Xuetong Zhang’s research while affiliated with Jiangnan University and other places

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Publications (120)


Comparison between the traditional route and our route
Schematic illustration of solvent-regulated switchable superhydrophobic–hydrophilic silica aerogels precursor transitions and synthesis of on-demand superhydrophobic/superhydrophilic aerogels reported in our study vs. synthesis of traditional silica aerogels without SB-A/SL-A precursor transitions. MTMS trimethoxymethylsilane, TMOS tetramethoxysilane, EtOH ethanol, SB-A superhydrophobic aerogel, SL-A superhydrophilic aerogel, Sc CO2 supercritical CO2.
Switchable SL-A/SB-A precursor transitions and corresponding superhydrophobic/superhydrophilic silica aerogels
SB-A superhydrophobic aerogel, SL-A superhydrophilic aerogel. a Synthesis route of on-demand superhydrophilic/superhydrophobic silica aerogels with switchable SL-A/SB-A precursor transition by using ethanol as reaction solvent. MTMS trimethoxymethylsilane; TMOS tetramethoxysilane, EtOH ethanol, Sc CO2 supercritical CO2. b Photographs of silica aerogels (b1) and water contact angle on superhydrophobic silica aerogels (b2) and droplets with diverse color standing on silica aerogels (b3). Scale bar: b1 and b3: 1 cm; b2: 500 μm. c Water contact angles of silica aerogels from SB-A precursor after hot water treatment for different times. Scale bar: 500 μm. Error bar: <6.0°. d Water contact angles of silica aerogels from SL-A precursor after hot ethanol treatment for different times. Scale bar: 500 μm. Error bar: <4.5°. e Water contact angles of silica aerogels from cyclic SL-A/SB-A precursor transitions by treating wet gels alternately with hot water/ethanol. Error bar: <2.6°. f Water contact angles of silica aerogels with diverse M/T molar ratios from initial SB-A precursors (left) and water-induced SL-A precursors (right). M/T: MTMS: TMOS. g SEM image of silica aerogel from initial SB-A precursor. Scale bar: 500 nm. h Illustration of Cassie state to Wenzel state transition of silica aerogel from the initial SB-A precursor to the water induced SL-A precursor. Source data are provided as a Source Data file.
Switchable SL-A/SB-A precursor transitions and corresponding superhydrophobic/superhydrophilic silica aerogels
SB-A superhydrophobic aerogel, SL-A superhydrophilic aerogel. a Synthetic route of on-demand superhydrophilic/superhydrophobic silica aerogels with switchable SL-A/SB-A precursor transition by using water as a reaction solvent. MTMS trimethoxymethylsilane, TMOS tetramethoxysilane, EtOH ethanol, Sc CO2 supercritical CO2. b Photographs of silica aerogels (b1) and water contact angles on superhydrophilic silica aerogels initially (b2) and later (b3). Scale bar: b1: 1 cm; b2 and b3: 500 μm. c Water contact angles of silica aerogels from SL-A precursor after hot ethanol treatment for different times. Scale bar: 500 μm. Error bar: <7.9°. d Water contact angles of silica aerogels from SB-A precursor after hot water treatment for different times. Scale bar: 500 μm. Error bar: <7.4°. e Water contact angles of silica aerogels from cyclic SL-A/SB-A precursor transitions by treating wet gels alternately with hot ethanol/water. Error bar: <2.5°. f Water contact angles of silica aerogels with diverse M/T molar ratios from initial SL-A precursors (left) and ethanol-induced SB-A precursors (right). M/T: MTMS: TMOS. g SEM image of silica aerogels from initial SB-A precursor. Scale bar: 500 nm. h Illustration of Wenzel state to Cassie state transition of silica aerogel from initial SL-A precursor to ethanol-induced SL-A precursor. Source data are provided as a Source Data file.
Mechanism investigation of switchable SL-A/SB-A precursor transitions
SB-A superhydrophobic aerogel, SL-A superhydrophilic aerogel. a Diagram illustration of solvent-regulable interfacial groups by reversible esterification reaction. b ATR-IR spectra, c²⁹Si CP MAS NMR spectra, and d¹³C CP MAS NMR spectra of corresponding superhydrophobic/superhydrophilic silica aerogels (MTMS/TMOS 5:5) from SB-A/SL-A precursors. MTMS trimethoxymethylsilane, TMOS tetramethoxysilane. Qn denotes a tetrahedral Si with n bridging oxygens, Tn stands for a tetrahedral Si with 1C and n bridging oxygens. Source data are provided as a Source Data file.
Universality of solvent-regulated SB-A/SL-A precursor transitions and on-demand application for corresponding superhydrophobic and superhydrophilic silica aerogels
SB-A superhydrophobic aerogel, SL-A superhydrophilic aerogel. a Chemical structures of diverse silica precursor mixtures for switchable SL-A/SB-A precursor transitions. MTMS trimethoxymethylsilane, TMOS tetramethoxysilane, TEOS tetraethyl orthosilicate, SMS sodium methicosilicate. b Water contact angles of MTMS/TEOS silica aerogels obtained from initial SB-A precursors and water-induced SL-A precursors. c Water contact angles of SMS/TMOS silica aerogels obtained from initial SL-A precursors and ethanol-induced SB-A precursors. d UV-vis spectra of residual MB in dichloromethane during adsorbing by superhydrophobic silica aerogels. MB: methylene blue. e Final residual concentrations of MB in dichloromethane after adsorbed by superhydrophobic silica aerogels and superhydrophilic ones. Error bar: <0.13 μg/g. f Final residual concentrations of MB in water after adsorbed by superhydrophobic silica aerogels and superhydrophilic ones. Error bar: <0.53 μg/g. g Photographs of MB in dichloromethane (below layer) and water (upper layer) before adsorption (g1) and after adsorbed by superhydrophobic silica aerogels (below layer) and superhydrophilic ones (upper layer) (g2). Scale bar: 1 cm. h Self-cleaning properties of superhydrophobic silica aerogels. Scale bar: 0.5 cm. i droplet resilience of superhydrophobic silica aerogels. Volume of water droplet is 10 μL. Scale bar: 1 cm. Source data are provided as a Source Data file.

