Production of multicarbon products (C ) from CO electroreduction reaction (CO RR) is highly desirable for storing renewable energy and reducing carbon emission. The electrochemical synthesis of CO RR catalysts that are highly selective for C products via electrolyte-driven nanostructuring is presented. Nanostructured Cu catalysts synthesized in the presence of specific anions selectively convert CO into ethylene and multicarbon alcohols in aqueous 0.1 m KHCO solution, with the iodine-modified catalyst displaying the highest Faradaic efficiency of 80 % and a partial geometric current density of ca. 31.2 mA cm for C products at -0.9 V vs. RHE. Operando X-ray absorption spectroscopy and quasi in situ X-ray photoelectron spectroscopy measurements revealed that the high C selectivity of these nanostructured Cu catalysts can be attributed to the highly roughened surface morphology induced by the synthesis, presence of subsurface oxygen and Cu species, and the adsorbed halides.
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http://dx.doi.org/10.1002/anie.201910155 | DOI Listing |
ACS Nano
January 2025
Songshan Lake Materials Laboratory (SLAB), Dongguan 523808, P. R. China.
Electrocatalytic CO reduction into high-value multicarbon products offers a sustainable approach to closing the anthropogenic carbon cycle and contributing to carbon neutrality, particularly when renewable electricity is used to power the reaction. However, the lack of efficient and durable electrocatalysts with high selectivity for multicarbons severely hinders the practical application of this promising technology. Herein, a nanoporous defective AuCu single-atom alloy (De-AuCu SAA) catalyst is developed through facile low-temperature thermal reduction in hydrogen and a subsequent dealloying process, which shows high selectivity toward ethylene (CH), with a Faradaic efficiency of 52% at the current density of 252 mA cm under a potential of -1.
View Article and Find Full Text PDFSmall Methods
January 2025
Liquid Sunlight Alliance, Lawrence Berkeley National Laboratory, 1 Cyclotron Rd, Berkeley, CA, 94720, United States.
Copper-tantalate, CuTaO (CTO), shows significant promise as an efficient photocathode for multi-carbon compounds (C) production through photoelectrochemical (PEC) CO reduction, owing to its suitable energy bands and catalytic surface. However, synthesizing CTO poses a significant challenge due to its metastable nature and thermal instability. In this study, this challenge is addressed by employing a flux-mediated synthesis technique using a sodium-based flux to create sodium-doped CTO (Na-CTO) thin films, providing enhanced nucleation and stabilization for the CTO phase.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, 230026, Hefei, China.
Electrolysis of carbon dioxide (CO) in acid offers a promising route to overcome CO loss in alkaline and neutral electrolytes, but requires concentrated alkali cations (typical ≥3 M) to mitigate the trade-off between low pH and high hydrogen evolution reaction (HER) rate, causing salt precipitation. Here we report a strategy to resolve this problem by introducing tensile strain in a copper (Cu) catalyst, which can selectively reduce CO to valuable multicarbon products, particularly ethylene, in a pH 1 electrolyte with 1 M potassium ions. We find that the tension-strained Cu creates an electron-rich surface that concentrates diluted potassium ions, contributing to CO activation and HER suppression.
View Article and Find Full Text PDFNat Energy
September 2024
Department of Interface Science, Fritz-Haber Institute of the Max-Planck Society, Berlin, Germany.
Electrochemical reduction of CO (CORR) to multi-carbon products is a promising technology to store intermittent renewable electricity into high-added-value chemicals and close the carbon cycle. Its industrial scalability requires electrocatalysts to be highly selective to certain products, such as ethylene or ethanol. However, a substantial knowledge gap prevents the design of tailor-made materials, as the properties ruling the catalyst selectivity remain elusive.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2024
Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, P. R. China.
An efficient electrocatalytic conversion of CO into valuable multicarbon (C) products requires enhanced C-C coupling of C1 intermediates. Herein, we combine a tandem effect with a confinement strategy to construct a hollow CuO@Ag nanoshell electrocatalyst with a well-defined porous structure to improve the *CO intermediate coverage on the catalyst surface. In CO electroreduction, in situ Raman spectroscopy shows that the introduction of Ag can not only promote the CO intermediate production but also improve the stability of Cu to capture the *CO intermediate due to a CO-tandem effect, and the fine-tuned hollowness degree and pore size of CuO@Ag create a spatially confined microenvironment for trapping CO as well as the enrichment of CO, which greatly facilitate subsequent C-C coupling for C product.
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