Laboratory of Nanochemistry for Energy (LNCE), Department of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne, CH-1950 Sion, Switzerland.
Acc Chem Res. 2022 Mar 1;55(5):629-637. doi: 10.1021/acs.accounts.1c00673. Epub 2022 Feb 9.
The carbon-neutral production of fuels and chemical feedstocks is one of the grand challenges for our society to solve. The electrochemical conversion of CO is emerging as a promising technology contributing to this goal. Despite the huge amount of progress made over the past decade, selectivity still remains a challenge. This Account presents an overview of recent progress in the design of selective catalysts by exploiting the structural sensitivity of the electrochemical CO reduction reaction (CORR). In particular, it shows that the accurate and precise control of the shape and size of Cu nanocatalysts is instrumental in understanding and in discovering the structure-selectivity relationships governing the reduction of CO to valuable hydrocarbons, such as methane and ethylene. It further illustrates the use of faceted Cu nanocatalysts to interrogate catalytic pathways and to increase selectivity toward oxygenates, such as ethanol, in the framework of tandem schemes. The last part of the Account highlights the role of well-defined nanocatalysts in identifying reconstruction mechanisms which might occur during operation. An outlook for the emerging paradigms which will empower the design of novel catalysts for CORR concludes the Account.
实现燃料和化学原料的碳中和生产是我们社会需要解决的重大挑战之一。电化学转化 CO 是一种很有前途的技术，有助于实现这一目标。尽管在过去十年中取得了巨大的进展，但选择性仍然是一个挑战。本账户介绍了通过利用电化学 CO 还原反应 (CORR) 的结构敏感性来设计选择性催化剂的最新进展。特别是，它表明精确控制 Cu 纳米催化剂的形状和尺寸对于理解和发现控制 CO 还原为有价值的碳氢化合物（如甲烷和乙烯）的结构选择性关系至关重要。它进一步说明了使用各向异性 Cu 纳米催化剂来探究催化途径，并在串联方案中提高对醇类（如乙醇）等含氧物的选择性。该账户的最后一部分强调了在确定操作过程中可能发生的重构机制方面，定义明确的纳米催化剂的作用。最后总结了新兴范例，这些范例将为 CORR 新型催化剂的设计提供支持。