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Solvent-regulable interfacial groups enable on-demand superhydrophobic/superhydrophilic silica aerogels
  • Article
  • Full-text available

March 2025

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14 Reads

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1 Citation

Lixiao Chen

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Lishan Li

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Xuetong Zhang

Silica aerogel, as the earliest synthetic and commercially available one among all known aerogels, holds significant value in fields including thermal and acoustic insulation, optics, catalysis, sorption, etc. However, throughout its nearly century-long history, the influence of solvent used during synthesis on the properties of silica aerogels has been neglected, resulting in inaccurate and ambiguous performance evaluation. Herein, we have uncovered and systematically investigated the solvent-regulable interfacial groups that enable on-demand superhydrophobicity/superhydrophilicity of silica aerogels. During either sol-gel transition or solvent exchange process both required for aerogel synthesis, the alteration of solvent either from water to ethanol or vice versa leads to silica interfacial groups switch from superhydrophilic Si-OH to superhydrophobic Si-OEt or reversely due to reversible esterification, thus enabling on-demand superhydrophobic/superhydrophilic silica aerogels. It is worth noting that on-demand solvent-regulated hydrophilicity/hydrophobicity holds true regardless of used silica precursors (the mixture of trimethoxymethylsilane (MTMS)/tetramethoxysilane (TMOS), MTMS/tetraethyl orthosilicate (TEOS), or sodium methicosilicate (SMS)/TMOS), thereby indicating its universality, which wakes up considerable attention for producers involved in silica aerogels. Additionally, the discovery also provides a green, economical, and efficient way to achieve silica aerogels with on-demand hydrophilic/hydrophobic performance for specific sorption, etc.

