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Semiconductor electrocatalysis with weak conductivity can accumulate extremely high carriers at semiconductor-electrolyte interface by self-gating effect, which strongly promotes electrocatalytic efficiency. The correlation between semiconductor carrier mobility and electrocatalysis performance is still unclear. Herein atomic-thin transition metal dichalcogenides based composites have been developed for hydrogen evolution reaction (HER) performed with on-chip microdevices. Electrical and electrochemical measurement of individual flack verified the key role of high carrier mobility for enhanced HER activity. Carrier mobility regulation further demonstrated its high dependence with HER performance under self-gating. Our study provides new insight into the carrier mobility of the semiconductor in the electrocatalysis, paving the way for designing high-performance semiconductor catalysts.

Machine learning approach was employed to guide the fabrication of blue carbon dots(CDs) with excellent result. The quantum yield of the CDs can increase up to 200% and can be used as fluorescent probes for bleaching teeth H2O2 detection.

Compared to traditional rigid-bodied robots, soft robots are constructed using physically flexible/elastic bodies and electronics to mimic nature and enable novel applications in industry, healthcare, aviation, military,etc.

Strong, reversible, and self-cleaning adhesion in the toe pads of geckos allow the lizards to climb on a variety of vertical and inverted surfaces, regardless of the surface conditions, whether hydrophobic or hydrophilic, smooth or tough, wet or dry, clean or dirty. Development of synthetic gecko-inspired surfaces has drawn a great attention over the past two decades. Despite many external-stimuli responsive mechanisms (i.e., thermal, electrical, magnetic) have been successfully demonstrated, smart adhesives controlled by light signals still substantially lag behind. Here, in this report, we integrate tetramethylpiperidinyloxyl (TEMPO)-doped polydopamine (PDA), namely, TDPDA, with PDMS micropillars using a template-assisted casting method, to achieve both improved adhesion and self-cleaning performances. To the best of our knowledge, this is the first report on PDA being used as a doping nanoparticle in bioinspired adhesive surfaces to achieve highly efficient self-cleaning controllable by light signals. Notably, the adhesion of the 5% TDPDA-PDMS sample is ∼688.75% higher than that of the pure PDMS at the individual pillar level, which helps to explain the highly efficient self-cleaning mechanism. The sample surfaces (named TDPDA-PDMS) can efficiently absorb 808 nm wavelength of light and heat up from 25 °C to 80.9 °C in 3 min with NIR irradiation. The temperature rise causes significant reduction of adhesion, which results in outstanding self-cleaning rate of up to 55.8% within five steps. The exploration of the photoenabled switching mechanism with outstanding sensitivity may bring the biomimetic smart surfaces into a new dimension, rendering varied applications, e.g., in miniaturized climbing robot, artificial intelligence programmable manipulation/assembly/filtration, active self-cleaning solar panels, including high output sensors and devices in many engineering and biomedical frontiers.

There is a high demand for hydrogels with multifunctional performance (a combination of adhesive, mechanical, and electrical properties) in biological, tissue engineering, robotics, and smart device applications. However, a majority of existing hydrogels are relatively rigid and brittle, with limited stretchability; this hinders their application in the emerging field of flexible devices. In this study, cheap and abundant potato residues were used with polyacrylamide (PAM) to fabricate a multifunctional hydrogel, and chitosan was used for the design of a three-dimentional (3D) network-structured hydrogel. The as-prepared hydrogels exhibited excellent stretchability, with an extension exceeding 900% and a recovery degree of over 99%. Due to the combination of physical and chemical cross-linking properties and the introduction of dopamine, the designed hydrogel exhibits a remarkable self-healing ability (80% mechanical recovery in 2 h), high tensile strength (0.75 MPa), and ultra-stretchability (900%). The resultant products offer superior properties compared to those of previously reported tough and self-healing hydrogels for wound adhesion. Chitosan and potato residues were used as scaffold materials for the hydrogels with excellent mechanical properties. In addition, in vitro experiments show that these hydrogels feature excellent antibacterial properties, effectively hindering the reproduction of bacteria. Moreover, the ternary hydrogel can act as a strain sensor with high sensitivity and a gauge factor of 1.6. The proposed strategy is expected to serve as a reference for the development of green and recyclable conductive polymers to fabricate hydrogels. The proposed hydrogel can also act as a suitable strain sensor for bio-friendly devices such as smart wearable electronic devices and/or for health monitoring.

