Selective electrocatalytic semihydrogenation of acetylene impurities for the production of polymer-grade ethylene

被引:122
|
作者
Bu, Jun [1 ,2 ]
Liu, Zhenpeng [1 ,2 ]
Ma, Wenxiu [1 ,2 ]
Zhang, Lei [1 ,2 ]
Wang, Tao [3 ]
Zhang, Hepeng [1 ,2 ]
Zhang, Qiuyu [1 ,2 ]
Feng, Xinliang [4 ,5 ]
Zhang, Jian [1 ,2 ]
机构
[1] Northwestern Polytech Univ, Sch Chem & Chem Engn, Minist Ind & Informat Technol, Key Lab Special Funct & Smart Polymer Mat, Xian, Peoples R China
[2] Northwestern Polytech Univ, Sch Chem & Chem Engn, Dept Adv Chem Engn, Xian, Peoples R China
[3] Westlake Univ, Ctr Artificial Photosynth Solar Fuels, Sch Sci, Hangzhou, Peoples R China
[4] Tech Univ Dresden, Ctr Adv Elect Dresden Cfaed, Dresden, Germany
[5] Tech Univ Dresden, Fac Chem & Food Chem, Dresden, Germany
基金
中国国家自然科学基金;
关键词
TOTAL-ENERGY CALCULATIONS; ELECTROCHEMICAL HYDROGENATION; CO2; ELECTROREDUCTION; PALLADIUM; REDUCTION; CATALYSTS; COPPER; ELECTRODES; KINETICS; METALS;
D O I
10.1038/s41929-021-00641-x
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The current thermocatalytic acetylene hydrogenation process suffers from the use of excessive hydrogen and the noble metal Pd, high temperatures and overhydrogenation. Here we report an electrocatalytic semihydrogenation strategy to selectively reduce acetylene impurities to ethylene under ambient conditions. For a crude ethylene flow that contains 1 x 10(4) ppm acetylene, electrochemically deposited Cu dendrites exhibited a high specific selectivity of 97%, continuous production of a polymer-grade ethylene stream (4 ppm acetylene) at a large space velocity of 9.6 x 10(4) ml g(cat)(-1) h(-1) and excellent long-term stability. Theoretical and operando electrochemical Raman investigations revealed that the outstanding electrocatalytic acetylene semihydrogenation performance of Cu catalysts originates from its exothermic acetylene adsorption and ethylene desorption. Meanwhile, the electrocatalytic semihydrogenation strategy is universally applicable for hydrogenating other alkyne impurities to produce polymer-grade olefins, for example, propylene and 1,3-butadiene.
引用
收藏
页码:557 / 564
页数:8
相关论文
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