Mechanistic Insights into the Electrochemical Reduction of CO2 to CO on Nanostructured Ag Surfaces

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2015-06-05 DOI:10.1021/acscatal.5b00840

Jonathan Rosen, Gregory S. Hutchings, Qi Lu, Sean Rivera, Yang Zhou, Dionisios G. Vlachos, Feng Jiao*

引用次数: 395

Abstract

Electroreduction of CO₂ in a highly selective and efficient manner is a crucial step toward CO₂ utilization. Nanostructured Ag catalysts have been found to be effective candidates for CO₂ to CO conversion. In this report, we combine experimental and computational efforts to explore the electrocatalytic reaction mechanism of CO₂ reduction on nanostructured Ag catalyst surfaces in an aqueous electrolyte. In contrast to bulk Ag catalysts, both nanoparticle and nanoporous Ag catalysts show enhanced ability to reduce the activation energy of the CO₂ to COOH_ads intermediate step through the low-coordinated Ag surface atoms, resulting in a reaction mechanism involving a fast first electron and proton transfer followed by a slow second proton transfer as the rate-limiting step.

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纳米结构银表面CO2电化学还原成CO的机理研究

以高选择性和高效率的方式电还原CO2是实现CO2利用的关键一步。纳米结构的银催化剂已被发现是CO2到CO转化的有效候选者。在本报告中，我们将实验和计算相结合，探讨了水电解质中纳米结构Ag催化剂表面上CO2还原的电催化反应机理。与块体Ag催化剂相比，纳米颗粒和纳米多孔Ag催化剂通过低配位的Ag表面原子降低CO2到COOHads中间步骤的活化能的能力增强，导致反应机制为快速的第一个电子和质子转移，然后缓慢的第二次质子转移作为限速步骤。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.