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Enhancing Molecular Electrocatalysis of CO2 Reduction with Pressure-Tunable CO2 -Expanded Electrolytes.
ChemSusChem ( IF 8.4 ) Pub Date : 2020-03-20 , DOI: 10.1002/cssc.202000390
David J Sconyers 1, 2 , Charles I Shaughnessy 1, 3 , Hyun-Jin Lee 1 , Bala Subramaniam 1, 3 , Kevin C Leonard 1, 3 , James D Blakemore 1, 2
Affiliation  

Electrochemical studies of CO2 conversion by molecular catalysts are typically carried out in a narrow range of near‐ambient CO2 pressures wherein low CO2 solubilities in the liquid phase can limit the rate of CO2 reduction. In this study, five‐fold rate enhancements are enabled by pairing CO2‐expanded electrolytes (CXEs), a class of media that accommodate multimolar concentrations of CO2 in organic solvents at modest pressures, with a homogeneous molecular electrocatalyst, [Re(CO)3(bpy)Cl] (1, bpy=2,2′‐bipyridyl). Analysis of cyclic voltammetry data reveals pressure‐tunable rate behavior, with first‐order kinetics at moderate CO2 pressures giving way to zero‐order kinetics at higher pressures. The significant enhancement in the space‐time yield of CO demonstrates that CXEs offer a simple yet powerful strategy for unlocking the intrinsic potential of molecular catalysts by mitigating CO2 solubility limitations commonly encountered in conventional liquid electrolytes. Moreover, our findings reveal that 1, a workhorse molecular catalyst, performs with intrinsic kinetic behavior, which is competitive with fast enzymes under optimal conditions in CXEs.

中文翻译:

用可调压的CO2膨胀电解质增强分子对CO2还原的电催化作用。

分子催化剂对CO 2转化的电化学研究通常在狭窄的CO 2压力范围内进行,其中液相中低的CO 2溶解度会限制CO 2的还原速率。在这项研究中,5倍速率的增强是通过配对CO启用2 -expanded电解质(CXEs),一类的媒体容纳CO的浓度multimolar 2在适度的压力下在有机溶剂中,用均一的分子电催化剂,[的Re(CO )3(bpy)Cl](1,bpy = 2,2'-联吡啶基)。循环伏安法数据分析显示压力可调速率行为,在中等CO时具有一级动力学2个压力让位于更高压力下的零级动力学。CO时空产率的显着提高表明,CXE提供了一种简单而有效的策略,可通过减轻常规液体电解质中常见的CO 2溶解度限制来释放分子催化剂的内在潜力。此外,我们的研究结果表明,1,一个主力分子催化剂,具有固有的动力学行为,这与在CXEs最佳条件下快速酶竞争的进行。
更新日期:2020-03-20
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