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A mononuclear copper complex as bifunctional electrocatalyst for CO2 reduction and water oxidation

机译:一种单核铜复合物作为二官能电催化剂,用于减少二氧化碳和水氧化

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摘要

To mimic natural photosynthesis, it is still a great challenge to couple catalytic CO2 reduction and water oxidation in one single system with high activity. In this work, we have successfully synthesized and characterized a tetra-coordinated mononuclear copper complex [CuIIL2](ClO4)2?2CH3OH (1) (L = methoxy-di-pyridin-2-ylmethanol) with planar configuration, which can simultaneously serve as an efficient molecular electrocatalyst for CO2 reduction and water oxidation. The copper complex displayed electrochemical activity for the reduction of CO2 to CO in DMF solution with the Faraday efficiency (FE) reached -85% and a turnover frequency (TOF) of 2.99 s?1 in the presence of proton donor water. Meanwhile, it also can perform electrocatalytic water oxidation with the FE of -86% and a high TOF of 9.20 s?1 at the pH of 11.84. The high electrochemical activity of complex 1 for the reduction of CO2 and water oxidation may due to the hydroxyl group on the methoxy-dipyridin-2-yl-methanol ligand. It represents the first copper complex as homogeneously bifunctional electrocatalyst for CO2 reduction and water oxidation.
机译:为了模拟自然光合作用,在一个高活性的单一系统中耦合催化CO2还原和水氧化仍然是一个巨大的挑战。在这项工作中,我们成功地合成并表征了四配位单核铜配合物[CuIl2](ClO4)2?平面构型的2CH3OH(1)(L=甲氧基二吡啶-2-基甲醇),可同时作为CO2还原和水氧化的高效分子电催化剂。铜配合物在DMF溶液中表现出将CO2还原为CO的电化学活性,法拉第效率(FE)达到-85%,转换频率(TOF)为2.99 s?1在质子供体水存在的情况下。同时,它还可以进行电催化水氧化,铁含量为-86%,飞行时间高达9.20秒?1,pH值为11.84。配合物1在还原二氧化碳和水氧化方面的高电化学活性可能是由于甲氧基-联吡啶-2-基-甲醇配体上的羟基。它代表了第一个铜配合物作为二氧化碳还原和水氧化的均匀双功能电催化剂。

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