Electrochemical CO2 reduction reaction (CO2RR) 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 CO2 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 CO2RR 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 CO2⋅− formation to activate CO2 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. Further integration of the robust electron‐rich Bi nanosheets into III–V‐based photovoltaic solar cell results in an unassisted artificial leaf with a high solar‐to‐formate (STF) efficiency of 13.7 %.

No abstract

In this study, the ultra-thin iron phosphate Fe7(PO4)6 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 m2·g−1), FP1 shows an extreme-high U(VI) adsorption capacity (704.23 mg·g−1 at 298 K, pH = 5.0 ± 0.1), which is about 27 times of conventional 3D Fe7(PO4)6 (24.51 mg·g−1-sample FP2) and higher than most 2D absorbent materials, showing a great value in the treatment of radioactive wastewater. According to the adsorption results, the sorption between U(VI) and FP1 is spontaneous and endothermic, and can be conformed to single molecular layer adsorption. Based on the analyses of FESEM, EDS, Mapping, FT-IR and XRD after adsorption, the possibile adsorption mechanism can be described as a Monolayer Surface Complexation and Stacking mode (MSCS-Mode). Additionally, the research not only provide a novel preparing method for 2D phosphate materials but also pave a new pathway to study other two-dimensional adsorption materials.

The 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) low activity and selectivity caused by the competitive adsorption of HMF and OH− and 2) low operational stability caused by the uncontrollable reconstruction of the catalyst. To overcome these limitations, a series of Ni3S2/NiOx‐n catalysts with controllable compositions and well‐defined structures were synthesized using a novel in‐situ controlled surface reconstruction strategy. The adsorption behavior of HMF and OH− could be continuously adjusted by varying the ratio of NiOx to Ni3S2 on the catalysts surface, as indicated by in‐situ characterizations, contact angle analysis and theoretical simulations. Owing to the balanced competitive adsorption of HMF and OH−, the optimized Ni3S2/NiOx‐15 catalyst exhibited remarkable HMF electrocatalytic oxidation performance, with the current density reaching 366 mA cm−2 at 1.5 VRHE and the Faradaic efficiency of the product, 2,5‐furanedicarboxylic acid, reaching 98%. Moreover, Ni3S2/NiOx‐15 exhibited excellent durability, with its activity and structure remaining stable for over 100 h of operation. This study provides a new route for the design and construction of catalysts for value‐added biomass conversion and offers new insights into enhancing catalytic performance by balancing competitive adsorption.This article is protected by copyright. All rights reserved

Photoconversion of CO2 and H2O 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 Bi2WO6 (BP/BWO) was constructed for photocatalytic CO2 reduction coupling with benzylamine (BA) oxidation. The as‐prepared BP/BWO catalyst exhibits a superior photocatalytic performance toward CO2 reduction, with a yield of 61.3 μmol g−1 h−1 for ethanol (selectivity of 91 %).In situ spectroscopic studies and theoretical calculations reveal that S‐scheme heterojunction can effectively promote photogenerated carrier separation via the Bi−O−P bridge to accelerate the PCET process. Meanwhile, electron‐rich BP acts as the active site and plays a vital role in the process of C−C coupling. In addition, the substitution of BA oxidation for H2O oxidation can further enhance the photocatalytic performance of CO2 reduction to C2H5OH. This work opens a new horizon for exploring novel heterogeneous photocatalysts in CO2 photoconversion to C2H5OH based on cooperative photoredox systems.