Geckos have the extraordinary ability to adhere and move across varied surfaces, while keeping their tiny high-aspect-ratio foot-hairs intact for thousands of attachment-detachment cycles. Inspired...

The high diffusion rate of sulfur with respect to metal oxide creates precursors that deviate from the stoichiometric ratio, leading to poor growth controllability and defects in the as-grown transition metal dichalcogenides (TMDCs). The introduction of a sulfur precursor with a high melting point is a hopeful strategy to solve these problems. Here, we first introduce sodium sulfate (Na2SO4) as a sulfur precursor, which plays roles in tuning diffusion of source precursors and balancing their mass flux based on the temperature-confined decomposition of Na2SO4. We deduced the specific growth process by characterizing the composition of intermediates; the results show that emissions of sulfur and metal sources were synchronously released and spanning the entire growth stage. This temperature-controlled source-feeding system reduced the diffusion gap between sulfur and metal, which promoted a faster kinetics for reactions. Moreover, this method has the wide applicability for producing other TMDCs.

Designing effective catalysts by controlling morphology and structure is key to improving the energy efficiency of fuel cells. A good understanding of the effects of specific structures on electrocatalytic activity, selectivity, and stability is needed. Here, we propose a facile method to synthesize PtCu bimetallic nanostructures with controllable compositions by using Cu nanowires as a template and ascorbic acid as a reductant. A further annealing process provided the alloy PtCu with tunable crystal structures. The combination of distinct structures with tunable compositions in the form of PtCu nanowires provides plenty of information for better understanding the reaction mechanism during catalysis. HClO4 cyclic voltammetry (CV) tests confirmed that various phase transformations occurred in bimetallic and alloy samples, affecting morphology and unit cell structures. Under a bifunctional synergistic effect and the influence of the insertion of a second metal, the two series of structures show superior performance toward methanol electrooxidation. Typically, the post-product alloy A-Pt14Cu86 with a cubic structure (a = 3.702 A) has better methanol oxidation reaction (MOR) catalysis performance. Density functional theory (DFT) calculations were performed to determine an optimal pathway using the Gibbs free energy and to verify the dependence of the electrocatalytic performance on the lattice structure via overpotential changes. Bimetallic PtCu has high CO tolerance, maintaining high stability. This work provides an approach for the systematic design of novel catalysts and the exploration of electrocatalytic mechanisms for fuel cells and other related applications.

Countless organisms in nature have adapted high-aspect-ratio micro-/nano-fibrillar arrays on their functional surfaces for achieving special and often optimized functionalities using earthly abundant materials. At the core of nanoscience and nanotechnology, rationally mimicking nature offers a promising route to create multifunctional superstructures that capture organisms and biological materials’ intriguing responsive and self-adjusting properties. Prior work has demonstrated that hierarchical vertically aligned multi-walled carbon nanotube (VA-MCNT) arrays can achieve ten folds of adhesive force comparing to the fibrillar structures of the gecko toe pads. However, little is known with regard to their wettability at the ultimate atomistic level, and how this may influence the adhesive performance and/or self-cleaning capabilities, despite water condensation and bridging are common phenomena at this length scale. In present study, molecular dynamics (MD) simulations were performed using Large-Scale Atomic / Molecular Massively Parallel Simulator (LAMMPS). Results indicate that commonly believed hydrophobic defect free CNTs (i.e., carbon sp2 hybridization without any dangling bonds) become super-hydrophilic at this length/temporal scale. The critical factors that influence the number of H-Bonds in water are: i) tube-tube spacing; and ii) shape/size and position of the water nanodroplet; and iii) how many droplets exists and how many nanotubes are bridged by the droplets. Chirality has little effect on the water interfacial behaviors. Future work will focus on the effect of water condensation and bridging on the adhesive and self-cleaning properties of carbon-based bio-inspired fibrillar dry adhesives considering defects and saline water.

