An Investigation of Electrocatalytic CO2 Reduction Using a Manganese Tricarbonyl Biquinoline Complex
An Investigation of Electrocatalytic CO2 Reduction Using a Manganese Tricarbonyl Biquinoline Complex
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DOI：
10.3389/fchem.2019.00628
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发表时间：
2019-09-24
影响因子：
5.5
通讯作者：
Rochford, Jonathan
中科院分区：
文献类型：
--
作者：
McKinnon, Meaghan;Belkina, Veronika;Rochford, Jonathan
本研究的主题[fac-Mn（bqn）（CO）（3）（CH 3CN）]（+）（bqn = 2，2 '-联喹啉）特别令人感兴趣，因为bqn配体对络合物的基本氧化还原性质以及因此其关于CO2活化的相关催化性质表现出空间和电子影响。虽然不是用于CO2至CO转化的特别有效的催化剂，但是[fac-Mn（bqn）（CO）（3）]（-）活性催化剂的原位生成和活性测量允许更好地理解Mn中心处的配体设计。通过伏安法、红外光谱电化学、控制电位电解和计算分析，与相关的2，2 '-联吡啶（bpy）、1，10-邻菲咯啉（phen）和2，9-二甲基-1，10-邻菲咯啉（dmphen）配体进行直接比较，讨论了空间位阻和电子效应对Mn基CO2还原电催化剂亲核性的影响.
The subject of this study [fac-Mn(bqn)(CO)(3)(CH3CN)](+) (bqn = 2,2'-biquinoline), is of particular interest because the bqn ligand exhibits both steric and electronic influence over the fundamental redox properties of the complex and, consequently, its related catalytic properties with respect to the activation of CO2. While not a particularly efficient catalyst for CO2 to CO conversion, in-situ generation and activity measurements of the [fac-Mn(bqn)(CO)(3)](-) active catalyst allows for a better understanding of ligand design at the Mn center. By making direct comparisons to the related 2,2'-bipyridyl (bpy), 1, 10-phenanthroline (phen), and 2,9-dimethyl-1,10-phenanthroline (dmphen) ligands via a combination of voltammetry, infrared spectroelectrochemistry, controlled potential electrolysis and computational analysis, the role of steric vs. electronic influences on the nucleophilicity of Mn-based CO2 reduction electrocatalysts is discussed.