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Publications (611)
MXenes represent one‐of‐a‐kind materials to devise radically novel technologies and achieve breakthroughs in optoelectronics. To exploit their full potential, precise control over the influence of stoichiometry on optical and thermal properties, as well as device performance, must be achieved. Here, the characteristics of optoelectronic devices bas...
We present a novel, portable sensor platform that enables concurrent monitoring of surface mass and charge density variations at thin biointerfaces. This platform combines a coplanar-gated field-effect transistor (FET) architecture with grating-coupled surface plasmon resonance (SPR), yielding an integrated disposable sensor chip prepared by nanoim...
In the brain, both the recording and decaying of memory information following external stimulus spikes are fundamental learning rules that determine human behaviors. The former is essential to acquire new knowledge and update the database, while the latter filters noise and autorefresh cache data to reduce energy consumption. To execute these funct...
Two-dimensional conjugated metal–organic frameworks (2D c-MOFs) have emerged as an intriguing class of quantum materials due to their high crystallinity, persistent spin centers, and tunable structures and topologies. However, it remains unclear how to achieve long spin relaxation time at room temperature in 2D c-MOFs via a bottom-up design strateg...
2D polymeric fullerene scaffolds, composed of covalently bonded superatomic C60 nanoclusters, are emerging semiconductors possessing unique hierarchical electronic structures. Hitherto their synthesis has relied on complex and time‐consuming reactions, thereby hindering scalable production and limiting the technological relevance. Here, the study d...
Despite advances in the field of 2D polymerization, the synthesis of high-quality, micrometre-thick films of oriented 2D covalent organic frameworks (COFs) remains challenging. Conventional approaches focusing on thermodynamic control of the polymerization pathway face a detrimental trade-off between orientation and thickness. Here we describe a st...
The controlled formation of a functional adlayer at the catalyst‐water interface is a highly challenging yet potentially powerful strategy to accelerate proton transfer and deprotonation for ultimately improving the performance of proton‐exchange membrane water electrolysis (PEMWE). In this study, the synthesis of robust vinylene‐linked covalent or...
The Graphene Flagship aimed at demonstrating the viability and performance of graphene in e-textile applications where mechanical properties such as flexibility and stretchability as well as sustainability have a crucial role. In this perspective we will discuss the Graphene Flagship work on GRM-containing conductive textile fibres, yarns, and fabr...
Many high-performance perovskite solar cells (PSCs) rely heavily on halogenated antisolvent methods, hampering their potential commercialization. In this work, the industry-compatible dimethyl sulfide (DMS) solvent, which coordinates strongly with the metal cation, is used in a bathing approach to investigate the crystallization of triple halide pe...
Isomer discrimination is of paramount importance across various sectors, including pharmaceuticals, agriculture, and the food industry, owing to their unique physicochemical characteristics. Because of their extremely similar characteristics, traditional analytical methods fail or encounter severe limitations in isomer discrimination. To overcome t...
sp²-carbon-linked covalent organic frameworks (sp²c-COFs) are crystalline porous polymers with repeat organic units linked by sp² carbons, and have attracted increasing interest due to their robust skeleton and tunable semiconducting properties. Single-crystalline sp²c-COFs with well-defined structures can represent an ideal platform for investigat...
Four distinct zeolitic imidazolate frameworks (ZIFs) are prepared using zinc and cobalt ions with 2-aminobenzimidazole and 2-methylimidazole as linkers to explore their electrochemical properties as platforms for aldehyde detection. The...
Covalent organic frameworks (COFs) are highly porous, thermally and chemically stable organic polymers. Their high porosity, crystallinity, and adjustable properties make them suitable for numerous applications. However, COFs encounter critical challenges, such as their difficult processability, self‐stacking propensity, low electrical conductivity...
High contact resistance remains the primary obstacle that hinders further advancements of organic semiconductors (OSCs) in electronic circuits. While significant effort has been directed toward lowering the energy barrier at OSC/metal contact interfaces, approaches toward reducing another major contributor to overall contact resistance – the bulk r...
Pressure sensing is a crucial technique for various biomedical applications, where it can provide valuable information about the health and function of different organs and systems. This paper reports the development of a novel integrated pressure sensor based on modified rGO, a graphene-derivative material with enhanced piezoresistive properties....