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Hierarchical architecture in natural woods and schematics for fabricating HPCCA that enables efficient flow electrochemistry. a) Photo images and CT‐scanned structures of natural woods. i) A photo image of a camphor tree. ii) A photo image of the sliced and well‐dried trunk. iii) CT‐scanned trunk structure exhibiting typical xylem and phloem parts. x‐y plane iv) and z‐y plane v) of the CT‐scanned structure. b) Fabrication pathway of HPCCA. The hierarchical porous structure is obtained via sol‐gel transition accompanied by multiphase co‐separation, followed by freeze‐drying and carbonization. c) HPCCAs work as electrodes in redox flow batteries and enable efficient flow electrochemical reactions. Compared with commercial carbon paper and bare aerogel without microchannels, HPCCA possesses a high active area, efficient mass transfer behavior, fast reaction kinetics, outstanding efficiency, scalability, and universality. A and A' represent active species with different valences at the anode, B and B’ represent active species with different valences at the cathode, and C represents the counterions.
Microstructure and surface chemistry characterization of HPCCA. a) Schematic diagram of HPCCA with structure hierarchy and rich chemical active sites. b‐e) SEM cross‐sectional morphology of HPCCA under different magnifications. f) The impact of diffusion directions on the orientation of microchannels. g) Elemental distributions of C, O, and N on the cross‐section of HPCCA. h) Pore size distribution curves extracted from mercury intrusion porosimetry results. High‐resolution i) C1s and j) N1s XPS spectra of HPCCA‐3, which is carbonized at 900 °C.
Mass transfer performance characterization of HPCCA. a) Schematic diagram of liquid penetration and wet‐ting process characterization for BA and HPCCA. b) Pressure drop with water as the fluid using an interdigitated flow field. c) Permeability of HPCCA‐1, HPCCA‐2, and HPCCA‐3. The error bars represent the standard deviation from three independent measurements (n = 3). d) Nyquist plot for 3.5 M H2SO4 in BA, HPCCA‐1, HPCCA‐2 and HPCCA‐3. e) Tortuosity of BA, HPCCA‐1, HPCCA‐2 and HPCCA‐3. f) Effective diffusion coefficient of H⁺, HSO4⁻, SO4²⁻, V²⁺/V³⁺, and VO²⁺/VO2⁺ in HPCCA‐1, HPCCA‐2, HPCCA‐3, and BA. g) Schematics illustrating the ion transport pathways in BA and HPCCA. h) Distributions of VO²⁺ in the bulk electrolyte for BA (top) and HPCCA (down). i) Ion flux of H⁺, HSO4⁻ and SO4²⁻ for BA and HPCCA, respectively.
Electrochemical analysis of HPCCAs as electrode materials. a) Schematic diagram of the metal‐free catalysis of O, N heteroatoms for HPCCA electrode reactions. b) Capacitance measurements for HPCCAs to determine the electrochemically accessible surface area in 3.5 M H2SO4 electrolyte. c) CV curves of HPCCAs toward VO²⁺/VO2⁺ redox couples at 2 mV s⁻¹. Insets show the photo images of solutions containing VO²⁺ and VO2⁺, and the scale bar is 1 cm. d) Nyquist plots of HPCCA toward VO²⁺/VO2⁺ redox reaction. e) Peak current versus square root of scan rate of HPCCAs toward VO²⁺/VO2⁺ redox couples. f) CV curves of HPCCAs toward V³⁺/V²⁺ redox couples at 2 mV s⁻¹. Insets show the photo images of solutions containing V³⁺ and V²⁺, and the scale bar is 1 cm. g) Nyquist plots of HPCCA toward V³⁺/V²⁺ redox reaction. h) Peak current versus square root of scan rate of HPCCAs toward V³⁺/V²⁺ redox couples.
Single‐cell redox flow battery performance based on HPCCA. a) Polarization curves for HPCCA‐3 and bare aerogel (BA). b) The response line of the overpotential for HPCCA‐3 and BA at different current densities. c) Charge–discharge curves for HPCCA‐3 at different current densities. d) Voltage efficiency of HPCCA‐3 and BA at 50–200 mA cm⁻². e) Energy efficiency of HPCCA‐3 and BA at 50–200 mA cm⁻². f) Energy efficiency comparison among the state‐of‐the‐art carbon electrodes.[26,46–59] g) Cycle performance of the VFB using HPCCA‐3 at 200 mA cm⁻². Inset: Optical photograph of a single cell and flow channel utilized in battery characterization. h) Energy efficiency of various FB single cell systems by using HPCCA‐3 and commercial material Toray TGP‐H60 as the electrodes, including active species of iron/chromium (Fe/Cr), zinc/bromine (Zn/Br), iron/vanadium (Fe/V), vanadium/methylene blue (V/MB), sodium salt of flavin mononucleotide/potassium ferrocyanide (FMN‐Na/K4[Fe(CN)6]), methyl viologen/4‐hydroxy‐2,2,6,6‐tetramethyl‐piperidin‐1‐oxyl (MV/4‐HO‐TEMPO), and all‐vanadium (all V).
Hierarchically Porous Carbon Colloidal Aerogels for Highly Efficient Flow Cells

