Nature Catalysis ( IF 42.8 ) Pub Date : 2021-07-01 , DOI: 10.1038/s41929-021-00641-x Jun Bu , Zhenpeng Liu , Wenxiu Ma , Lei Zhang , Tao Wang , Hepeng Zhang , Qiuyu Zhang , Xinliang Feng , Jian Zhang
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 × 104 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 × 104 ml gcat–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.
中文翻译:
乙炔杂质的选择性电催化半加氢生产聚合物级乙烯
目前的乙炔热催化加氢工艺存在使用过量氢气和贵金属钯、高温和过度加氢等问题。在这里,我们报告了一种在环境条件下选择性地将乙炔杂质还原为乙烯的电催化半加氢策略。对于含有 1 × 10 4 ppm 乙炔的粗乙烯流,电化学沉积的 Cu 枝晶表现出 97% 的高比选择性,以 9.6 × 10 的大空速连续生产聚合物级乙烯流(4 ppm 乙炔)4 毫升 g猫–1 小时–1和出色的长期稳定性。理论和操作电化学拉曼研究表明,铜催化剂优异的电催化乙炔半加氢性能源于其放热的乙炔吸附和乙烯脱附。同时,电催化半加氢策略普遍适用于加氢其他炔烃杂质以生产聚合物级烯烃,例如丙烯和1,3-丁二烯。