School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 611731, PR China.
Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Strongly Coupled Quantum Matter Physics of Chinese Academy of Sciences, National Synchrotron Radiation Laboratory, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, PR China.
Nat Commun. 2023 Jan 20;14(1):340. doi: 10.1038/s41467-023-35960-z.
Renewable electricity-powered CO evolution from CO emissions is a promising first step in the sustainable production of commodity chemicals, but performing electrochemical CO reduction economically at scale is challenging since only noble metals, for example, gold and silver, have shown high performance for CO-to-CO. Cu is a potential catalyst to achieve CO reduction to CO at the industrial scale, but the C-C coupling process on Cu significantly depletes CO* intermediates, thus limiting the CO evolution rate and producing many hydrocarbon and oxygenate mixtures. Herein, we tune the CO selectivity of Cu by alloying a second metal Sb into Cu, and report an antimony-copper single-atom alloy catalyst (SbCu) of isolated Sb-Cu interfaces that catalyzes the efficient conversion of CO-to-CO with a Faradaic efficiency over 95%. The partial current density reaches 452 mA cm with approximately 91% CO Faradaic efficiency, and negligible C products are observed. In situ spectroscopic measurements and theoretical simulations reason that the atomic Sb-Cu interface in Cu promotes CO adsorption/activation and weakens the binding strength of CO*, which ends up with enhanced CO selectivity and production rates.
可再生电力驱动的 CO 排放中 CO 的演变是可持续生产商品化学品的有前途的第一步，但在经济规模上进行电化学 CO 还原具有挑战性，因为只有贵金属（例如金和银）显示出对 CO 到 CO 的高性能。Cu 是在工业规模上实现 CO 还原为 CO 的潜在催化剂，但 Cu 上的 C-C 偶联过程会大大耗尽 CO中间体，从而限制 CO 的演化速率并产生许多碳氢化合物和含氧化合物的混合物。在此，我们通过将第二种金属 Sb 合金化到 Cu 中来调整 Cu 的 CO 选择性，并报告了一种具有孤立 Sb-Cu 界面的锑铜单原子合金催化剂 (SbCu)，该催化剂能以超过 95%的法拉第效率有效地将 CO 转化为 CO。部分电流密度达到 452 mA cm，CO 的法拉第效率约为 91%，几乎观察不到 C 产物。原位光谱测量和理论模拟表明，Cu 中的原子 Sb-Cu 界面促进了 CO 的吸附/活化，并削弱了 CO的结合强度，最终提高了 CO 的选择性和产率。
