Changda Wang

Unsaturated-sulfur-rich MoS2 nanosheets decorated on free-standing SWNT film: Synthesis, characterization and electrocatalytic application

Herein, we report a bottom-up solvothermal route to synthesize a flexible, highly efficient MoS2@SWNT electrocatalyst for hydrogen evolution reactions (HER). Characterization revealed that branch-like MoS2 nanosheets containing sulfurrich sites were in situ uniformly dispersed on free-standing single-walled carbon nanotube (SWNT) film, which could expose more unsaturated sulfur atoms, allowing excellent electrical contact with active sites. The flexible catalyst exhibited excellent HER performance with a low overpotential (~150 mV at 10 mA/cm2) and small Tafel slope (41 mV/dec). To further explain the improved performance, the local electronic structure was investigated by X-ray absorption near-edge structure (XANES) analysis, proving the presence of unsaturated sulfur atoms and strong electronic coupling between MoS2 and SWNT. This study provides an in-situ synthetic route to create new multifunctional flexible hybridized catalysts and useful insights into the relationships among the catalyst microstructure, electronic structure, and properties.

All-Carbon Ultrafast Supercapacitor by Integrating Multidimensional Nanocarbons.

Ultrafast and high capacity all-carbon supercapacitors with 3D porous aerogel electrode are realized by combining carbon nanostructures of various dimensionalities, including 0D carbon onions, 1D carbon nanotubes, and 2D graphene oxide. The synergistic effects from the different forms of nanocarbons render this hybrid outstanding capacitance with excellent stability, even at ultrafast charge-discharge rates.

Metallic 1T-WS2 nanoribbons as highly conductive electrodes for supercapacitors

Layered tungsten disulfide (WS2) has attracted great attention because of its high potential for electrochemical energy applications. However, the semiconducting nature of WS2 with a 2H phase largely hinders its electrochemical performance due to poor electronic conductivity. In this study, we have successfully synthesized a metallic 1T-WS2 nanoribbon with stable ammonia-ion intercalation as a highly conductive electrode for high-performance supercapacitors. The specific capacitance using the metallic 1T-WS2 electrode exhibits significant enhancement upto the value of 2813 μF cm−2. This value is 12 times higher compared to semiconducting 2H-WS2. Moreover, the 1T-WS2 electrode has good stability even under high current scans, which is ascribed to the stable ammonia-ion interaction. The correlation between the 1T-WS2 structure and its electrochemical performance has also been discussed.

Hierarchical 1T-MoS2 nanotubular structures for enhanced supercapacitive performance

Layered transition metal disulfides are currently being widely studied for advanced energy generation and storage applications. Here we report a facile template-assisted solvothermal strategy to obtain a hierarchical nanotubular structure consisting of ultrathin MoS2 nanosheets with a metallic 1T phase. Synchrotron radiation based X-ray absorption fine structure (XAFS) and X-ray photoelectron spectroscopy (XPS) are used to investigate the structure and electronic properties of the 1T-MoS2, which are largely different from annealed samples. Its hierarchical structure makes the obtained nanotubular 1T-MoS2 an excellent electrode material for supercapacitors, with a high specific capacitance of 328.547 F g−1 at a current density of 1 A g−1 and 243.66 F g−1 at a current density of 15 A g−1. Moreover, the material displays excellent capacitance retention, retaining 98.4% capacity after 5000 cycles at a current density of 3 A g−1. Notably, a high specific capacitance of 250 F g−1 at 1 A g−1 is also achieved in a two-electrode symmetrical cell, suggesting its great potential for new-generation supercapacitors.

Engineering interfacial charge-transfer by phase transition realizing enhanced photocatalytic hydrogen evolution activity

Thin, planar nanojunctions between layered 2H/1T-MoS2 and graphitic C3N4 (g-C3N4) were fabricated and 1T phase nanojunctions allowed faster photogenerated electrons across the junction interfaces to facilitate hydrogen evolution. This research represents a proof of concept for the rational fabrication of thin 1T phase interfacial junctions and the importance of the 1T phase for further improving the HER perfomance.

In situ growth of metallic 1T-WS2 nanoislands on single-walled carbon nanotube films for improved electrochemical performance

Layered tungsten disulfide (WS2) is a potential electrode material for electric double layer capacitance (EDLC) and hydrogen evolution reaction (HER). However, the electrochemical performance of WS2 has been hindered by the semiconducting nature and poor active sites. Herein, we have demonstrated a bottom-up hydrothermal approach to fabricate metallic 1T-WS2 nanoislands in situ grown on flexible single-walled carbon nanotube nonwovens (1T-WS2@SWCNT). The robust hybrids with a tight interface possess nanoscopic few-layered WS2 pieces with an abundance of exposed sites, along with a unique woven-architecture originating from the high conductive carbon nanotube network. The in situ-growing enhanced interface between metallic WS2 nanoislands and SWCNTs provides a relatively strong electrical coupling integrity, which facilitates charge transfer during electrochemical reactions. The merits of rich active sites, excellent conductivity and well bonding-interactions are significantly beneficial to improve the electrochemical performance. Particularly, in contrast to the pure material, the as-obtained hybrids are found to exhibit higher EDLC capacity (226 mF cm−2), almost 646-fold higher than pure 1T-WS2, smaller Tafel slope (57 mV per decade) and lower HER overpotential (∼25 mV) than any WS2-based materials reported so far.