Entropy, a measure of disorder or uncertainty in the thermodynamics system, has been widely used to confer desirable functions to alloys and ceramics. The incorporation of three or more principal elements into a single sublattice increases the entropy to medium and high levels, imparting these materials a mélange of advanced mechanical and catalyti...
High‐work function transparent electrodes (HWFTEs) are key for establishing Schottky and Ohmic contacts with n‐type and p‐type semiconductors, respectively. However, the development of printable materials that combine high transmittance, low sheet resistance, and tunable work function remains an outstanding challenge. This work reports a high‐perfo...
Monitoring the cardiovascular health of patients and early diagnosis of heart diseases are highly sought after as they can represent a true cornerstone in tomorrow's healthcare surveillance. Here, an unprecedented non‐invasive device prototype is reported for pulse wave velocity (PWV) measurement based on a piezoelectric graphene pressure sensor. P...
Proton chemistry is becoming a focal point in the development of zinc‐ion energy storage devices due to its swift H⁺ insertion/extraction kinetics. This characteristic feature confers to electrodes a remarkable power density, rate capability, and prolonged cycling durability. However, the storage mechanism of H⁺ in electrodes based on covalent‐orga...
Two-dimensional (2D) in-plane heterostructures display exceptional optical and electrical properties well beyond those of their pristine components. However, they are usually produced by tedious and energy-intensive bottom-up growth approaches, not...
The optically tuneable nature of hybrid organic/inorganic heterostructures tailored by interfacing photochromic molecules with 2D semiconductors (2DSs) can be exploited to endow multi‐responsiveness to the exceptional physical properties of 2DSs. In this study, a spiropyran‐molybdenum disulfide (MoS2) light‐switchable bi‐functional field‐effect tra...
Anthraquinone-based hollow COFs (COF shells) were synthesized via template-assisted method involving polystyrene nanospheres as hard template, which enabled doubling the specific capacitance and energy density compared to non-templated COFs. Our...
Manipulating and exerting a nanoscale control over the structure of multicomponent materials represents a powerful strategy for tailoring multifunctional composites for structural health monitoring applications. The use of self-sensing, electroactive...
Hybrid systems based on graphene and organic molecules are highly appealing for “correcting” the limited optoelectronic properties of the 2D material. However, in-depth understanding of the correlation between the structure...
Materials combining stretchability and sensitivity to external stimuli are key for wearable electronics applications to enable the emergence of disruptive technologies in biosensing, health monitoring, photodetection and human motion recognition. Conductive organohydrogels have gained significant attention due to their high sensitivity and cost‐eff...
Conspectus
Two-dimensional conjugated metal–organic frameworks (2D c-MOFs) have emerged as a novel class of multifunctional materials, attracting increasing attention due to their highly customizable chemistry yielding programmable and unprecedented structures and properties. In particular, over the past decade, the synergistic relationship betwee...
Molybdenum ditelluride (MoTe2) nanosheets have displayed intriguing physicochemical properties and opto-electric characteristics as a result of their tunable and small band gap (Eg ∼ 1 eV), facilitating concurrent electron and hole transport. Despite the numerous efforts devoted to the development of p-type MoTe2 field-effect transistors (FETs), th...
Aqueous zinc‐ion hybrid supercapacitors (Zn‐HSCs) are promising devices for sustainable and efficient energy storage. However, they suffer from a limited energy density compared to lithium‐ion batteries. This limitation can be overcome by developing novel electrode materials, with covalent organic frameworks (COFs) standing out as a particularly in...
The artificial brain is conceived as advanced intelligence technology, capable to emulate in‐memory processes occurring in the human brain by integrating synaptic devices. Within this context, improving the functionality of synaptic transistors to increase information processing density in neuromorphic chips is a major challenge in this field. In t...
Zinc hybrid supercapacitors (Zn‐HSCs) hold immense potential toward the next‐generation energy storage systems, effectively spanning the divide between conventional lithium‐ion batteries (LIBs) and supercapacitors. Unfortunately, the energy density of most of Zn‐HSCs has not yet rivalled the levels observed in LIBs. The electrochemical performance...
