal reduction method using
silicon dioxide and expanded graphite. Graphene has a
unique internal microstructure, high dielectric loss, and
self-repair time is signicantly reduced. In other words, this
dual reversible network nanoarchitectonics strategy suc-
cessfully reconciles the conicting properties of mechanical
performance and self-healing eciency. Such materials can
be expected to have ultra-fast self-healing eciency, capa-
ble of completing the self-repair process in a few minutes.
The materials will have excellent toughness and self-heal-
ing brains. It will encourage a variety of further practical
applications, such as remote freeze/thaw materials. The
composite elastomer has potential applications as a remote
de-icing surface.
Daytime passive radiative cooling is a promising meth-
odology for reducing energy demand and mitigating global
warming. However, surface contamination due to dust and
bacteria deposition hinders practical passive radiative cool-
ing applications. Cai and co-workers proposed composite
nanoarchitectonics to integrate passive radiative cooling
materials with self-cleaning and antimicrobial functions
[246]. Hierarchically patterned nanoporous composite
materials were developed using a simple template mold-
ing method (Fig. 17). Radiative cooling and superhydro-
phobic properties can be achieved by creating hierarchical
Fig. 15 Composite with a stretchable biodegradable array of pil-
lars composed of a biodegradable elastomer, poly(l-lactide-co-ε-
caprolactone), and biocompatible/biodegradable nanoparticles,
polytetrauoroethylene and silicon dioxide in which the micro-pattern
reduces the diusion area of water molecules, and the embedded
nanoparticles block water permeation, which synergistically enhances
the water barrier performance. Reproduced with permission from Ref.
[244]. Copyright 2023 American Chemical Society
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
exhibits optimal electromagnetic wave absorption proper-
ties. The three-dimensional dispersion nanoarchitecton-
ics of graphene improves the impedance matching of the
material. The advantages of large specic surface area, high
defect density, and excellent electrical conductivity increase
dielectric and magnetic losses.
Wood-based solar steam generators are gaining promi-
nence in the eld of desalination and water purication. The
material is considered to be particularly cost-eective and
good electrical conductivity, which improves the imped-
ance matching of the material and increases magnetic loss.
the SiC/multilayer graphene composite powder could be an
excellent electromagnetic wave absorber. In-situ synthesis
of graphene is an eective way to improve the electromag-
netic wave absorption properties of SiC nanopowders. With
an appropriate excess amount of expanded graphite, multi-
layer graphene of appropriate thickness is formed in-situ in
the composite powder. The structure-optimized composite
Fig. 17 Composite nanoarchitectonics to integrate passive radiative cooling materials with self-cleaning and antimicrobial functions with radiative
cooling and superhydrophobic properties. Reproduced with permission from Ref. [246]. Copyright 2023 American Chemical Society
Fig. 16 Composite elastomers
based on polydimethylsiloxane
with ultrafast light-controlled
healing capability and toughness
with dynamic bond breakdown
and reconstruction and the
strengthening eect of the carbon
nanotubes contained in the
composite elastomer. Repro-
duced with permission from Ref.
[245]. Copyright 2023 American
Chemical Society
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
retardant properties. Well-dispersed anionic and cationic
clay nanosheets in the polymer matrix signicantly enhance
thermal stability, mechanical properties, and ame retar-
dancy. It is expected that a similar methodology can be
applied to various polymer composite materials, where a
rational composite of anionic and cationic clays can be used
to develop environmentally friendly ame retardants with
improved thermal and mechanical properties.
Habi and co-workers have developed composite materi-
als for package applications under the design guideline of
composite nanoarchitectonics of poly(lactic acid)/metal-
organic framework. Specically, they used poly(lactic acid)
(PLA), metal-organic framework (MOF-5), and metal-
organic framework/graphene oxide (MOF-5/GO) [250].
The nanocomposites were prepared by melt extrusion using
a vertical co-rotating biaxial microcompounder. In particu-
lar, the water vapor permeability was strongly reduced by
the incorporation of MOF-5/GO. The presence of MOF-5/
GO ller was found to have a signicant impact on the
water vapor barrier properties. This property will be a useful
insight for the development of materials with tailored bar-
rier properties in packaging, especially in food packaging.
