Plasma-assisted synthesis of porous bismuth nanosheets for electrocatalytic CO_(2)-to-formate reduction

The electrochemical carbon dioxide reduction(eCO_(2)RR)to formate,driven by clean energy,is a promising approach for producing renewable chemicals and high-value fuels.Despite its potential,further development faces challenges due to limitations in electrocatalytic activity and durability,especially for nonnoble metal-based catalysts.Here,naturally abundant bismuth-based nanosheets that can effectively drive CO_(2)-to-formate electrocatalytic reduction are prepared using the plasma-activated Bi_(2)Se_(3) followed by a reduction process.Thus-obtained plasma-activated Bi nanosheets(P-BiNS)feature ultrathin structures and high surface areas.Such nanostructures ensure the P-BiNS with outstanding eCO_(2)RR catalytic performance,highlighted by the current density of over 80 mA cm^(-2) and a formate Faradic efficiency of>90%.Furthermore,P-BiNS catalysts demonstrate excellent durability and stability without deactivation following over 50h of operation.The selectivity for formate production is also studied by density functional theory(DFT)calculations,validating the importance and efficacy of the stabilization of intermediates(^(*)OCHO)on the P-BiNS surfaces.This study provides a facile plasma-assisted approach for developing high-performance and low-cost electrocatalysts.

Porous Indium Nanocrystals on Conductive Carbon Nanotube Networks for High-Performance CO_(2)-to-Formate Electrocatalytic Conversion

Ever-increasing emissions of anthropogenic carbon dioxide(CO_(2))cause global environmental and climate challenges.Inspired by biological photosynthesis,developing effective strategies NeuNlto up-cycle CO_(2)into high-value organics is crucial.Electrochemical CO_(2)reduction reaction(CO_(2)RR)is highly promising to convert CO_(2)into economically viable carbon-based chemicals or fuels under mild process conditions.Herein,mesoporous indium supported on multi-walled carbon nanotubes(mp-In@MWCNTs)is synthesized via a facile wet chemical method.The mp-In@MWCNTs electrocatalysts exhibit high CO_(2)RR performance in reducing CO_(2)into formate.An outstanding activity(current density-78.5 mA cm^(-2)),high conversion efficiency(Faradaic efficiency of formate over 90%),and persistent stability(∼30 h)for selective CO_(2)-to-formate conversion are observed.The outstanding CO_(2)RR process performance is attributed to the unique structures with mesoporous surfaces and a conductive network,which promote the adsorption and desorption of reactants and intermediates while improving electron transfer.These findings provide guiding principles for synthesizing conductive metal-based electrocatalysts for high-performance CO_(2)conversion.

Reduced Ti-MOFs encapsulated black phosphorus with high stability and enhanced photocatalytic activity

The generation of green hydrogen(H_2) energy is of great significance to solve worldwide energy and environmental issues. Reduced Ti based photocatalyst has recently attracted intensive attention due to its excellent photocatalytic activity, while the synthesis of reduced Ti based photocatalysts with high stability is still a great challenge. Here, we report a facile method for synthesis of reduced Ti metal organic frameworks(small amounts of Pt incorporated) encapsulated BP(BP/R-Ti-MOFs/Pt) hybrid nanomaterial with enhanced photocatalytic activity. The strong interaction between Ti and P reduces the valence state of the binding Ti^(4+)on the BP surface, forming abundant reduced Ti^(4+)within R-Ti-MOFs/BP. Such reduced Ti^(4+)render R-Ti-MOFs/BP efficient charge transfer and excellent light absorption capability, thus promote the photocatalytic H_2 production efficiency. Furthermore, the Ti-P interaction stabilizes both reduced Ti^(4+)and BP during the photocatalytic reaction, which greatly enhanced the stability of the obtained BP/R-TiMOFs/Pt photocatalyst.