Zinc‐ion batteries (ZIBs) are promising energy storage systems due to high energy density, low‐cost, and abundant availability of zinc as a raw material. However, the greatest challenge in ZIBs research is lack of suitable cathode materials that can reversibly intercalate Zn²⁺ ions. 2D layered materials, especially MoS2‐based, attract tremendous in...
We demonstrate the synthesis and application of “clickable” graphene nanoribbons (GNRs) as a versatile interface for electrochemical biosensors.
Despite the rapid progress in the field of 2D polymerisation, the fabrication of high-quality films of 2D covalent organic frameworks (2D COFs) remains a longstanding challenge. Herein, we describe a two-stage method for preparing mechanically robust, large-area, porous, highly oriented, imine-linked 2D COF films from kinetically trapped, amorphous...
Despite the advancements in the field of 2D polymerization, the synthesis of high-quality films of oriented 2D covalent organic frameworks (2D COFs) remains a longstanding challenge. Herein, we describe a method for preparing robust, large-area, porous 2D COF films with near-perfect face-on orientation via amorphous covalent adaptable network (CAN)...
Despite the advancements in the field of 2D polymerization, the synthesis of high-quality films of oriented 2D covalent organic frameworks (2D COFs) remains a longstanding challenge. Herein, we describe a method for preparing robust, large-area, porous 2D COF films with near-perfect face-on orientation via amorphous covalent adaptable network (CAN)...
Despite advances in the field of 2D polymerization, the synthesis of high-quality, micron-thick films of oriented 2D covalent organic frameworks (COFs) remains challenging. Conventional approaches focusing on thermodynamic control of the polymerization pathway face a detrimental trade-off between orientation and thickness. In this study, we describ...
Supercapacitors and transistors are two key devices for future electronics that must combine portability, high performance, easy scalability, etc. Graphene‐related materials (GRMs) are frequently chosen as active materials for these applications given their unique physical properties that are tunable via chemical functionalization. Up to date, amon...
Ambipolar electrolyte‐gated transistors (EGTs) based on reduced graphene oxide (rGO) have been demonstrated as ultra‐sensitive and highly specific immunosensors. However, the physics and chemistry ruling the device operation are still not fully unraveled. In this work, the aim is to elucidate the nature of the observed sensitivity of the device. To...
Lithium–sulphur batteries (LSBs) prevail as a viable alternative to Li-ion batteries due to their high theoretical specific capacity (1672 mAh gS−1). However, the formation of soluble polysulfides and their shuttle...
Transition metal dichalcogenides (TMDs) are promising 2D materials which are attracting significant interest because of their distinctive physicochemical properties. The possibility of being exfoliated and dispersed in liquid solutions offers a viable pathway to scalable production. This personal account focuses on recent advancements in 2D TMD ink...
Thin film networks of solution processed nanosheets show remarkable promise for use in a broad range of applications including strain sensors, energy storage, printed devices, textile electronics and more. While it is known that their electronic properties rely heavily on their morphology, little is known of their mechanical nature, a glaring omiss...
Artificial synapses combining multiple yet independent signal processing strategies in a single device are key enabler to achieve high‐density of integration, energy efficiency and fast data manipulation in brain‐like computing. By taming functional complexity, the use of hybrids comprising multiple materials as active components in synaptic device...
Core-shell MOF@COF hybrids were synthesized via subsequent modification of MOF UiO-66-NH2 with 1,3,5-triformylphloroglucinol (TFP) and 2,3,5,6-tetraaminobenzoquinone (TABQ). The hybrids exhibited significant surface area (236m2/g) and outstanding electrochemical performance (103F/g at...
The coupling of different two‐dimensional materials (2DMs) to form van der Waals heterostructures (vdWHs) is a powerful strategy for adjusting the electronic properties of 2D semiconductors, for applications in opto‐electronics and quantum computing. 2D molybdenum disulfide (MoS 2 ) represents an archetypical semiconducting, monolayer thick versati...
The presence of oxygen-containing functional groups on the basal plane and at the edges endows graphene oxide (GO) with an insulating nature, which makes it rather unsuitable for electronic applications. Fortunately, the reduction process makes it possible to restore the sp2 conjugation. Among various protocols, chemical reduction is appealing beca...