7 Summary and Perspectives
Nanoarchitectonics is a post-nanotechnology concept that
involves building functional materials that reect the nano-
structures. Functional material systems are assembled from
units such as atoms and molecules. Since materials are in
principle made of atoms and molecules, the methodology
of nanoarchitectonics may be applicable to the creation of
all materials science. In particular, the approach of combin-
ing and building multiple types of components to create
renewable. Li, Xu, and co-workers have developed a unique
bilayer composite that incorporates polyaniline nanorods
homogeneously into a 3D mesoporous matrix of natural
wood (Fig. 18) [248]. The synthesis is a simple, ecient,
and environmentally friendly one-step approach. Wood
decorated with polyaniline exhibited ultra-high absorbance
over a wide wavelength range due to the conjugation of
wood with coral-like polyaniline nanorods. In particular,
the large number of aligned wood microchannels allowed
constant and rapid water transport at the air-water interface
under the pressure of capillary forces. This eect generates
water vapor at a high evaporation rate. The result is a robust,
low-cost, promising evaporator that can be used for water
purication. Polyaniline wood exhibits long-term oatabil-
ity and is chemically stable. Therefore, it could be an ideal
candidate for low-energy solar-driven water evaporation
applications.
Widely used ame retardants have been brominated ame
retardants, which are problematic because of their harmful
properties. In response to such problems, there is a need to
develop environmentally friendly ame retardants. Choy
and co-workers have developed a ame retardant compos-
ite using a tactic called composite nanoarchitectonics with
ionic clay nanollers-embedded polypropylene [249]. Spe-
cically, polypropylene is used to composite ionic nano-
llers, layered double hydroxide (LDH) and cationic clay
(mica). The ionic nanollers are modied with stearate and
cetyltrimethylammonium to make them compatible with
polypropylene. In other words, to improve the molecular
bonding interaction of ionic nanollers, anionic stearate and
cationic cetyltrimethylammonium surfactants were inserted
between the clay layers and the corresponding nanollers
were synthesized by coprecipitation and ion exchange reac-
tions. The composite material exhibited excellent ame
Fig. 18 A unique bilayer composite with incorporates polyaniline
nanorods homogeneously into a 3D mesoporous matrix of natu-
ral wood in which the large number of aligned wood microchannels
allowed constant and rapid water transport at the air-water interface
under the pressure of capillary forces. Reproduced with permission
from Ref. [248]. Copyright 2023 Oxford University Press
1 3
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Journal of Inorganic and Organometallic Polymers and Materials (2024) 34:2926–2947
to transform single-function research examples into prac-
tical products that can meet a variety of requirements. To
expand such industrial potential, technology for mass pro-
duction should be developed. This may also require process
optimization using articial intelligence. It would also be
very interesting to develop articial synthesis machines for
complex processes through the use of robot technology.
If we can solve the above problems, we may be able to
develop a device that automatically prefects very complex
material systems. Nanoarchitectonics is a method for every-
thing in materials science. A nanoarchitectonics machine
may become the ultimate device to create all materials from
atoms and molecules. Humans may create devices that pro-
duce functional material systems that function as versatile
as living organisms.
Acknowledgements This study was partially supported by Japan
Society for the Promotion of Science KAKENHI (Grant Numbers,
JP20H00392 and JP23H05459).
Author Contributions This is a single author manuscript. All the tasks
were done by this author.
Funding Open Access funding provided by The University of Tokyo.
Data Availability No datasets were generated or analysed during the
current study.
Declarations
Competing Interests The authors declare no competing interests.
Open Access This article is licensed under a Creative Commons
Attribution 4.0 International License, which permits use, sharing,
adaptation, distribution and reproduction in any medium or format,
as long as you give appropriate credit to the original author(s) and the
source, provide a link to the Creative Commons licence, and indicate
if changes were made. The images or other third party material in this
article are included in the article’s Creative Commons licence, unless
indicated otherwise in a credit line to the material. If material is not
included in the article’s Creative Commons licence and your intended
use is not permitted by statutory regulation or exceeds the permitted
use, you will need to obtain permission directly from the copyright
holder. To view a copy of this licence, visit http://creativecommons.
org/licenses/by/4.0/.
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... Efficient catalysts are highly in demand and necessary for cleaner and sustainable chemistry [1]. The catalysts should be concurrently active, selective towards the expected product, and easily recyclable. ...
... Therefore, such methods should be developed to achieve this aim. Initially, the goal was to pursue homogeneous catalysis by developing finer catalytic systems that involve structural reactivity and well-stabilized reaction intermediates [1,2]. This system has already achieved substantial success in olefin hydrogenation, polymerization, and metathesis [3,4]. ...
