Electrochemical CO2 Reduction in a Continuous Non-Aqueous Flow Cell with [Ni(cyclam)]2.,Inorganic Chemistry

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Electrochemical CO2 Reduction in a Continuous Non-Aqueous Flow Cell with [Ni(cyclam)]2.
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-01-14 , DOI: 10.1021/acs.inorgchem.9b03171
Changcheng Jiang ₁ , Asa W Nichols ₁ , John F Walzer ₂ , Charles W Machan ₁

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A significant number of molecular catalysts have been developed for electrochemical CO2 reduction with high efficiency and selectivity; however, testing of these electrocatalysts in an application-ready system is lacking. Here, we present an example of a nonaqueous flow cell electrolyzer with [Ni(cyclam)]2+ as the homogeneous electrocatalyst for CO2 reduction. Using ferrocene as a sacrificial electron donor and ammonium salts as both electrolyte and proton donor, efficient catalytic CO2 reduction is achieved. The nonaqueous design shows high selectivity for the reduction of CO2 to CO (>80%) and achieves high current densities with a graphite felt working electrode (up to 50 mA·cm-2 with 0.5 M proton donor in MeCN solution), producing >40 mL·h-1 of CO. The choice of a molecular electrocatalyst, solvent, and proton donor are the key factors for achieving high activity with an efficient flow electrolyzer and the eventual development of a viable continuous process.

中文翻译：

[Ni（cyclam）] 2在连续非水流通池中电化学还原CO2。

已经开发出大量的分子催化剂以高效率和选择性地电化学还原CO 2。但是，缺乏在可立即投入使用的系统中测试这些电催化剂的能力。在此，我们以[Ni（cyclam）] 2+为均相电催化剂还原CO2的非水流通池电解池为例。使用二茂铁作为牺牲电子供体，同时使用铵盐作为电解质和质子供体，可实现有效的催化CO2还原。非水设计显示了将CO2还原为CO（> 80％）的高选择性，并使用石墨毡工作电极（在MeCN溶液中具有0.5 M质子供体的最大50 mA·cm-2的电流）实现了高电流密度，从而产生了> 40 mL·h-1的CO。选择分子电催化剂，溶剂，

更新日期：2020-01-15

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