![LC‐MS analysis (Extracted Ion Current (EIC) chromatograms of the [M+H]⁺...](publication/374480613/figure/fig3/AS:11431281245953473@1716258870657/LC-MS-analysis-Extracted-Ion-Current-EIC-chromatograms-of-the-M-H-ions-at-m-z-577_Q320.jpg)
Storing solar energy is a key challenge in modern science. MOlecular Solar Thermal (MOST) systems, in particular those based on azobenzene switches, have received great interest in the last decades. The energy storage properties of azobenzene (t1/2<4 days; ΔH~270 kJ/kg) must be improved for future applications. Herein, we introduce peptoids as prog...
The advent of immunotherapies with biological drugs has revolutionized the treatment of cancers and auto-immune diseases. However, in some patients the production of anti-drug antibodies (ADAs) hampers the drug efficacy. The concentration of ADAs is typically in the range of 1-10 pM, hence their immunodetection is challenging. We focus here on ADAs...
Electrochemical reactions represent essential processes in fundamental chemistry that foster a wide range of applications. Although most electrochemical reactions in bulk substances can be well described by the classical Marcus-Gerischer charge transfer theory, the realistic reaction character and mechanism in dimensionally confined systems remain...
Optically switchable field‐effect transistors (OSFETs) are non‐volatile photonic memory devices holding a great potential for applications in optical information storage and telecommunications. Solution processing of blends of photochromic molecules and π‐conjugated polymers is a low‐cost protocol to integrate simultaneously optical switching and c...
Electrochemical reactions represent essential processes in fundamental chemistry that foster a wide range of applications. Although most electrochemical reactions in bulk substances can be well described by the classical Marcus-Gerischer charge transfer theory, the realistic reaction character and mechanism in dimensionally confined systems remain...
Recent developments in the design and synthesis of more and more sophisticated organic building blocks with controlled structures and physical properties, combined with the emergence of novel assembly modes and nanofabrication methods, make it possible to tailor unprecedented structurally complex porous systems with precise multiscale control over...
Chiral molecules are known to behave as spin filters due to the chiral induced spin selectivity (CISS) effect. Chirality can be implemented in molecular semiconductors in order to study the role of the CISS effect in charge transport and to find new materials for spintronic applications. In this study, the design and synthesis of a new class of ena...
The unique electrochemical properties of polyoxometalates (POMs) render them ideal components for the fabrication of next‐generation high‐performance energy storage systems. However, their practical applications have been hindered by their high solubility in common electrolytes. This problem can be overcome by the effective hybridization of POMs wi...
The capability to finely tailor material thickness with simultaneous atomic precision and non-invasivity would be useful for constructing quantum platforms and post-Moore microelectronics. However, it remains challenging to attain synchronized controls over tailoring selectivity and precision. Here we report a protocol that allows for non-invasive...
The spatially precise integration of arrays of micro-patterned two-dimensional (2D) crystals onto three-dimensionally structured Si/SiO$_2$ substrates represents an attractive strategy towards the low-cost system-on-chip integration of extended functions in silicon microelectronics. However, the reliable integration of the arrays of 2D materials on...
The unique electrochemical properties of polyoxometalates (POMs) render them ideal components for the fabrication of next‐generation high‐performance energy storage systems. However, their practical applications have been hindered by their high solubility in common electrolytes. This problem can be overcome by the effective hybridization of POMs wi...
Graphene and related 2D material (GRM) thin films consist of 3D assembly of billions of 2D nanosheets randomly distributed and interacting via van der Waals forces. Their complexity and the multiscale nature yield a wide variety of electrical characteristics ranging from doped semiconductor to glassy metals depending on the crystalline quality of t...
Chemical sensing of water contamination by heavy metal ions is key as it represents a most severe environmental problem. Liquid‐phase exfoliated two‐dimensional (2D) transition metal dichalcogenides (TMDs) are suitable candidates for chemical sensing thanks to their high surface‐to‐volume ratio, sensitivity, unique electrical characteristics, and s...
The scarcity of fossil fuels calls for immediate action toward the development of clean and renewable energy resources. In this context, proton exchange membrane fuel cells (PEMFCs) are gaining ever‐increasing attention as clean technology. Although covalent organic frameworks (COFs) do not usually exhibit high intrinsic proton conductivity (σ), th...