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Recent advances in industrial catalysis are very important for the development of effective and efficient catalysts and catalytic methods. The review largely focuses on immobilization techniques that have been utilized for metal complexes, usually mesoporous materials such as silica, alumina, and zeolite. The supported catalysts have a wider range of catalytic applications than their neat or homogeneous counterparts. The active metal compound may be retained on the solid support by adsorption, ion exchange, encapsulation, or the formation of a covalent bond between the metal–ligand and the solid support. The supported complexes are used as catalysts for organic transformation reactions, such as oxidation and functionalization of organic compounds.
... Their essential advantage their use of complementary properties, identified as ying-and-yang in the above classifications. Nanoarchitectonics of composite materials has been recently highlighted [204], where such complementarity was underlined. Figure 4 shows an example of the incorporation of glass beads into PLA film, where enhanced barrier-and optical-properties have been obtained. ...
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... In a sense, rocks can be considered a type of composite material, and it is natural to study petrophysics from the material perspective. The approach to studying digital rock cores is not fundamentally different from studying digital polymers (Katsuhiko et al., 2024). ...
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In this paper we discuss the latest developments in colloidal plasmonics, a field with over a century of history, applied to the biomedical sector. Emphasis is placed on the nanoarchitectonic nature of plasmonic systems that can be used for sensing, drug delivery and manipulation of biomolecules. For instance, quantum effects linked to plasmonic phenomena are being used to enhance monitoring of chiral particles and their interaction with light, which is essential for the pharmaceutical industry in reaching the required enantiopurity in some drugs. In diagnostics, radiofrequency waves can excite surface plasmon resonance through amplified photoacoustic effects, thus permitting thermo-acoustic imaging. An example of enhanced therapy was introduced in carefully designed nanoarchitectures where a multi-branched gold nanooctopus was surrounded by a mesoporous polydopamine and loaded with ribonucleoproteins for the target delivery into tumor cells. Moreover, the longstanding challenge of heating due to Ohmic losses, which has hindered the use of plasmonic tweezers for manipulating biologically relevant analytes, is now being exploited for enhanced trapping, manipulation, and transport of cells and other biological particles. The combination of magnetic materials and plasmonic colloids in the realms of magnetoplasmonics can also be explored in sensing and enhanced drug delivery, which further exemplifies the versatility of nanoarchitectonics.
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Isotopically labeled alkanes play a crucial role in organic and pharmaceutical chemistry. While some deuterated methylating agents are readily available, the limited accessibility of other deuteroalkyl reagents has hindered the synthesis of corresponding products. In this study, we introduce a nickel‐catalyzed system that facilitates the synthesis of various deuterium‐labeled alkanes through the hydrodeuteroalkylation of d2‐labeled alkyl TT salts with unactivated alkenes. Diverging from traditional deuterated alkyl reagents, alkyl thianthrenium (TT) salts can effectively and selectively introduce deuterium at α position of alkyl chains using D2O as the deuterium source via a single‐step pH‐dependent hydrogen isotope exchange (HIE). Our method allows for high deuterium incorporation, and offers precise control over the site of deuterium insertion within an alkyl chain. This technique proves to be invaluable for the synthesis of various deuterium‐labeled compounds, especially those of pharmaceutical relevance.
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π-Conjugated polymers such as polythiophene provide intramolecular wire effects upon analyte capture, which contribute to sensitive detection in chemical sensing. However, inherent aggregation-induced quenching causes difficulty in fluorescent chemical sensing in the solid state. Herein, we propose a solid-state fluorescent chemosensor array device made of a paper substrate (PCSAD) for the qualitative and quantitative detection of metal ions. A polythiophene derivative modified by dipicolylamine moieties (1poly), which shows optical changes upon the addition of target metal ions (i.e., Cu²⁺, Cd²⁺, Ni²⁺, Co²⁺, Pb²⁺, Zn²⁺, and Hg²⁺), was highly dispersed on the paper substrate using office apparatus. In this regard, morphological observation of the PCSAD after printing of 1poly suggested the contribution of the fiber structures of the paper substrate to the homogeneous dispersion of 1poly ink to suppress aggregation-induced quenching. The optical changes in the PCSAD upon the addition of metal ions was rapidly recorded using a smartphone, which was further applied to imaging analysis and pattern recognition techniques for high-throughput sensing. Indeed, the printed PCSAD embedded with 1poly achieved the accurate detection of metal ions at ppm levels contained in river water. The limit of detection of the PCSAD-based sensing system using a smartphone (48 ppb for Cu²⁺ ions) is comparable to that of a solution-based sensing system using a stationary spectrophotometer (16 ppb for Cu²⁺ ions). Therefore, the methodology based on a combination of a paper-based sensor array and a π-conjugated polymer will be a promising approach for solid-state fluorescent chemosensors.
