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Highly efficient ethylene production via electrocatalytic hydrogenation of acetylene under mild conditions
Nature Communications ( IF 16.6 ) Pub Date : 2021-12-06 , DOI: 10.1038/s41467-021-27372-8
Suheng Wang 1, 2 , Kelechi Uwakwe 2, 3 , Liang Yu 2, 3 , Jinyu Ye 1 , Yuezhou Zhu 1 , Jingting Hu 1, 2 , Ruixue Chen 1, 2 , Zheng Zhang 1, 2 , Zhiyou Zhou 1 , Jianfeng Li 1 , Zhaoxiong Xie 1 , Dehui Deng 1, 2, 3
Affiliation  

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−2 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.



中文翻译:

温和条件下乙炔电催化加氢高效生产乙烯

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有吸引力的替代品,但由于竞争性析氢反应导致其法拉第效率低,因此具有挑战性。在此,我们报告了一种在室温和环境压力下在 Cu 催化剂上的高效和选择性 E-HAE 工艺。乙烯法拉第效率高达 83.2%,电流密度为 29 mA cm -2与可逆氢电极相比,在 -0.6 V 时达到。原位光谱表征结合第一性原理计算表明,电子从铜表面转移到吸附的乙炔会导致乙炔优先吸附和氢化而不是氢形成,从而通过电子耦合质子转移实现高选择性的 E-HAE 过程机制。这项工作为 E-HAE 高效生产乙烯提供了一条可行的途径。

更新日期:2021-12-06
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