Structure Sensitivity in the Electrocatalytic Reduction of CO2 with Gold Catalysts,Angewandte Chemie International Edition

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Structure Sensitivity in the Electrocatalytic Reduction of CO2 with Gold Catalysts
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2019-02-11 , DOI: 10.1002/anie.201811422
Stefano Mezzavilla _{1,

2} , Sebastian Horch ₁ , Ifan E. L. Stephens _{1,

3} , Brian Seger ₁ , Ib Chorkendorff ₁

Affiliation

An understanding of the influence of structural surface features on electrocatalytic reactions is vital for the development of efficient nanostructured catalysts. Gold is the most active and selective known electrocatalyst for the reduction of CO₂ to CO in aqueous electrolytes. Numerous strategies have been proposed to improve its intrinsic activity. Nonetheless, the atomistic knowledge of the nature of the active sites remains elusive. We systematically investigated the structure sensitivity of Au single crystals for electrocatalytic CO₂ reduction. Reaction kinetics for the formation of CO are strongly dependent on the surface structure. Under‐coordinated sites, such as those present in Au(110) and at the steps of Au(211), show at least 20‐fold higher activity than more coordinated configurations (for example, Au(100)). By selectively poisoning under‐coordinated sites with Pb, we have confirmed that these are the active sites for CO₂ reduction.

中文翻译：

金催化剂电催化还原CO2的结构敏感性。

了解结构表面特征对电催化反应的影响对于开发高效的纳米结构催化剂至关重要。金是用于将水性电解质中的CO ₂还原为CO的最活跃和选择性最高的已知电催化剂。已经提出了许多策略来改善其内在活性。但是，关于活性位点性质的原子学知识仍然难以捉摸。我们系统地研究了金单晶对电催化CO ₂的结构敏感性减少。形成CO的反应动力学在很大程度上取决于表面结构。配位不足的位点（例如Au（110）和Au（211）的步骤中存在的位点）显示的活性比配位更强的配置（例如Au（100））至少高20倍。通过用Pb选择性地毒害配位不足的位点，我们证实了这些是CO ₂还原的活性位点。

更新日期：2019-02-11

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