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Optimizing Electrocatalyst Selectivity for CO_2 Reduction Over H_2 Evolution

机译:优化H_2生成过程中还原CO_2的电催化剂选择性

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摘要

The electrocatalytic reduction of CO_2 to fuels or chemicals is an attractive alternative to fossil- or biomass-based feedstocks. However, since the reduction typically requires protons in the reaction pathway, the evolution of H_2 is a common side reaction; in practice H_2 often dominates the observed products. In the current work, ways in which the selectivity between these two reactions can be understood and optimized are presented. First, it is shown that the identification and optimization of the expression of active edge sites in nanostructured Au catalysts for CO evolution results in catalysts with extremely high selectivities and mass activities at low overpotentials. Second, it is shown that the reactive state of the catalyst surface can have a strong steering effect on the selectivity. Fundamental adsorbate-adsorbate interactions drive the reactivity and selectivity across more reactive catalyst surfaces, and it is shown that in the example cases of Cu and Mo catalysts, the interaction can have opposite qualitative trends.
机译:将CO_2电催化还原为燃料或化学物质是基于化石或生物质原料的有吸引力的替代方法。但是,由于还原通常需要在反应路径中形成质子,因此H_2的逸出是常见的副反应。在实践中,H_2通常主导着观察到的产物。在当前的工作中,提出了可以理解和优化这两个反应之间选择性的方法。首先,显示出用于CO放出的纳米结构Au催化剂中活性边缘位点的表达的鉴定和优化导致了在低超电势下具有极高的选择性和质量活性的催化剂。其次,表明催化剂表面的反应态可以对选择性具有强烈的控制作用。基本的被吸附物-被吸附物相互作用驱动更多反应性催化剂表面上的反应性和选择性,并且表明在Cu和Mo催化剂的示例情况下,该相互作用可以具有相反的定性趋势。

著录项

  • 来源
  • 会议地点 Chicago IL(US)
  • 作者

    A. A. Peterson;

  • 作者单位

    School of Engineering, Brown University, Providence, Rhode Island, 02912, USA;

  • 会议组织
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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