Impact of the Dissolved Anion on the Electrocatalytic Reduction of CO2 to CO with Ruthenium CNC Pincer Complexes
Impact of the Dissolved Anion on the Electrocatalytic Reduction of CO2 to CO with Ruthenium CNC Pincer Complexes
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DOI：
10.1002/cctc.202000742
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发表时间：
2020-10
期刊：
影响因子：
4.5
通讯作者：
Hunter Shirley;Matthew T. Figgins;Chance M. Boudreaux;Nalaka P. Liyanage;R. W. Lamb;C. E. Webster;Elizabeth T. Papish;J. Delcamp
中科院分区：
文献类型：
--
作者：
Hunter Shirley;Matthew T. Figgins;Chance M. Boudreaux;Nalaka P. Liyanage;R. W. Lamb;C. E. Webster;Elizabeth T. Papish;J. Delcamp
三个钌电催化剂的反应性示出调制通过添加阴离子更有选择性和更快的电催化。控制电位电解研究证实了从CO2生成CO。通过向反应溶液中引入Cl-，研究了三种钌催化剂的法拉第效率。有趣的是，一个中性的钌配位络合物与相关的氯化物也给出了相同或更快的催化速率时，Cl−加成。在这份报告中，系统地研究了添加卤化物（I-，Br-，Cl-和F-）与不同的抗衡阳离子（K+和TBA+）在有水和无水的情况下的影响。计算分析提供了这种有趣的增加FE的基础上阴离子添加的见解。这些结果表明，向电催化反应混合物中添加阴离子增加了额外的参数，以提高催化的速率和选择性，其中一个实施例对于CO生产从19%FE提高到91%FE。
The reactivity of three ruthenium electrocatalysts is shown to be modulated through the addition of anions for more selective and faster electrocatalysis. Controlled potential electrolysis studies confirm the generation of CO from CO2. The Faradaic efficiency increased for the three ruthenium catalysts studied through the introduction of Cl– to the reaction solution. Interestingly, a neutral ruthenium coordination complex with an associated chloride also gave equal or faster rates of catalysis upon Cl− addition. In this report, a systematic study on the effects of added halides (I−, Br−, Cl−, and F−) with varied counter cations (K+ and TBA+) with and without water is examined. Computational analysis provides insights into this interesting increase in FE based on anion addition. These results show anion addition to electrocatalysis reaction mixtures add an additional parameter to increase both rate and selectivity of catalysis with one example improving from 19 % FE to 91 % FE for CO production.