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Peptides have been established as modular catalysts for various transformations. Still, the vast number of potential amino acid building blocks renders the identification of peptides with desired catalytic activity challenging. Here, we develop a machine-learning workflow for the optimization of peptide catalysts. First—in a hypothetical competition—we challenged our workflow to identify peptide catalysts for the conjugate addition reaction of aldehydes to nitroolefins and compared the performance of the predicted structures with those optimized in our laboratory. On the basis of the positive results, we established a universal training set (UTS) containing 161 catalysts to sample an in silico library of ∼30,000 tripeptide members. Finally, we challenged our machine learning strategy to identify a member of the library as a stereoselective catalyst for an annulation reaction that has not been catalyzed by a peptide thus far. We conclude with a comparison of data-driven versus expert-knowledge-guided peptide catalyst optimization.
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The interaction between diverse nanoarchitectured fullerenes and cells is crucial for biomedical applications. Here, we detailed the preparation of hydrophilic self-assembled fullerenes by the liquid-liquid interfacial precipitation (LLIP) method and hydrophilic coating of the materials as a possible vascularization strategy. The interactions of vascular endothelial cells (ECs) with hydrophilic fullerene nanotubes (FNT-P) and hydrophilic fullerene nanowhiskers (FNW-P) were investigated. The average length and diameter of FNT-P were 16 ± 2 μm and 3.4 ± 0.4 μm (i.e. aspect ratios of 4.6), respectively. The average length and diameter of FNW-P were 65 ± 8 μm and 1.2 ± 0.2 μm (i.e. aspect ratios of 53.9), respectively. For two-dimensional (2D) culture after 7 days, the ECs remained viable and proliferated up to ~ 420% and ~ 400% with FNT-P and FNW-P of 50 μg/mL, respectively. Furthermore, an optimized chitosan-based self-healing hydrogel with a modulus of ~400 Pa was developed and used to incorporate self-assembled fullerenes as in vitro three-dimensional (3D) platforms to investigate the impact of FNT-P and FNW-P on ECs within a 3D environment. The addition of FNW-P or FNT-P (50 μg/mL) in the hydrogel system led to proliferation rates of ECs up to ~323% and ~280%, respectively, after 7 days of culture. The ECs in FNW-P hydrogel displayed an elongated shape with aligned morphology, while those in FNT-P hydrogel exhibited a rounded and clustered distribution. Vascular-related gene expressions of ECs were significantly upregulated through interactions with these fullerenes. Thus, the combined use of different nanoarchitectured self-assembled fullerenes and self-healing hydrogels may offer environmental cues influencing EC development in a 3D biomimetic microenvironment, holding promise for advancing vascularization strategy in tissue engineering.
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Considerable efforts have been devoted to the development of new organic‐inorganic hybrid perovskites as well as their passivation‐layer materials to improve the performance of solution‐processable thin‐film solar cells for practical applications. For this purpose, monocations, such as monoammonium ions, have been studied extensively as organic building blocks. Herein, a new class of cationic molecules featuring a triptycene framework is introduced, to which three ammonium ions are attached close to each other. Inspired by the previous finding that 1,8,13‐trisubstituted triptycenes have an excellent ability to form 2D assemblies, two derivatives with ammonium ion groups at these positions are synthesized, linked either directly or via methylene spacers. Hybrid perovskites with different dimensionalities in terms of the inorganic octahedral units were prepared by reaction of the triammonium‐appended triptycene tripods with PbI 2 , however, the optoelectronic properties obtained were unsatisfactory. Even so, the triammonium‐containing triptycene tripod having methylene spacers was shown to serve as a good passivation layer for perovskites solar cells (PSCs), leading to improvements in power conversion efficiency and long‐term stability. Given the large degree of design freedom, triptycene tripods merit further investigation as a new motif in the development of surface‐passivation materials for PSCs.