Self-cleaning surfaces are desirable in many engineering applications where low energy consumption, reusability and sustainability are of the biggest concerns. Inspired by the gecko’s unique ‘dry self-cleaning’ hierarchical structures. Here we fabricated artificial Fe 3 O 4 /PDMS composites that show robust self-cleaning capabilities. The enhanced adhesion performance is attributable to the decrease of PDMS polymerization degree and the load transfer between PDMS matrix and Fe 3 O 4 magnetic particles. The self-cleaning surfaces showed up to 24.3% self-cleaning rate with as few as 4 steps. Simulation result indicated that the changing of cross linking between Fe 3 O 4 and PDMS is the main reason for the enhanced self-cleaning surfaces. This work reveals an alternative route of making high-performance self-cleaning smart surfaces that are applicable in the textile industry, robotic locomotion/gripping technology, outer-space explorations and tissue engineering.

Shape engineering plays a crucial role in the application of two-dimensional (2D) layered metal dichalcogenide (LMD) crystalline materials in terms of physical and chemical property modulation. How...

Present study reports a controllable phase transformation of nickel (Ni) from amorphous to cubic crystal structures on tungsten (W) substrate by electrodeposition. X-ray powder diffraction, scanning electron microscopy, transmission electron microscopy and energy dispersive spectroscopy were used to characterize the microstructure, micro-constituents and surface morphology of as-prepared Ni. The microstructure of Ni was strongly affected by the applied overpotential and deposition time. It is demonstrated that by controlling these two parameters either amorphous or cubic crystal structure of Ni on the W substrate could be obtained. The crystallization mechanism is discussed based on Gibbs crystal growth theory and Ostwald’s rule. It is concluded that W substrate, acting as a heat sink, can effectively promote the thermal stability of amorphous Ni, based on the data from differential scanning calorimetry and Kissinger’s model. This work contributes to the elucidation of the crystallization mechanism of Ni on W powder substrates, and proves that, better than alloying with other elements, incorporating powder substrates will significantly improve the crystallization temperature, hence the thermostability of amorphous Ni.

Substitutional doping has been proven to be an effective route to engineer band gap, transport characteristics, and magnetism in transition metal dichalcogenides. Herein, we demonstrate substitutio...

Two-dimensional layered molybdenum disulfide (MoS2) is a promising catalyst for hydrogen evolution reaction (HER), and a good replacement for platinum (Pt) in elelctrochemical water splitting. Most transition metal dichalcogenides (TMDs) show excellent catalytic activity, which stems from their active sites located along the edges. However, small density of the active sites in the basal plane, largely limits TMDs performance. To enhance the HER catalysis activity of MoS2, we developed an efficient and scalable approach to significantly increase the overall electrochemically active sites using mild sodium hypochlorite (NaClO) solution anisotropic etching. The effect is further enhanced by oxygen-plasma pretreatment of the material, which - upon chemical etching - leads to highly porous and highly reactive structure. The resulting chemically activated MoS2 (ca-MoS2) was systematically characterized and optimized. The optimized ca-MoS2 powder exhibits enhanced HER performance with an overpotential of 0.34 V at a current density of 0.5 mA cm−2 in this experiment due to the increasing active sites, and the Tafel slope also smaller than other samples. This chemical etching method provides new ways to design atomic structure modification, including controlling layered TMD electrochemical property and new type of transistor fabrication.