In situ trapped high-density single metal atoms within graphene: Iron-containing hybrids as representatives for efficient oxygen reduction

Atomically dispersed catalysts have attracted attention in energy conversion applications because their efficiency and chemoselectivity for special catalysis are superior to those of traditional catalysts. However, they have limitations owing to the extremely low metal-loading content on supports, difficulty in the precise control of the metal location and amount as well as low stability at high temperatures. We prepared a highly doped single metal atom hybrid via a single-step thermal pyrolysis of glucose, dicyandiamide, and inorganic metal salts. High-angle annular dark field-scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption fine structure spectroscopy (XAFS) revealed that nitrogen atoms doped into the graphene matrix were pivotal for metal atom stabilization by generating a metal-Nx coordination structure. Due to the strong anchoring effect of the graphene matrix, the metal loading content was over 4 wt.% in the isolated atomic hybrid (the Pt content was as high as 9.26 wt.% in the Pt-doped hybrid). Furthermore, the single iron-doped hybrid (Fe@N-doped graphene) showed a remarkable electrocatalytic performance for the oxygen reduction reaction. The peak power density was ∼199 mW·cm−2 at a current density of 310 mA·cm−2 and superior to that of a commercial Pt/C catalyst when it was used as a cathode catalyst in assembled zinc-air batteries. This work offered a feasible approach to design and fabricate highly doped single metal atoms (SMAs) catalysts for potential energy applications.

The Effect of High Concentration and Small Size of Nanodiamonds on the Strength of Interface and Fracture Properties in Epoxy Nanocomposite

The concentration and small size of nanodiamonds (NDs) plays a crucial role in the mechanical performance of epoxy-based nanocomposites by modifying the interface strength. Herein, we systemically analyzed the relation between the high concentration and small size of ND and the fracture properties of its epoxy-based nanocomposites. It was observed that there is a two-fold increase in fracture toughness and a three-fold increase in fracture energy. Rationally, functionalized-NDs (F-NDs) showed a much better performance for the nanocomposite than pristine NDs (P-NDs) because of additional functional groups on its surface. The F-ND/epoxy nanocomposites exhibited rougher surface in contrast with the P-ND/epoxy, indicating the presence of a strong interface. We found that the interfaces in F-ND/epoxy nanocomposites at high concentrations of NDs overlap by making a web, which can efficiently hinder further crack propagation. In addition, the de-bonding in P-ND/epoxy nanocomposites occurred at the interface with the appearance of plastic voids or semi-naked particles, whereas the de-bonding for F-ND/epoxy nanocomposites happened within the epoxy molecular network instead of the interface. Because of the strong interface in F-ND/epoxy nanocomposites, at high concentrations the de-bonding within the epoxy molecular network may lead to subsequent cracks, parallel to the parent crack, via crack splitting which results in a fiber-like structure on the fracture surface. The plastic void growth, crack deflection and subsequent crack growth were correlated to higher values of fracture toughness and fracture energy in F-ND/epoxy nanocomposites.

Facile synthesis of mesoporous detonation nanodiamond-modified layers of graphitic carbon nitride as photocatalysts for the hydrogen evolution reaction

The hydrogen evolution reaction (HER) may contribute substantially to energy resources in the future through solar energy conversion. In this study, mesoporous graphitic carbon nitride (g-C3N4) layers modified by detonation nanodiamond (DND) were synthesized by condensation from urea to obtain a robust and efficient hybrid (g-C3N4–DND) photocatalyst for the HER. Our characterizations revealed that no significant structural changes occurred in g-C3N4 during the synthesis of the g-C3N4–DND hybrid. Compared with pure g-C3N4, hydrogen production increased by almost 50% when using the hybrid photocatalyst due to the synergetic effect of the enhanced charge transfer, high surface area and low recombination rate of the photogenerated charge carriers.

Well‐Defined Cobalt Catalyst with N‐Doped Carbon Layers Enwrapping: The Correlation between Surface Atomic Structure and Electrocatalytic Property

Admittedly, the surface atomic structure of heterogenous catalysts toward the electrochemical oxygen reduction reaction (ORR) are accepted as the important features that can tune catalytic activity and even catalytic pathway. Herein, a surface engineering strategy to controllably synthesize a carbon-layer-wrapped cobalt-catalyst from 2D cobalt-based metal-organic frameworks is elaborately demonstrated. Combined with synchrotron radiation X-ray photoelectron spectroscopy, the soft X-ray absorption near-edge structure results confirmed that rich covalent interfacial CoNC bonds are efficiently formed between cobalt nanoparticles and wrapped carbon-layers during the polydopamine-assisted pyrolysis process. The X-ray absorption fine structure and corresponding extended X-ray absorption fine structure spectra further reveal that the wrapped cobalt with Co-N coordinations shows distinct surface distortion and atomic environmental change of Co-based active sites. In contrast to the control sample without coating layers, the 800 °C-annealed cobalt catalyst with N-doped carbon layers enwrapping achieves significantly enhanced ORR activity with onset and half-wave potentials of 0.923 and 0.816 V (vs reversible hydrogen electrode), highlighting the important correlation between surface atomic structure and catalytic property.