Search

High-performance and low-cost photocatalysts play the key role in achieving the large-scale solar hydrogen production. In this work, we report a liquid-exfoliation approach to prepare NiPS3 ultrathin nanosheets as a versatile platform to greatly improve the light-induced hydrogen production on various photocatalysts, including TiO2, CdS, In2ZnS4 and C3N4. The superb visible-light-induced hydrogen production rate (13,600 μmol h−1 g−1) is achieved on NiPS3/CdS hetero-junction with the highest improvement factor (~1,667%) compared with that of pure CdS. This significantly better performance is attributed to the strongly correlated NiPS3/CdS interface assuring efficient electron-hole dissociation/transport, as well as abundant atomic-level edge P/S sites and activated basal S sites on NiPS3 ultrathin nanosheets advancing hydrogen evolution. These findings are revealed by the state-of-art characterizations and theoretical computations. Our work for the first time demonstrates the great potential of metal phosphorous chalcogenide as a general platform to tremendously raise the performance of different photocatalysts. While light-driven water splitting offers a renewable means to produce fuel, the limited availability of high-performance materials inspires the search for new photocatalysts. Here, authors demonstrate two-dimensional NiPS3 to enhance semiconductor photocatalytic H2 evolution activities. [ABSTRACT FROM AUTHOR]

Electroreduction of carbon dioxide (CO2) into multicarbon products provides possibility of large-scale chemicals production and is therefore of significant research and commercial interest. However, the production efficiency for ethanol (EtOH), a significant chemical feedstock, is impractically low because of limited selectivity, especially under high current operation. Here we report a new silver–modified copper–oxide catalyst (dCu2O/Ag2.3%) that exhibits a significant Faradaic efficiency of 40.8% and energy efficiency of 22.3% for boosted EtOH production. Importantly, it achieves CO2–to–ethanol conversion under high current operation with partial current density of 326.4 mA cm−2 at −0.87 V vs reversible hydrogen electrode to rank highly significantly amongst reported Cu–based catalysts. Based on in situ spectra studies we show that significantly boosted production results from tailored introduction of Ag to optimize the coordinated number and oxide state of surface Cu sites, in which the *CO adsorption is steered as both atop and bridge configuration to trigger asymmetric C–C coupling for stablization of EtOH intermediates. It is of high interest to convert CO2 into valuable ethanol product. Here the authors demonstrate the asymmetric C-C coupling triggered on Ag-modified oxide-derived Cu sites can accelerate and steer the reaction pathway for ethanol production with high faradaic efficiency and current density. [ABSTRACT FROM AUTHOR]

Owing to their scientific and technological importance, inorganic single crystals with highly reactive surfaces have long been studied [1-13]. Unfortunately, surfaces with high reactivity usually diminish rapidly during the crystal [...]

Converting CO2 into high‐value fuels and chemicals by renewable‐electricity‐powered electrochemical CO2 reduction reaction (CRR) is a viable approach toward carbon‐emissions‐neutral processes. Unlike the thermocatalytic hydrogenation of CO2 at the solid‐gas interface, the CRR takes place at the three‐phase gas/solid/liquid interface near the electrode surface in aqueous solution, which leads to major challenges including the limited mass diffusion of CO2 reactant, competitive hydrogen evolution reaction, and poor product selectivity. Here we critically examine the various methods of surface and interface engineering of the electrocatalysts to optimize the microenvironment for CRR, which can address the above issues. The effective modification strategies for the gas transport, electrolyte composition, controlling intermediate states, and catalyst engineering are discussed. The key emphasis is made on the diverse atomic‐precision modifications to increase the local CO2 concentration, lower the energy barriers for CO2 activation, decrease the H2O coverage, and stabilize intermediates to effectively control the catalytic activity and selectivity. The perspectives on the challenges and outlook for the future applications of three‐phase interface engineering for CRR and other gas‐involving electrocatalytic reactions conclude the article. [ABSTRACT FROM AUTHOR]

We demonstrate a widely applicable method to alter the adsorption configuration of multi‐carbon containing reactants by no catalyst engineering but simply adjusting the local reaction environment of the catalyst surface. Using electrocatalytic acetone to propane hydrogenation (APH) as a model reaction and common commercial Pt/Pt‐based materials as catalysts, we found local H+ concentration can significantly influence the adsorption mode of acetone reactant, for example, in vertical or flat mode, and target product selectivity. Electrocatalytic measurement combined with in situ spectroscopic characterizations reveals that the vertically adsorbed acetone is favorable for propane production while the flatly adsorbed mode suppresses the reaction. DFT calculations indicate that the H coverage on catalyst surface plays a decisive role in the adsorption configuration of acetone. The increased local acidity can facilitate the adsorption configuration of acetone from flat to vertical mode and suppress the competing hydrogen evaluation reaction, which consequently enhances the APH selectivity. [ABSTRACT FROM AUTHOR]

Powered by inexhaustible solar energy, photoelectrochemical (PEC) hydrogen/ammonia production and reduction of carbon dioxide to high added‐value chemicals in eco‐friendly and mild conditions provide a highly attractive solution to carbon neutrality. Recently, substantial advances have been achieved in PEC systems by improving light absorption and charge separation/transfer in PEC devices. However, less attention is given to the atomic design of photoelectrocatalysts to facilitate the final catalytic reactions occurring at photoelectrode surface, which largely limits the overall photo‐to‐energy conversion of PEC system. Fundamental catalytic mechanisms and recent progress in atomic design of PEC materials are comprehensively reviewed by engineering of defect, dopant, facet, strain, and single atom to enhance the activity and selectivity. Finally, the emerging challenges and research directions in design of PEC systems for future photo‐to‐energy conversions are proposed. [ABSTRACT FROM AUTHOR]