Hu Fei, Yang Li, Jiang Yawen, Duan Chongxiong, Wang Xiaonong, Zeng Longjiao, Lv Xuefeng, Duan Delong, Liu Qi, Kong Tingting, Jiang Jun, Long Ran, Xiong Yujie
School of Materials Science and Energy Engineering, Guangdong Key Laboratory for Hydrogen Energy Technologies, Foshan University, Foshan, Guangdong, 528000, China.
Hefei National Laboratory for Physical Sciences at the Microscale, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026, China.
Angew Chem Int Ed Engl. 2021 Dec 6;60(50):26122-26127. doi: 10.1002/anie.202110303. Epub 2021 Nov 9.
Production of multicarbon (C ) liquid fuels is a challenging task for electrocatalytic CO reduction, mainly limited by the stabilization of reaction intermediates and their subsequent C-C couplings. In this work, we report a unique catalyst, the coordinatively unsaturated Cu sites on amorphous CuTi alloy (a-CuTi@Cu) toward electrocatalytic CO reduction to multicarbon (C ) liquid fuels. Remarkably, the electrocatalyst yields ethanol, acetone, and n-butanol as major products with a total C faradaic efficiency of about 49 % at -0.8 V vs. reversible hydrogen electrode (RHE), which can be maintained for at least 3 months. Theoretical simulations and in situ characterization reveals that subsurface Ti atoms can increase the electron density of surface Cu sites and enhance the adsorption of *CO intermediate, which in turn reduces the energy barriers required for *CO dimerization and trimerization.
对于电催化CO还原反应而言，生产多碳（C）液体燃料是一项具有挑战性的任务，主要受限于反应中间体的稳定性及其后续的C-C偶联反应。在本工作中，我们报道了一种独特的催化剂，即非晶态CuTi合金（a-CuTi@Cu）上的配位不饱和Cu位点，用于电催化CO还原制备多碳（C）液体燃料。值得注意的是，该电催化剂以乙醇、丙酮和正丁醇作为主要产物，在相对于可逆氢电极（RHE）为-0.8 V时，总C法拉第效率约为49%，且该效率至少可维持3个月。理论模拟和原位表征表明，亚表面Ti原子可增加表面Cu位点的电子密度，并增强CO中间体的吸附，进而降低CO二聚和三聚所需的能垒。
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