A robust Janus bilayer with tailored ionic conductivity and interface stability for stable Li metal anodes

The formation and growth of Li-dendrites caused by inhomogeneous Li deposition severely hinder the commercial applications of Li metal batteries due to the consequence of short-circuiting.Herein,we propose a Janus bilayer composed of black phosphorus(BP)and graphene oxide(GO)as an artificial interface with chemical/mechanical stability and well-regulated Li-ion flux distribution for Li metal anode protection.Owing to the synergy between the fast Li-ion transport of BP in the inner layer and the high mechanical and chemical stability of GO in the outer layer,the GO/BP with good electrolyte wettability acts as a Li-ion regulator that can induce homogeneous growth of Li to suppress the Li dendrites growth.Accordingly,long-term stability(500 h at 1 mA cm^(-2))with a low overpotential of 30 mV is achieved in the symmetric cell with GO/BP-Li anode.Furthermore,the Li–S cell with GO/BP-Li exhibits enhanced cycling performance with a high capacity retention rate of 76.2%over 500 cycles at 1 C.

In-situ liquid-phase transmission electron microscopy for two-dimensional energy materials

Two-dimensional(2D)materials are vital for the development of advanced materials in the next-generation energy conversion and storage devices.In-situ liquid-phase transmission electron microscopy(LP-TEM)acts as a powerful tool for characterizing the dynamic evolution of materials under work condition in real time and in operando.Herein,this mini-review highlights the considerable advances in the utilization of in-situ LP-TEM for studying the physical and chemical process dynamics of 2D materials,such as their nucleation growth and phase transformation.The electrocatalytic water splitting reactions and CO_(2) electroreduction of 2D energy materials are highlighted.The underlying electrochemical reaction mechanisms of the 2D electrode materials in rechargeable batteries are discussed and summarized.Finally,the current challenges and perspectives for future research are proposed.This min-review aims to inspire and stimulate further innovation and encourage the broader adoption of LP-TEM in exploring the fascinating dynamics of 2D energy materials.

An invisible hand:Hydrogen bonding guided synthesis of ultrathin two-dimensional amorphous TiO_(2)nanosheets

Ultrathin two-dimensional(2 D)porous nanosheets are one of the most promising nanomaterials in various applications,whereas their synthesis is still challenging.Herein,ultrathin 2 D amorphous TiO_(2)(a-TiO_(2))porous nanosheet aerogel is synthesized via a surfactant-free assembly process followed by low-temperature calcination.The co-existing O-O and-OH groups on the surface of TiO_(2)precursor break the 3 D spherical symmetry,and the hydrogen bonding among the TiO_(2)precursors is proposed as the main driving force guiding the 2 D assembly.The surfactant-free assembly endows the ultrathin a-TiO_(2)porous nanosheet with improved ionic and electronic conductivity.The porous structure provides high surface area and easy electrolyte penetration,accelerating the Li ion diffusion rate of the a-TiO_(2)porous nanosheet.Attributing to the above advantages,the obtained a-TiO_(2)porous nanosheets are one of the best anode materials for lithium-ion batteries,which is proved by the enhanced electrochemical performance.

Probing surface structure on two-dimensional metal-organic layers to understand suppressed interlayer packing

Two-dimensional metal-organic layers(MOLs)from alternatively connected benzene-tribenzoate ligands and Zr6(μ3-O)_(4)(μ3-OH)_(4) or Hf6(μ3-O)_(4)(μ3-OH)_(4) secondary building units can be prepared in gram scale via solvothermal synthesis.However,the reason why the monolayers did not pack to form thick crystals is unknown.Here we investigated the surface structure of the MOLs by a combination of sum-frequency generation spectroscopy,nanoscale infrared microscopy,atomic force microscopy,aberration-corrected transmission electron microscopy,and compositional analysis.We found a partial coverage of the monolayer surface by dangling tricarboxylate ligands,which prevent packing of the monolayers.This finding illustrates low-density surface modification as a strategy to prepare new two-dimensional materials with a high percentage of exposed surface.