The controlled chemical functionalization of graphene oxide (GO) represents a powerful strategy to finely tune its physical and chemical properties toward applications in energy storage. Herein, an unprecedented approach for the GO modification with thioamide‐based polymers featuring numerous heteroatoms (S,N,O) is reported, which is instrumental f...
During the last fifteen years, the reduction of electrically insulating graphene oxide (GO) through the elimination of oxygen containing functional groups and the restoration of sp2 conjugation yielding its conducting form, known as reduced graphene oxide (rGO), has been widely investigated as a scalable and low-cost method to produce materials fea...
Device performance of solution‐processed 2D semiconductors in printed electronics has been limited so far by structural defects and high inter‐flake junction resistance. Covalently interconnected networks of transition metal dichalcogenides potentially represent an efficient strategy to overcome both limitations simultaneously. Yet, the charge tran...
MXenes have recently emerged as a revolutionary class of material displaying exceptional tailored-made properties. The onward journey and remarkable rise are establishing MXene-based materials as multifaceted playgrounds for the technology-oriented explorations and are offering a tool-box for the ad hoc tailoring of advanced materials capable to ef...
Precise monitoring of the humidity level is important for the living comfort and for many applications in various industrial sectors. Humidity sensors have thus become one among the most extensively studied and used chemical sensors by targeting a maximal device performance through the optimization of the components and working mechanism. Among dif...
Transition metal carbides and nitrides (MXenes) are an emerging class of 2D materials, which are attracting ever‐growing attention due to their remarkable physicochemical properties. The presence of various surface functional groups on MXenes’ surface, e.g., F, O, OH, Cl, opens the possibility to tune their properties through chemical functionaliza...
Electrochemical reaction represents an essential action in fundamental chemistry that fosters wide applications. Although most electrochemical reactions involving bulk substances can be well described by the classical Marcus-Gerischer charge transfer theory, the realistic reaction character and mechanism in atomically confined systems remain unknow...
Two‐dimensional covalent organic frameworks (COFs) have emerged as promising materials for energy storage applications exhibiting enhanced electrochemical performance. While most of the reported organic cathode materials for zinc‐ion batteries use carbonyl groups as electrochemically‐active sites, their high hydrophilicity in aqueous electrolytes r...
The mutual conversion between light and electricity lies at the heart of optoelectronic and photonic applications. Maximization of the photoelectric conversion is a long-term goal which can be pursued via the fabrication of devices with ad-hoc architectures. In this framework it is of utter importance to harvest and transform light irradiation into...
Two‐dimensional covalent organic frameworks (COFs) have emerged as promising materials for energy storage applications exhibiting enhanced electrochemical performance. While most of the reported organic cathode materials for zinc‐ion batteries use carbonyl groups as electrochemically‐active sites, their high hydrophilicity in aqueous electrolytes r...
Rechargeable aqueous zinc-ion hybrid supercapacitors (Zn-HSCs) are promising candidates as large-scale energy storage devices owing to their high electrochemical performance, safety, long life, and low price. The development of nanostructured...
The design of novel organic electrochemical transistor (OECT) channel materials that can be controlled by a whole range of external stimuli is key towards the emergence of unprecedented technologies in...
We report the polymorph investigation, crystallographic study, and fabrication of organic field-effect transistors (OFETs) in solution-processed thin-films of a prototypical organic semiconductor, i.e., 2,7-diheptylbenzo[b]benzo[4,5]thieno[2,3-d]thiophene (C7-BTBT-C7). We found that this molecule...
Organic materials represent a promising alternative to critical raw materials for energy storage applications due to their sustainable production combined with tunable structures and functionalities. Unfortunately, the biggest limitation of...
Two-dimensional (2D) materials with the atomically thin thickness have attracted great interest in the post-Moore's Law era because of their tremendous potential to continue transistor downscaling and offered advances in device performance at the atomic limit. However, the metal-semiconductor contact is the bottleneck in field-effect transistors (F...
Neuromorphic engineering and artificial intelligence demands hardware elements that emulates synapse algorithms. During the last decay electrolyte‐gated organic conjugated materials have been explored as a platform for artificial synapses for neuromorphic computing. Unlike biological synapses, in current devices the synaptic facilitation and depres...
