Angew Chem Int Ed Engl
January 2025
The multi-carbon (C) alcohols produced by electrochemical CO reduction, such as ethanol and n-propanol, are considered as indispensable liquid energy carriers. In most C-C coupling cases, however, the concomitant gaseous CH product results in the low selectivity of C alcohols. Here, we report rational construction of mesostructured CuO electrocatalysts, specifically mesoporous CuO (m-CuO) and cylindrical CuO (c-CuO), enables selective distribution of C products.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2024
Selective CO photoreduction to value-added multi-carbon (C) feedstocks, such as CH, holds great promise in direct solar-to-chemical conversion for a carbon-neutral future. Nevertheless, the performance is largely inhibited by the high energy barrier of C-C coupling process, thereby leading to C products with low selectivity. Here we report that through facile surface immobilization of a 1-ethyl-3-methylimidazolium tetrafluoroborate (EMIM-BF) ionic liquid, plasmonic Cu nanowires could enable highly selective CO photoreduction to CH product.
View Article and Find Full Text PDFElectrocatalytic CO reduction reaction (CORR) to high value-added products, such as ethylene (CH), offers a promising approach to achieve carbon neutrality. Although recent studies have reported that a tandem catalyst (for example, Cu-Ag systems) exhibits advantage in CH production, its practical application is largely inhibited by the following: (1) a traditional tandem catalyst cannot effectively stabilize the *CO intermediate, resulting in sluggish C-C coupling, and (2) inadequate HO activation ability hinders the hydrogenation of intermediates. To break through the above bottleneck, herein, palladium (Pd) was introduced into CuO-Ag, a typical conventional tandem catalyst, to construct a CuO-Pd-Ag ternary catalyst.
View Article and Find Full Text PDFThe acidic electrochemical CO reduction reaction (CORR) for direct formic acid (HCOOH) production holds promise in meeting the carbon-neutral target, yet its performance is hindered by the competing hydrogen evolution reaction (HER). Understanding the adsorption strength of the key intermediates in acidic electrolyte is indispensable to favor CORR over HER. In this work, high-density Sn single atom catalysts (SACs) were prepared and used as catalyst, to reveal the pH-dependent adsorption strength and coverage of *CO intermediatethat enables enhanced acidic CORR towards direct HCOOH production.
View Article and Find Full Text PDFThe electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) is a promising method for the efficient production of biomass-derived high-value-added chemicals. However, its practical application is limited by: 1) the low activity and selectivity caused by the competitive adsorption of HMF and OH and 2) the low operational stability caused by the uncontrollable reconstruction of the catalyst. To overcome these limitations, a series of Ni S /NiO -n catalysts with controllable compositions and well-defined structures are synthesized using a novel in situ controlled surface reconstruction strategy.
View Article and Find Full Text PDFPhotoconversion of CO and H O into ethanol is an ideal strategy to achieve carbon neutrality. However, the production of ethanol with high activity and selectivity is challenging owing to the less efficient reduction half-reaction involving multi-step proton-coupled electron transfer (PCET), a slow C-C coupling process, and sluggish water oxidation half-reaction. Herein, a two-dimensional/two-dimensional (2D/2D) S-scheme heterojunction consisting of black phosphorus and Bi WO (BP/BWO) was constructed for photocatalytic CO reduction coupling with benzylamine (BA) oxidation.
View Article and Find Full Text PDFElectrochemical CO reduction reaction (CO RR) to chemical fuels such as formate offers a promising pathway to carbon-neutral future, but its practical application is largely inhibited by the lack of effective activation of CO molecules and pH-universal feasibility. Here, we report an electronic structure manipulation strategy to electron-rich Bi nanosheets, where electrons transfer from Cu donor to Bi acceptor in bimetallic Cu-Bi, enabling CO RR towards formate with concurrent high activity, selectivity and stability in pH-universal (acidic, neutral and alkaline) electrolytes. Combined in situ Raman spectra and computational calculations unravel that electron-rich Bi promotes CO ⋅ formation to activate CO molecules, and enhance the adsorption strength of *OCHO intermediate with an up-shifted p-band center, thus leading to its superior activity and selectivity of formate.
View Article and Find Full Text PDFIn this study, the ultra-thin iron phosphate Fe(PO) nanosheets (FP1) with fine-controlled morphology, has been designed as a new two-dimensional (2D) material for uranium adsorption. Due to its unique high accessible 2D structure, atom-dispersed phosphate/iron anchor groups and high specific surface area (27.77 m⋅g), FP1 shows an extreme-high U(VI) adsorption capacity (704.
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