Edward H. Sargent：Ga掺杂CuAl催化剂提升CO₂还原制甲烷的法拉第效率

电化学CO₂还原反应(CO₂RR)提供了一条可将间歇电流以燃料形式储存的有效路径，例如甲烷。本文作者详细论述了如何在保持高CO覆盖度的条件下打断C-C偶联、抑制析氢反应(HER)的同时提高甲烷选择性。CuAl材料在CO₂RR的活性和选择性方面位于火山曲线的顶端，作者通过在材料中引入具有较弱CO吸附能的元素Au，Zn和Ga来研究掺杂效应。受到初始甲烷选择性提升的鼓舞，作者对Ga掺杂进行了系统优化，证实高度分散的Ga对CO₂RR高选择性甲烷制备至关重要，并排除了多孔表面和粗糙度对产物选择性的影响。相比于可逆氢电极，在中性电解质，1.4 V电势条件下，Ga-掺杂CuAl催化剂能使甲烷的法拉第效率达到53%，而HER降低至23%。

The electrochemical CO₂ reduction reaction (CO₂RR) provides a route to store intermittent electricity in the form of fuels like methane. We reasoned that disrupting C-C coupling while maintaining high *CO coverage could enhance methane selectivity and suppress the hydrogen evolution reaction (HER). We studied the effect of doping CuAl, a material at the top of the CO₂RR activity and selectivity volcano plot, with elements having low *CO binding energies: Au, Zn, and Ga. Encouraged by initial improvements in selectivity to methane, we optimized the Ga content and showed that the presence of uniformly dispersed Ga is crucial in CO₂RR-to-methane performance enhancement. We rule out porosity and roughness and conclude that the presence of Ga in the doped catalysts enables high methane selectivity. The Ga-doped CuAl catalysts achieve a methane Faradaic efficiency (FE) of 53% by suppressing HER to 23% in neutral electrolyte at -1.4 V versus reversible hydrogen electrode.

李晓娜，中国科学院化学研究所，研究员。主要从事气相团簇催化反应机理研究(CO、CO₂等小分子的催化转化)，在J. Am. Chem. Soc.、Angew. Chem. Int. Ed.、Nat. Commun.、J. Phys. Chem. Lett.等期刊发表一作&通讯作者论文50余篇。2016年入选中科院青年创新促进会会员，2020年被评为青促会优秀会员。2020年获国家优秀青年科学基金项目资助。现受邀担任《化学通报》编委和《应用化学》青年编委。

Xiao-Na Li is a professor in Institute of Chemistry, Chinese Academy of Sciences (ICCAS). Her research focused on the mechanism of gas-phase cluster reactions (e.g., catalytic conversion of CO and CO₂). As the first or the corresponding author, she has more than 50 publications on international journals, including J. Am. Chem. Soc., Angew. Chem. Int. Ed., Nat. Commun., J. Phys. Chem. Lett., etc. In 2016, she became a member of Youth Innovation Promotion Association (YIPA) CAS, and in 2020, she was cited as the excellent member of YIPA. In 2020, she received the National Science Fund for Excellent Young Scholars.