During the last 15 years, 2D materials have revolutionized the field of materials science. Moreover, because of their highest surface‐to‐volume ratio and properties extremely susceptible to their interaction with the local environment they became powerful active components for the development the high‐performance chemical sensors. By combining diff...
The use of postsynaptic current to drive long-lasting luminescence holds a disruptive potential for harnessing the next-generation of smart displays. Multiresponsive long afterglow emission can be achieved by integrating light-emitting polymers in electric spiked transistors trigged by distinct presynaptic signals inputs. Here, we report a highly e...
Tunable physicochemical properties combined with the high chemical and thermal stabilities of covalent organic frameworks (COFs) make them ideal candidates for the next generation of energy storage systems. The integration of redox-active moieties (e.g., thiols) in COFs imparts them a pseudocapacitive characteristic and represents an efficient stra...
The increasing population and industrial development are responsible for environmental pollution. Among toxic chemicals, polycyclic aromatic hydrocarbons (PAHs) are highly carcinogenic contaminants resulting from the incomplete combustion of organic materials. Two-dimensional materials, such as transition metal dichalcogenides (TMDCs), are ideal se...
Health monitoring is experiencing a radical shift from clinic‐based to point‐of‐care and wearable technologies, and a variety of nanomaterials and transducers have been employed for this purpose. 2D materials (2DMs) hold enormous potential for novel electronics, yet they struggle to meet the requirements of wearable technologies. Here, aiming to fo...
Well-defined π-conjugated thiophene donor-acceptor molecules play an important role in different fields ranging from synthetic chemistry to materials science. Their chemical structure provides specific electronic and physicochemical properties, which can be further tuned by the introduction of functional groups. Herein, we design and synthesize two...
This work describes the design and synthesis of a π‐conjugated telluro[3,2‐β][1]‐tellurophene‐based synthon that, embodying pyridyl and haloaryl chalcogen‐bonding acceptors, self‐assembles into nanoribbons through chalcogen bonds. The ribbons π‐stack in a multi‐layered architecture both in single crystals and thin films. Theoretical studies of the...
We report a fast and ultrasensitive colorimetric method for the detection of transition metal ions (Fe3+, Cu2+, Ni2+) in a mixture of toluene-acetonitrile using Schiff base functionalized gold nanoparticles. We...
The capability to finely tailor material thickness with simultaneous atomic precision and non-invasivity would be useful for constructing quantum platforms and post-Moore microelectronics. However, it remains challenging to attain synchronized controls over tailoring selectivity and precision. Here we report a protocol that allows for non-invasive...
Defect Engineering of Transition Metal Dichalcogenides The great variety of defects in solution‐processed transition metal dichalcogenides (TMDs) and their crucial influence on the physicochemical properties have recently prompted worldwide scientists to master their inherent features. In article number 2100122, Stefano Ippolito and Paolo Samorì re...
Human health can be affected by materials indirectly through exposure to the environment or directly through close contact and uptake. With the ever‐growing use of 2D materials in many applications such as electronics, medical therapeutics, molecular sensing, and energy storage, it has become more pertinent to investigate their impact on the immune...
The charge transport of crystalline organic semiconductors is limited by dynamic disorder that tends to localize charges. It is the main hurdle to overcome in order to significantly increase charge carrier mobility. An innovative design that combines a chemical structure based on sulfur‐rich thienoacene with a solid‐state herringbone (HB) packing i...
Organic light-emitting devices are key components for emerging opto- and nanoelectronics applications including health monitoring and smart displays. Here, we report a foldable inverted polymer light-emitting diode (iPLED) based on a self-suspended asymmetrical vertical nanoscaffold replacing the conventional sandwich-like structured LEDs. Our empt...
This work describes the design and synthesis of a p‑conjugated telluro[3,2‐ b ][1]‐tellurophene‐based synthon that, embodying pyridyl and haloaryl chalcogen‐bonding acceptors, self‐assembles into nanoribbons through chalcogen bonds. The ribbons π‐stack in a multi‐layered architecture both in single crystals and thin films. Theoretical studies of th...
