Wang Suheng, Uwakwe Kelechi, Yu Liang, Ye Jinyu, Zhu Yuezhou, Hu Jingting, Chen Ruixue, Zhang Zheng, Zhou Zhiyou, Li Jianfeng, Xie Zhaoxiong, Deng Dehui
State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
Nat Commun. 2021 Dec 6;12(1):7072. doi: 10.1038/s41467-021-27372-8.
Renewable energy-based electrocatalytic hydrogenation of acetylene to ethylene (E-HAE) under mild conditions is an attractive substitution to the conventional energy-intensive industrial process, but is challenging due to its low Faradaic efficiency caused by competitive hydrogen evolution reaction. Herein, we report a highly efficient and selective E-HAE process at room temperature and ambient pressure over the Cu catalyst. A high Faradaic efficiency of 83.2% for ethylene with a current density of 29 mA cm is reached at -0.6 V vs. the reversible hydrogen electrode. In-situ spectroscopic characterizations combined with first-principles calculations reveal that electron transfer from the Cu surface to adsorbed acetylene induces preferential adsorption and hydrogenation of the acetylene over hydrogen formation, thus enabling a highly selective E-HAE process through the electron-coupled proton transfer mechanism. This work presents a feasible route for high-efficiency ethylene production from E-HAE.
在温和条件下,基于可再生能源的乙炔电催化加氢制乙烯(E-HAE)是传统能源密集型工业过程的一种有吸引力的替代方法,但由于竞争性析氢反应导致法拉第效率较低,该过程具有挑战性。在此,我们报道了在室温及常压下,在铜催化剂上实现的高效且选择性的E-HAE过程。相对于可逆氢电极,在-0.6 V时,乙烯的法拉第效率高达83.2%,电流密度为29 mA cm 。原位光谱表征与第一性原理计算相结合表明,电子从铜表面转移到吸附的乙炔上,导致乙炔比氢更优先吸附和加氢,从而通过电子耦合质子转移机制实现了高选择性的E-HAE过程。这项工作为通过E-HAE高效生产乙烯提供了一条可行的途径。