December 2024

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23 Reads

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1 Citation

Electrodes with high active areas often compromise with limited ion transport kinetics in flow electrochemical devices. Herein, hierarchically porous carbon colloidal aerogels (HPCCAs) are constructed with multiscale porosities to meet the tradeoff between highly active areas and efficient mass transfer behavior. It is realized by introducing multiphase co‐separation in a sol‐gel transition process of aramid nanofibers/polyvinylpyrrolidone/carbon nanotubes followed by subsequent freeze‐drying and carbonization. The resulting HPCCA possesses a high volumetric electrochemically accessible surface area (3.27 × 10⁷ m⁻¹) and excellent mass transfer efficiency, 2–3 times higher permeability than commercial Toray carbon paper and 9.86 times higher than bare aerogel. An all‐vanadium single cell with HPCCAs as electrodes possesses a high energy efficiency of 83.18% under the current density of 100 mA cm⁻², which is 10–31% higher than most of the state‐of‐the‐art carbon electrode materials including commercial carbon papers. In addition, the cell with HPCCAs shows outstanding long‐term stability up to 1000 cycles. Notably, HPCCAs are applicable to more flow battery systems, such as iron/chromium (Fe/Cr), iron/vanadium (Fe/V), zinc/bromine (Zn/Br), vanadium/methylene blue (V/MB), sodium salt of flavin mononucleotide/potassium ferrocyanide (FMN‐Na/K4[Fe(CN)6]), and methyl viologen/4‐hydroxy‐2,2,6,6‐tetramethyl‐piperidin‐1‐oxyl (MV/4‐HO‐TEMPO). This work offers a new chemistry paradigm for developing advanced nanoporous aerogel materials and paves the way toward highly efficient flow electrochemical devices.


Design and results of superblacks. a) Optical photo of the synthesized transparent URSA with 10 cm × 10 cm × 1 cm. b) Reflectance of the resulting silica aerogels synthesized with different catalyst/molecular precursor molar ratios. c) Refractive index curves of URSA, air, water, and PDMS in the visible spectrum measured by the laser Fraunhofer method. d) Optical photo of the URSA/MXene superblack with a diameter of 10 cm and thickness of 1 cm. e) Light absorbance comparison among URSA/Ti3C2 MXene, URSA/Ti3AlC2 MAX, and URSA. f) Average visible light (380–780 nm) absorbance of URSA/MXene samples with different thicknesses. g) Optical photos of various suspending matrixes (including semitransparent silica aerogel (STSA), super‐white silica aerogel (SWSA), aramid nanofiber aerogel (ANFA), and polyvinyl alcohol (PVA) hydrogel) with light absorbing Ti3C2 MXene. h) Visible light (380–780 nm) absorbance curves of various suspending matrixes (URSA, STSA, SWSA, ANFA, and PVA hydrogel) with light‐absorbing Ti3C2 MXene.
Semiconductive LNs‐based superblacks. a) Schematic illustration of visible light photons in the electromagnetic spectrum. b) The relationship among bandgap (Eg), wavelength, and absorbance of semiconductive LNs. c) Absorbance spectrum illustration of semiconductive LNs‐based superblacks with different Eg: Fe2O3 (2.2 eV), TiO2 (3.2 eV), Fe3O4 (0.1 eV). d) Various superblacks derived from semiconductive LNs with different Eg: Fe3O4 (0.1 eV), WS2 (1.35 eV), MnO2 (0.25 eV), black phosphorus (BP, 0.3 eV), polyaniline (PANI, 0.6 eV), PdO (1.0 eV), CuO (1.2 eV), MoS2 (1.2 eV), PtO2 (1.3 eV). e) The magnetic hysteresis loop of the resulting superblack URSA/Fe3O4, inset photograph was URSA/Fe3O4 suspended in the air under the assistance of magnet and transparent tape.
Conductive LNs‐based superblacks, suspending various conductive LNs in URSA and obtaining various superblacks. a) Schematic illustration of UV–Vis–IR light photons in the electromagnetic spectrum. b) Absorbance spectra of URSA/MWCNT, URSA/C, and URSA/Pt in the UV–Vis–IR regions, all of them exhibited near‐complete absorption in UV–Vis–IR regions. C–e) SEM images of superblacks with 0D Pt, 1D MWCNT, and 2D Ti3C2 MXene, LNs with different dimensions can be suspended in the porous network of silica aerogel. f) Average absorbance values of URSA/0D Pt, URSA/1D MWCNT, and URSA/2D Ti3C2 MXene with different volume fractions in the wavelength range of 380–780 nm. g) Absorbance of URSA/MWCNT before and after heat treatment at 600 °C. Inset is optical and infrared photos of URSA/MWCNT in a tube furnace at 600 °C for 6 h, the absorbance and shape preserved very well after heat treatment. h) Transmission electron microscope images of URSA/Pt before and after heat treatment at 600 °C for 6 h, Pt nanoparticles still are nano‐size without sintering/melting together after heat treatment.
The universality and unique performance of URSA/LNs superblacks. a) Numerous superblacks can be fabricated in theory by the arbitrary combination of LNs with different dimensions (0D, 1D, and 2D) and different chemical components (organic and inorganic) in the URSA matrix. b) Ultra‐light superblacks standing on a rose, indicating the low density of superblacks. Scale bar in b: 2 cm. c) Photographs of the laser spot with a power of 1 W irradiated on the surface of SWSA (upper left) and superblacks (upper right), illustration (left bottom), and photographs of the laser spot with a power of 1 W irradiated inside the superblack with a hole. As the laser irradiated inside the superblack, this laser spot is invisible, indicating the complete absorption of the laser in the superblack hole, which might mimic the black hole in the universe. Scale bar in c: 2 cm. d) Optical photos of superblacks and PDMS/iron oxide blue models with different 3D structures at different angles, indicating that the surface details of superblacks are invisible while the surface details of blue models are evident. e) Concentration‐time curves of Rhodamine B in different circumstances, including solar irradiation (orange curve), superblack (blue curve), and co‐existing (red curve) of solar irradiation and superblack. Inset photos are the Rhodamine B solution before and after the reaction under the co‐assistance of superblack and solar irradiation. f) Mass change of water (orange curve) and ethanol (red curve) with hydrophilic superblacks, and hexane (blue curve) with hydrophobic superblacks over time under solar illumination of 1.0 sun. g) contact angle images of water (I) and hexane (II) on hydrophobic URSA/MWCNT. Scale bar in d,e: 2 cm.
Schematic illustration of the design and fabrication of superblacks. a) Light transmitting to various LNs‐based architectures with different configurations including stacked together, dispersed in the solid dense matrix, sparsely arrayed in the pattern, and suspended in the air, leading to light absorbance with different degrees. b) A novel universal strategy to create numerous superblacks by suspending Ti3C2 MXene or other 99 species of LNs in the ultra‐low reflective silica aerogel with ultra‐high light transparency.
Suspending Light‐Absorbing Nanoparticles in Silica Aerogel Enables Numerous Superblacks

