Theory-Guided Enhancement of CO2 Reduction to Ethanol on Ag–Cu Tandem Catalysts via Particle-Size Effects,ACS Catalysis

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Theory-Guided Enhancement of CO2 Reduction to Ethanol on Ag–Cu Tandem Catalysts via Particle-Size Effects
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-10-18 , DOI: 10.1021/acscatal.1c03717
Pranit Iyengar ₁ , Manuel J. Kolb ₂ , James Pankhurst ₁ , Federico Calle-Vallejo ₂ , Raffaella Buonsanti ₁

Affiliation

In the CO₂ reduction reaction, the design of electrocatalysts that selectively promote alcohols over hydrocarbons (e.g., ethanol over ethylene) hinges on the understanding of the pathways and specific sites that form alcohols. Herein, theoretical considerations guide state-of-the-art synthesis of well-defined catalysts to show that higher selectivity toward ethanol is achieved on Cu(110) edge sites compared to Cu(100) terraces. Specifically, we study the catalytic behavior of Cu nano-cubes (Cu_cub) of different sizes in the framework of tandem catalysis with CO-producing Ag nano-spheres. We predict and experimentally find that the smaller Cu_cub possess higher selectivity for ethanol in view of their larger edge-to-faces ratio and of the fact that ethylene is produced at terraces while ethanol is selectively produced at step edges. These results call for synthetic developments toward Cu nanostructures exposing only edge sites, such as hollow cubic nanocages, to further increase ethanol selectivity. More generally, this study encourages the application of well-defined nano catalysts as a bridge between theory and experiments in electrocatalysis.

中文翻译：

理论指导下通过粒度效应在 Ag-Cu 串联催化剂上促进 CO2 还原为乙醇

在 CO ₂还原反应中，选择性地促进醇而不是烃（例如乙醇而不是乙烯）的电催化剂的设计取决于对形成醇的途径和特定位点的理解。在此，理论考虑指导了定义明确的催化剂的最先进合成，以表明与 Cu(100) 平台相比，在 Cu(110) 边缘位点上实现了对乙醇的更高选择性。具体而言，我们研究了不同尺寸的 Cu 纳米立方体 (Cu _cub ) 在与产生 CO 的 Ag 纳米球串联催化的框架中的催化行为。我们预测并通过实验发现较小的 Cu_幼崽鉴于其较大的边面比以及乙烯在梯田生产而乙醇在阶梯边缘选择性生产的事实，它们对乙醇具有更高的选择性。这些结果要求对仅暴露边缘位点（如空心立方纳米笼）的 Cu 纳米结构进行合成开发，以进一步提高乙醇选择性。更一般地说，这项研究鼓励应用定义明确的纳米催化剂作为电催化理论和实验之间的桥梁。

更新日期：2021-11-05

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