The electrochemical CO reduction reaction (CO RR) over Cu-based catalysts shows great potential for converting CO into multicarbon (C ) fuels and chemicals. Herein, we introduce an A M O structure into a Cu-based catalyst through a solid-state reaction synthesis method. The Cu P O catalyst is electrochemically reduced to metallic Cu with a significant structure evolution from grain aggregates to highly porous structure under CO RR conditions. The reconstructed Cu P O catalyst achieves a Faradaic efficiency of 73.6 % for C products at an applied current density of 350 mA cm , remarkably higher than the CuO counterparts. The reconstructed Cu P O catalyst has a high electrochemically active surface area, abundant defects, and low-coordinated sites. In situ Raman spectroscopy and density functional theory calculations reveal that CO adsorption with bridge and atop configurations is largely improved on Cu with defects and low-coordinated sites, which decreased the energy barrier of the C-C coupling reaction for C products.
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http://dx.doi.org/10.1002/anie.202114238 | DOI Listing |
Adv Mater
January 2025
School of Chemistry, The University of New South Wales, Sydney, NSW, 2052, Australia.
The electrocatalytic synthesis of multicarbon compounds from CO is a promising method for storing renewable electricity and addressing global CO issues. Single-atom catalysts are promising candidates for CO reduction, but producing high-value multicarbon (C) products using a single-atom structure remains a significant challenge. In this study, a fluorine doping strategy is proposed to facilitate the reconstruction of isolated Cu atoms, promoting multicarbon generation.
View Article and Find Full Text PDFJ Colloid Interface Sci
January 2025
Key Laboratory of Fine Chemicals of College of Heilongjiang Province, Qiqihar University, Qiqihar 161006, China; School of Materials Science and Engineering, Jiamusi University, Jiamusi 154007, China. Electronic address:
Most transition metal-based electrocatalysts, when used for the oxygen evolution reaction (OER), undergo significant restructuring under alkaline conditions, forming localized oxides/hydroxides (MOOH), which act as the real active centers, activating adjacent metal sites and creating new active sites that enhance electrocatalytic behavior. Nevertheless, inducing rapid and in-depth self-reconstruction of catalyst surfaces remains a huge challenge. Herein, this work achieves rapid and in-depth self-reconstruction by doping fluorine into the lattice of transition metal oxides (MO).
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Hong Kong 999077, P. R. China.
Fe-N-C materials are emerging catalysts for replacing precious platinum in the oxygen reduction reaction (ORR) for renewable energy conversion. However, their potential is hindered by sluggish ORR kinetics, leading to a high overpotential and impeding efficient energy conversion. Using iron phthalocyanine (FePc) as a model catalyst, we elucidate how the local strain can enhance the ORR performance of Fe-N-Cs.
View Article and Find Full Text PDFSmall
January 2025
Institute for Sustainable Energy and Resources, Key Laboratory of Shandong Provincial Universities for Functional Molecules and Materials, College of Chemistry and Chemical Engineering, Qingdao University, Qingdao, Shandong, 266071, China.
Alkaline water (HO) electrolysis is currently a commercialized green hydrogen (H) production technology, yet the unsatisfactory hydrogen evolution reaction (HER) performance severely limits its energy conversion efficiency and cost reduction. Herein, PtRuFeCoNi high entropy alloys (HEAs) is synthesized and subsequently exploited electrochemically induced structural oxidation processes to construct self-reconfigurable HEAs, as an efficient alkaline HER catalyst. The optimized self-reconstructed PtRuFeCoNi HEAs with the HEAs and cobalt rutheniate interface (HEAs-CoRuO) exhibits excellent alkaline HER performance, requiring just 11.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong SAR 999077, China.
Carboranyl amines are distinct from typical organic amines. Due to the electronic influence of the carborane cage, they have low nucleophilicity and are reluctant to alkylate. Moreover, asymmetric synthesis of chiral carboranes is still in its infancy.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!