December 2024

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35 Reads

Current strategies for constructing sparse nanostructures for fabricating superblacks are only suitable for a few light‐absorbing materials, severely limiting their applications. Herein, ultra‐low reflective silica aerogels with ultra‐high light transparency are used as solid smokes to individually or simultaneously suspend at least 100 species of light‐absorbing nanoparticles with a volume fraction as low as 0.005%, for creating > 100 superblacks in practice and one billion superblacks in theory if taken permutation and combination among these 0D, 1D, or 2D nanoparticles into account. Depending on the composition of suspended nanoparticles and the structure of solid smoke, the resulting mechanically robust superblacks with supplementary properties including magnetism, full‐spectrum absorption, high thermal stability, and excellent mechanical strength, are first observed. The wide choice of metallic or semiconductive LNs allows as‐made superblacks to glitter in different catalytic reactions, and the resulting superblacks have been on‐demand modified for endowing the self‐cleaning performance in some contaminable environments. Benefiting from the superblack feature and porous network, these superblack monoliths have shown high‐efficiency solar‐heat conversion in some emerging light harvesting and managing fields. This powerful synthetic strategy for superblacks is expected to inspire researchers to conduct in‐depth investigations on super‐black optics, functional materials, etc.



Transparent Silica Aerogels: Optical and Chemical Design, Controlled Synthesis, and Emerging Applications

August 2024

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120 Reads

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1 Citation

Transparent silica aerogel, serving as one typical porous and transparent material, possesses various unique features (e. g., large amounts of pores and interfaces, super‐lightweight, super thermal insulation, low refractive index similar to gas), and it has attracted great attention in the fields of science, technology, engineering, art, and others. Transparency is one important evaluation index of transparent silica aerogel, and it was influenced by various factors such as raw materials, sol‐gel reactions, phase separation, and drying methods. The structure design and fabrication of transparent silica aerogel is one huge and fine engineering. In this review, the optical/chemical guidance and design for the preparation of transparent silica aerogels are discussed, and typical applications, such as Cherenkov detectors, solar energy collection, lighting systems, and transparent fabric, were also discussed. Finally, a future outlook on the opportunities and challenges of transparent silica aerogels was proposed.


