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使用三元 Pd/CuO-Cu 催化剂进行二氧化碳电还原。

Electrohydrogenation of Carbon Dioxide using a Ternary Pd/Cu O-Cu Catalyst.

机构信息

School of Chemistry, Monash University, Clayton, Victoria, 3800, Australia.

State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering, College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan, Ningxia, 750021, P. R. China.

出版信息

ChemSusChem. 2019 Oct 8;12(19):4471-4479. doi: 10.1002/cssc.201901636. Epub 2019 Sep 3.

Abstract

A simple one-pot method has been developed to synthesize a palladium/cuprous oxide-copper (Pd/Cu O-Cu) material with a well-defined structure, by modification of Cu O-Cu with Pd through a galvanic replacement reaction. Compared with the well-known copper/cuprous oxide (Cu/Cu O) catalysts, the Pd/Cu O-Cu material can catalyze the electroreduction of CO into C products with much higher faradaic efficiencies at lower overpotentials in a CO -saturated 0.5 m NaHCO solution. In particular, the highest faradaic efficiencies of 92 % for formate and 30 % for methane were achieved at -0.25 and -0.65 V (vs. the reversible hydrogen electrode), respectively. The improvement is suggested to be the result of a synergistic effect between PdH and the catalytically active copper sites during electrochemical CO reduction.

摘要

一种简单的一锅法已经被开发出来,通过电置换反应用钯对氧化铜-铜(CuO-Cu)进行修饰,从而合成具有明确结构的钯/氧化亚铜-铜(Pd/CuO-Cu)材料。与著名的铜/氧化亚铜(Cu/CuO)催化剂相比,在 CO 饱和的 0.5m NaHCO3 溶液中,Pd/CuO-Cu 材料在更低的过电势下,可以催化 CO 电化学还原为 C 产物,具有更高的法拉第效率。特别是,在-0.25 和-0.65V(相对于可逆氢电极)时,甲酸的最高法拉第效率达到 92%,甲烷的最高法拉第效率达到 30%。这种改进被认为是在电化学 CO 还原过程中 PdH 和催化活性铜位之间协同作用的结果。

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