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将银核/多孔铜壳纳米颗粒中的纳米限域与气体扩散电极相结合以改善电催化二氧化碳还原

Combining Nanoconfinement in Ag Core/Porous Cu Shell Nanoparticles with Gas Diffusion Electrodes for Improved Electrocatalytic Carbon Dioxide Reduction.

作者信息

Junqueira João R C, O'Mara Peter B, Wilde Patrick, Dieckhöfer Stefan, Benedetti Tania M, Andronescu Corina, Tilley Richard D, Gooding J Justin, Schuhmann Wolfgang

机构信息

Analytical Chemistry - Center for Electrochemical Sciences (CES) Faculty of Chemistry and Biochemistry Ruhr-Universität Bochum Universitätsstraße 150 D-44780 Bochum Germany.

School of Chemistry and Australian Centre for NanoMedicine University of New South Wales Sydney 2052 Australia.

出版信息

ChemElectroChem. 2021 Dec 13;8(24):4848-4853. doi: 10.1002/celc.202100906. Epub 2021 Dec 23.

DOI:10.1002/celc.202100906
PMID:35909946
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9303450/
Abstract

Bimetallic silver-copper electrocatalysts are promising materials for electrochemical CO reduction reaction (CORR) to fuels and multi-carbon molecules. Here, we combine Ag core/porous Cu shell particles, which entrap reaction intermediates and thus facilitate the formation of C products at low overpotentials, with gas diffusion electrodes (GDE). Mass transport plays a crucial role in the product selectivity in CORR. Conventional H-cell configurations suffer from limited CO diffusion to the reaction zone, thus decreasing the rate of the CORR. In contrast, in the case of GDE-based cells, the CORR takes place under enhanced mass transport conditions. Hence, investigation of the Ag core/porous Cu shell particles at the same potentials under different mass transport regimes reveals: (i) a variation of product distribution including C products, and (ii) a significant change in the local OH activity under operation.

摘要

双金属银铜电催化剂是用于将电化学CO还原反应(CORR)转化为燃料和多碳分子的有前景的材料。在这里,我们将Ag核/多孔Cu壳颗粒与气体扩散电极(GDE)相结合,Ag核/多孔Cu壳颗粒能够捕获反应中间体,从而在低过电位下促进C产物的形成。传质在CORR的产物选择性中起着关键作用。传统的H型电池配置存在CO向反应区扩散受限的问题,从而降低了CORR的速率。相比之下,在基于GDE的电池中,CORR在增强的传质条件下发生。因此,在不同传质条件下研究相同电位下的Ag核/多孔Cu壳颗粒揭示了:(i)包括C产物在内的产物分布变化,以及(ii)运行过程中局部OH活性的显著变化。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9fc/9303450/dcc8735f08ee/CELC-8-4848-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9fc/9303450/25d23058c277/CELC-8-4848-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9fc/9303450/4e43ec49c6ca/CELC-8-4848-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9fc/9303450/b9b93cd36852/CELC-8-4848-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9fc/9303450/2bdd5088f606/CELC-8-4848-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9fc/9303450/96cd5cd4be38/CELC-8-4848-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9fc/9303450/dcc8735f08ee/CELC-8-4848-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9fc/9303450/25d23058c277/CELC-8-4848-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9fc/9303450/4e43ec49c6ca/CELC-8-4848-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9fc/9303450/b9b93cd36852/CELC-8-4848-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9fc/9303450/2bdd5088f606/CELC-8-4848-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9fc/9303450/96cd5cd4be38/CELC-8-4848-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f9fc/9303450/dcc8735f08ee/CELC-8-4848-g007.jpg

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