Features of the ANF spinning dopes. a) Apparent viscosity of ANF dispersions with different content of water as a function of shear rate. b) Modulus of ANF dispersions different content of water as a function of shear stress. c) Modulus of ANF‐6%H2O as a function of shear stress under different temperature. d) Schematic diagram of the effect of a small amount of water on the ANF dispersion, and mechanism diagram of the sol‐gel transition process. e) The force analysis of spinning dope during centrifugal spinning. f) The critical rotation speed of different ANF spinning dope. Five experiments were conducted for each concentration to calculate the statistically average values. g) Spinning speed comparison of the SCS strategy with previously reported spinning methods.[13–15,17,20,21]
Characterizations of the SCS ANF gel fibers and aerogel fibers. a) Photograph of the SCS ANF gel fibers. b) Optical microscope photograph of the SCS ANF gel fibers. c) Diameter distribution of the SCS ANF gel fibers. One hundred data were collected to acquire the diameter distribution of each type of SCS ANF gel fiber. d) The surface SEM image of the SCS ANF aerogel fibers. The inset is the photograph of the SCS ANF aerogel fibers. e) The cross‐section SEM images of the SCS ANF aerogel fibers. f) The polarization microscope image of the SCS ANF aerogel fibers. g) Nitrogen adsorption–desorption isotherms of the SCS ANF aerogel fibers. h) The pore volume distribution of the SCS ANF aerogel fibers. i) Stress–strain curves of the individual SCS ANF aerogel fibers.
Generality demonstration of the SCS Strategy. a) Surface SEM image of the SCS sodium alginate aerogel fibers. b) Cross‐section SEM image of the SCS sodium alginate aerogel fibers. c) Surface SEM image of the SCS cellulose aerogel fibers. d) Cross‐section SEM image of the SCS cellulose aerogel fibers. e) Surface SEM image of the SCS chitosan aerogel fibers. f) Cross‐section SEM image of the SCS chitosan aerogel fibers. g) Nitrogen adsorption–desorption isotherms of the SCS sodium alginate aerogel fibers, cellulose aerogel fibers, and chitosan aerogel fibers. h) The pore volume distribution of the SCS sodium alginate aerogel fibers, cellulose aerogel fibers, and chitosan aerogel fibers. i) The specific surface area of the SCS sodium alginate aerogel fibers, cellulose aerogel fibers, and chitosan aerogel fibers. Three samples for each type of the SCS aerogel fiber were measured to obtain their reliable specific surface area.
VOCs adsorption performance of the aramid aerogel fibers. a) Schematic diagram of the measuring setup for VOCs adsorption performance of the aramid aerogel fibers. b) Schematic illustration of the VOCs adsorption mechanism. c) The pressure before and after adsorption bed. d) The VOCs adsorption capacity of the aramid aerogel fibers and other adsorbent materials (i.e., nanocrystal minerals, molecular sieves, active carbon fibers, and aramid aerogel powder). Three samples were measured for each condition in order to acquire the statistically reliable values. e) Adsorption curve of the aramid aerogel fibers for ethanol. The inset is the corresponding adsorption speed. f) Breakthrough curve at ambient temperature for ethanol. g) The cycle stability of the aramid aerogel fibers during the 5 cycles of VOCs adsorption–desorption procedure. h) The adsorption capacity of the aramid aerogel fibers for various VOCs (i.e., o‐xylene, formaldehyde, acetone, and ethyl acetate, respectively). Three experiments were conducted for each condition.
Schematic description of the fabrication of the aerogel fibers via SCS strategy and the application. a) Schematic fabrication of the SCS strategy towards aerogel fibers. b) Schematic diagram of dynamic removal of VOCs with the SCS aerogel fiber‐aggregates.
Aerogel Fibers Made via Generic Sol‐Gel Centrifugal Spinning Strategy Enable Dynamic Removal of Volatile Organic Compounds From High‐Flux Gas