Growth of large-area, uniform, and high-quality monolayer transition-metal dichalcogenides (TMDs) for practical and industrial applications remains a long-standing challenge. The present study demonstrates a modified predeposited chemical vapor deposition (CVD) process by employing an annealing procedure before sulfurization, which helps in achieving large-area, highly uniform, and high-quality TMDs on various substrates. The annealing procedure resulted in a molten liquid state of the precursors in the CVD process, which not only facilitated a uniform redistribution of the precursor on the substrate (avoid the aggregation) because of the uniform redistribution of the liquid precursor on the substrate but more importantly avoided the undesired multilayer growth via the self-limited lateral supply precursors mechanism. A 2 in. uniform and continuous monolayer WS2 film has been synthesized on the SiO2/Si substrate. Moreover, uniform monolayer WS2 single crystals can be prepared on more general and various substrates including sapphire, mica, quartz, and Si3N4 using the same growth procedure. Besides, this growth mechanism can be generalized to synthesize other monolayer TMDs such as MoS2 and MoS2/WS2 heterostructures. Hence, the present method provides a generalized attractive strategy to grow large-area, uniform, single-layer two-dimensional (2D) materials. This study has significant implications in the advancement of batch production of various 2D-material-based devices for industrial and commercial applications.

Gecko lizards have a remarkable climbing capability that enables them to adapt to a variety of environments. Although the hierarchical structures and adhesion mechanism of gecko feet have been studied extensively, there lacks a fundamental understanding of adhesion at relatively low temperature, in particular below icing point. Here, we study the adhesion forces of nanoscale gecko spatulae and setae on multiple surfaces in a broad range of temperature from 40 to -10°C. Results demonstrate that the adhesion force of a single gecko spatula on a mica substrate at -10 °C increased by ∼100% compared with that at room temperature. The adhesion and friction forces of a single seta also display similar trends. It is found that hydrogen bonds play a key role in the temperature-induced tunable adhesion. Emulating gecko feet, we have fabricated fibrillary adhesive surfaces and tested them under different environments. Like their biological counterparts, regulating temperature can tune their adhesion and self-cleaning capacity. This study shed lights on the adhesion mechanism of gecko at low temperature, and provides a base for the design of new generations of smart tires, climbing robots and/or biomedical devices that would perform robustly under extreme environments.

Shape engineering plays a crucial role in the application of two-dimensional (2D) layered metal dichalcogenide (LMD) crystalline materials in terms of physical and chemical property modulation. However, controllable growth of 1T phase tin disulfide (SnS

Geckos have adapted to the complicated natural environment with its excellent climbing ability. Current artificial gecko-inspired synthetic adhesives (GSAs) mimic gecko's attach-detach mechanism by creating anisotropic and hierarchical structures. Easy detachment and high self-cleaning capability are still the unsolved problems in GSAs. This study presents an unprecedented photodetachable mechanism of making bioinspired smart surfaces utilizing carbon dot (CD)-doped polydimethylsiloxane (PDMS) composites. Under ultraviolet (UV) irradiation, it could be triggered up to 80.46% reduction of adhesion force between PDMS-CDs bioinspired surfaces and contaminating particles. A load-drag-pull (i.e., LDP) test mimicking gecko's locomotion was adopted to test the dry self-cleaning capabilities of these bioinspired surfaces, where the falling rate of the model contaminates (PS micropellets; average size in diameter ∼8 μm) can reach up to 54.83% after seven repeated steps under UV irradiation. The significantly improved dry self-cleaning capability is attributed to the photothermal effect of CDs inside the PDMS matrix. The mechanism proposed in this work will find its applications in the realms of climbing robots, space adhesive devices, and self-cleaning, advanced gripping technologies for pick and place or assembly.

Self-healing triboelectric nanogenerators (SH-TENGs) with fast self-healing, high output performance, and wearing comfort have wide and promising applications in wearable electronic devices. This work presents a high-performance hydrogel-based SH-TENG, which consists of a high dielectric triboelectric layer (HDTL), a self-healing hydrogel electrode layer (SHEL), and a physical cross-linking layer (PCLL). Carbon nanotubes (CNTs), obtained by a chemical vapor deposition (CVD) method, were added into polydimethylsiloxane (PDMS) to produce the HDTL. Compared with pure PDMS, the short-circuit transferred charge (44 nC) and the open circuit voltage (132 V) are doubled for PDMS with 0.01 wt% CNTs. Glycerin, polydopamine particles (PDAP) and graphene were added to poly (vinyl alcohol) (PVA) to prepare the self-healing hydrogel electrode layer. SHEL can physically self-heal in ~1 min when exposed to air. The self-healing efficiency reaches up to 98%. The PCLL is made of poly(methylhydrosiloxane) (PMHS) and PDMS. It forms a good physical bond between the hydrophilic hydrogel and hydrophobic PDMS layers. The electric output performance of the SH-TENG can reach 94% of the undamaged one in 1 min. The SH-TENG (6 × 6 cm2) exhibits good stability and superior electrical performance, enabling it to power 37 LEDs simultaneously.

