Metal phthalocyanines as efficient electrocatalysts for acetylene semihydrogenation

CHEMICAL ENGINEERING JOURNAL(2022)

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摘要
Compared to their booming thermocatalytic counterparts, electrocatalytic acetylene semihydrogenation still remain stagnant owing to its low activity and poor selectivity. Here, we first explore metal phthalocyanines (M (Pc)s) featuring a defined metal coordination environment as electrocatalysts for acetylene semihydrogenation. Consequently, CoPc exhibits an ethylene current density of 150.8 mA cm(-2) and a -96% ethylene faradaic efficiency under a pure acetylene stream. In-situ electrochemical Raman and theoretical calculations demonstrate that CoPc favors acetylene absorption/hydrogenation processes. Even for crude ethylene containing 1 x 10(4) ppm acetylene, CoPc manifests a -99.5% acetylene conversion, a high turnover frequency of 4.86 x 10(-3) s(-1) and a large space velocity of 2.4 x 10(5) ml.g(cat)(-1).h(-1), outperforming those for reported thermocatalysts. This work facilitates the development of electrocatalytic acetylene semihydrogenation and promises alternatives to traditional thermocatalytic processes.
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关键词
Metal phthalocyanines,Electrocatalysts,Acetylene,Semihydrogenation,Ethylene
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