August 2024

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64 Reads

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7 Citations

Aerogels with ultrahigh porosity and large specific surface area have demonstrated great potential for capturing volatile organic compounds (VOCs). Especially, aerogel fiber aggregates with macropores formed by overlapping aerogel fibers and mesopores in the aerogel fibers might realize fast sorption kinetics and high sorption capacity simultaneously. However, how to develop fast fabrication and large‐scale production of aerogel fibers remains a challenge. Herein, a generic sol‐gel centrifugal spinning (SCS) strategy with a spinning rate capable of reaching 700 m min⁻¹ is developed for producing aerogel fibers. The representative SCS aerogel fiber made from aramid nanofiber (ANF) dispersion exhibits a large specific surface area (313 m² g⁻¹) and high tensile strength (12.48 MPa). The SCS strategy is further applied to fabricate various kinds of aerogel fibers, including sodium alginate, cellulose, and chitosan. The ANF aerogel fiber aggregates exhibit superior VOC adsorption capacity of 438.0 mg g⁻¹ under an ultrafast gas flux of 3.8 × 10⁴ L m⁻² h⁻¹, which also has satisfactory cyclic stability. This work not only develops a powerful and generic strategy for fabricating aerogel fibers in large scale, but also provides inspiration for applying these SCS aerogel fibers in dynamic removal of VOCs and other environmental protection fields.


Aerogel‐Involved Triple‐State Gels Resemble Natural Living Leaves in Structure and Multi‐Functions

June 2024

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65 Reads

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17 Citations

Natural plant leaves with multiple functions, for example, spectral features, transpiration, photosynthesis, etc., have played a significant role in the ecosystem, and artificial synthesis of plant leaves with multiple functions of natural ones is still a great challenge. Herein, this work presents an aerogel‐involved living leaf (AL), most similar to natural ones so far, by embedding super‐hydrophobic SiO2 aerogel microparticles in polyvinyl alcohol hydrogel in the presence of hygroscopic salt and chlorophyllin copper sodium to form solid‐liquid‐vapor triple‐state gel. The AL shows a high spectral similarity with all sampled 15 species of natural leaves and exhibits ≈4–7 times transpiration speed higher than natural leaves. More importantly, AL can achieve several times higher photosynthesis than natural leaves without the energy provided by the respiratory action of natural ones. This work demonstrates the feasibility of creating ALs with natural leaf‐like triple‐state gel structures and multiple functions, opening up new avenues for energy conversion, environmental engineering, and biomimetic applications.