Poly(aryloxy)phosphazenes emerge as an important class of hybrid polymers for a whole range of potential applications. To date, however, little is known about the detailed reaction mechanisms during preparation. This draws a great deal of attention for developing well-defined and well-controllable synthesis methods. In this paper, poly(dichlorophosphazene) (PDCP) has been successfully synthesized, and subsequent reaction with sodium phenoxide or phenol in the presence of K2CO3 can produce poly(bis(phenoxy)phosphazene) (PBPP). To elucidate the issues of branching and cross-linking, focuses have been placed on the change of various reaction conditions, in terms of concentration, temperature, time, solvent, catalysis, etc. The product polymers were examined using the techniques of 31P and 13C NMR, GPC, XPS, and FT-IR, in order to characterize the structural defects, in particular, branching and unwanted substitutions, such as addition of water molecules or oxidation of the phosphorus atoms on the backbone of...

Uniform and stable core-shell microspheres composed of a polyimide (PI) core and thin metal/oxide/sulphide shells were prepared by an interfacial reaction of metal-ion-doped polymeric cores in reduction or in the air or sodium sulphide solutions, respectively. The silver shells on polyimide microspheres were prepared by the introduction of silver ions into ion-exchangeable surface-modified polyimide, and subsequently an in situ reduction of the silver ions in solution. Oxides shells such as SnO 2 , Co 3 O 4 , NiO, CuO or ZnO were prepared by thermally treating the ion-doped microspheres in air, while amorphous sulphides shells such as CuS, ZnS, CoS or Ag 2 S were prepared by an interfacial reaction of metal-ion-doped microspheres in its corresponding sodium sulphide solutions. The adhesion properties between the copper sulphide and PI substrates are demonstrated superior. This simple strategy is promising in the fabrication of a whole range of inorganic shells on polyimide microspheres, which may offer tailor-designed multi-functionalities based on the distinctive species of these inorganic shells.

Poly(aryloxy)phosphazenes emerge as an important class of hybrid polymers for a whole range of potential applications. To date, however, little is known about the detailed reaction mechanisms during preparation. This draws a great deal of attention for developing well-defined and well-controllable synthesis methods. In this paper, poly(dichlorophosphazene) (PDCP) has been successfully synthesized, and subsequent reaction with sodium phenoxide or phenol in the presence of K

Geckos have the extraordinary ability to prevent their sticky feet from fouling while running on dusty walls and ceilings. Understanding gecko adhesion and self-cleaning mechanisms is essential for elucidating animal behaviours and rationally designing gecko-inspired devices. Here we report a unique self-cleaning mechanism possessed by the nano-pads of gecko spatulae. The difference between the velocity-dependent particle-wall adhesion and the velocity-independent spatula-particle dynamic response leads to a robust self-cleaning capability, allowing geckos to efficiently dislodge dirt during their locomotion. Emulating this natural design, we fabricate artificial spatulae and micromanipulators that show similar effects, and that provide a new way to manipulate micro-objects. By simply tuning the pull-off velocity, our gecko-inspired micromanipulators, made of synthetic microfibers with graphene-decorated micro-pads, can easily pick up, transport, and drop-off microparticles for precise assembling. This work should open the door to the development of novel self-cleaning adhesives, smart surfaces, microelectromechanical systems, biomedical devices, and more., A running gecko can adhere to any surfaces at wet or dry conditions, whilst it keeps its toe pads clean. Here, Xu et al. attribute this self-cleaning mechanism to the rate-independent adhesion response between dirt particles and the gecko's foot and use synthetic microfibers to reproduce the effect.