Schematic illustration of the aerogel‐confined liquid‐based composite membrane for highly efficient uranium capture. a) The establishment of the aerogel‐confined liquid‐based composite membrane (ALCM). Aerogel pore provides sufficient nanoconfinement space for the uranium‐specific functional liquid, and the functional liquid is preferentially wet and adheres to the solid counterpart. b) Selective uranium ion capture enabled by ALCM. The specific binding motifs are formed by the coordinating ligands (tributyl phosphate and calix[6]arene), uranyl ion, and NO3⁻. c) Alternative pressure‐enhanced ion transport at the dynamic liquid‐liquid interface, greatly reducing the thickness of the aqueous diffusion layer. df and df’ represent the thickness of the aqueous diffusion layer at the feeding solution/functional liquid interface, whereas dr and dr’ represent the thickness of the aqueous diffusion layer at the functional liquid/receiving solution interface without and with the alternating pressure, respectively. ΔP stands for the alternative pressure, which should be below the critical pressure for permeating feeding solution through aerogel membrane (PFS, critical).
Characterization of aerogel‐confined liquid‐based composite membranes, the interface design, and the interface stability. a) Cross‐sectional SEM image of Kevlar aerogel membrane. Macroscopic photo of the membrane (Inset). b) N2 adsorption‐desorption isotherms of original Kevlar aerogel membrane (KAM), densified Kevlar aerogel membrane (DKAM), and further fluorocarbon functionalized Kevlar aerogel membrane (FKAM). c) FI‐IR spectra of KAM, FKAM, and its solid‐liquid host‐guest membrane (ALCM). d) Tensile stress‐strain curves of aerogel membrane KAM and solid‐liquid host‐guest membrane (ALCM). e) AFM 2D topography of the i) solid porous membrane, ii) liquid layer, and iii) the underlying porous matrix of ALCM. iv) 3D topography of the liquid layer and v) underlying porous matrix of ALCM. f) AFM force curve indicating the liquid thickness infused in the aerogel membrane. Schematic illustration of the AFM tip at variant areas of the ALCM (inset). g) Work of adhesion between the uranyl‐specific functional liquid and aerogel solid film. h) Critical pressures for air permeating the bare aerogel membrane and ALCM, compared with the analogous commercial PTFE ones. The inset shows a schematic illustration of gas intrusion process and the recovery of functional liquid after the pressure is released. i) The cycle stability for air transporting through the ALCM. The inset shows a typical gas permeation curve, including the gas permeation status and functional liquid recovery status.
The binding mechanism between uranyl ion and tributyl phosphate (TBP) as well as calix[6]arene (C6) in the functional liquid of ALCMs. a) The molecular structure and ball‐stick model of TBP and C6. b) Molecular Dynamic calculations of the uranium capture, with the coordinating moiety of i) 4TBP+UO2²⁺+NO3⁻, ii) C6+UO2²⁺+NO3⁻, and iii) C6+TBP+UO2²⁺+NO3⁻. c–f) ¹H NMR spectroscopy showing the complexation between TBP and UO2²⁺, as well as the binding between C6 and UO2²⁺. g) Impedance spectra of ALCMs using TBP or C6/TBP as the functional liquid. h) UV–vis absorption spectra of the receiving solution after 6 days’ diffusion adopting TBP or C6/TBP in ALCMs.
The tunability, ion selectivity, and cyclic performance of ALCMs. a) Schematic illustration of the influential factors that determine the uranium extraction by ALCMs. b) UV–vis spectra profile of uranium receiving solution with increasing extraction time. The inset shows the spectra intensity in relation to uranyl ion concentrations. c) The influence of aerogel membrane thickness on the uranyl capture concentration. d) Effect of the coordination agents on the uranium capture concentration. e) The uranium concentration in the original feeding solution and receiving solution after 10 h based on variant UO2²⁺:C6 molar ratios. f) UV–vis spectra of uranium receiving solution from pure UO2(NO3)2 solution and ion mixtures with competing cations. The inset shows the extraction rate in these two conditions. g) The selectivity of uranium with competing ions in HNO3‐based solutions. Photos of ion mixture as the feeding source and captured UO2²⁺ in receiving solution (inset). The error bars represent the standard deviation from three independent measurements (n = 3). h) The selectivity of uranium with competing ions in uranium‐spiked natural seawater. Photos of U‐spiked natural seawater as the feeding source and captured UO2²⁺ in receiving solution (inset). The error bars represent the standard deviation from three independent measurements (n = 3). i) The uranium extraction stability of ALCMs after multiple cycles of operation.
Alternating pressure‐enhanced uranyl ion transport, antifouling behavior, and endurance of ALCMs in extreme conditions. a) Schematics of alternating pressure‐enhanced uranyl ion transport. b) Influence of alternating pressure on the uranium extraction compared with pure diffusion in the interval of 1 h. c) The frequency effect of alternating pressure on the uranium extraction for 1 h. d) The comparison between alternating pressure‐enhanced ion transport and ion diffusion. e) The concentration profile of the ALCMs without and with the alternating pressure. The contour images in the case of with and without the alternating pressure (Inset). f) Uranium extraction efficiency under different dynamic interface regulating methods. The error bars represent the standard deviation from three independent measurements (n = 3). g) Uranium extraction efficiency compared with reported sorbent materials. h) Antifouling behavior of ALCMs. i) The stability of ALCMs encountering extremely alkaline, acidic, and highly salty conditions.
Kevlar Aerogel‐Confined Functional Liquid‐Based Composite Membrane Enables Dynamic Uranium Capture

May 2024

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Solid–liquid composite materials that confine a functional liquid within a porous solid have appeared in a wealth of emerging applications. However, creating dynamic liquid interfaces for efficient ion capture while stably retaining functional liquid in porous confinements is challenging. Here, an aerogel‐confined liquid‐based composite membrane (ALCM) for dynamic and highly efficient uranium capture is reported. As a proof of concept, Kevlar aerogel membrane is selected as the nanoporous solid, and calix[6]arene/tributyl phosphate (C6/TBP) is used as the guest liquid. The obtained ALCMs possess high stability, optimum adhesion between solid‐liquid interface, and high selectivity for uranyl ions (250–6510 times over other competing ions). Different dynamic interface regulating approaches are explored for ALCMs, and uranium extraction efficiency under alternating pressures can be up to 258.48 mg g⁻¹ h⁻¹, outperforming many reported uranium capture materials. This strategy can be applicable to develop a rich family of solid‐liquid composite materials and may spearhead a new paradigm for uranium capture from sustainable seawater resources.


Citations (79)


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