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CO2 to CO: Photo‐ and Electrocatalytic Conversion Based on Re(I) Bis‐Arene Frameworks: Synergisms Between Catalytic Subunits
Helvetica Chimica Acta ( IF 1.5 ) Pub Date : 2020-09-24 , DOI: 10.1002/hlca.202000147 Daniel Hernández‐Valdés 1 , Ricardo Fernández‐Terán 1 , Benjamin Probst 1 , Bernhard Spingler 1 , Roger Alberto 1
Helvetica Chimica Acta ( IF 1.5 ) Pub Date : 2020-09-24 , DOI: 10.1002/hlca.202000147 Daniel Hernández‐Valdés 1 , Ricardo Fernández‐Terán 1 , Benjamin Probst 1 , Bernhard Spingler 1 , Roger Alberto 1
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Reduction of CO2 to CO and H2O is a two electron/two proton process. For this process, multinuclear complexes offer advantages by concentrating reduction equivalents more efficiently than mononuclear systems. We present novel complexes with [Re(η6‐C6H6)2]+ as scaffold conjugated to one or two catalytically active [Ru(dmbpy)(CO)2Cl2] subunits (dmbpy=5,5′‐dimethyl‐2,2′‐bipyridine). The [Re(η6‐C6H6)2]+ scaffold was chosen due to its very high photo‐ and chemical stability, as well as the multiple degrees of freedom it offers for any conjugated functionalities. High efficiency and selectivity for the reduction of CO2 to CO (over H2 or HCOOH) is reported. TONs and TOFs were found to be comparable or higher than for the catalyst subunit without the rhenium framework. Cooperativity in photo‐ and electrocatalysis is observed for the complex comprising two catalytic subunits. The synergistic communication between the two catalytic subunits is responsible for the observed enhancement in both photo‐ and electrocatalytic performance. Confirmation of electronic communication between the two [Ru(dmbpy)(CO)2Cl2] subunits as well as the elucidation of a possible mechanism was supported by electrochemistry, IR‐spectroelectrochemistry and DFT studies.
中文翻译：
CO2到CO：基于Re（I）Bis-Arene框架的光催化和电催化转化：催化亚基之间的协同作用
CO 2还原为CO和H 2 O是两个电子/两个质子的过程。对于此过程，多核配合物通过比单核系统更有效地浓缩还原当量来提供优势。我们呈现与新的配合物[回复（η 6 -C 6 H ^ 6）2 ] +为支架缀合至一个或两个催化活性的[Ru（dmbpy）（CO）2氯2亚基（dmbpy = 5,5'-二甲基-2,2'-联吡啶）。的[再（η 6 -C 6 H ^ 6）2 ] +之所以选择脚手架，是因为其非常高的光化学稳定性，以及其为任何共轭官能团提供的多重自由度。据报道，用于将CO 2还原为CO（在H 2或HCOOH之上）的高效性和选择性。发现TON和TOF与没有without骨架的催化剂亚单元相当或更高。对于包含两个催化亚基的配合物，在光催化和电催化方面具有协同作用。两个催化亚基之间的协同通讯负责观察到的光催化和电催化性能的增强。确认两个[Ru（dmbpy）（CO）2 Cl 2之间的电子通信]亚基以及对可能机制的阐明得到了电化学，红外光谱电化学和DFT研究的支持。
更新日期：2020-10-30
中文翻译：
CO2到CO：基于Re（I）Bis-Arene框架的光催化和电催化转化：催化亚基之间的协同作用
CO 2还原为CO和H 2 O是两个电子/两个质子的过程。对于此过程，多核配合物通过比单核系统更有效地浓缩还原当量来提供优势。我们呈现与新的配合物[回复（η 6 -C 6 H ^ 6）2 ] +为支架缀合至一个或两个催化活性的[Ru（dmbpy）（CO）2氯2亚基（dmbpy = 5,5'-二甲基-2,2'-联吡啶）。的[再（η 6 -C 6 H ^ 6）2 ] +之所以选择脚手架，是因为其非常高的光化学稳定性，以及其为任何共轭官能团提供的多重自由度。据报道，用于将CO 2还原为CO（在H 2或HCOOH之上）的高效性和选择性。发现TON和TOF与没有without骨架的催化剂亚单元相当或更高。对于包含两个催化亚基的配合物，在光催化和电催化方面具有协同作用。两个催化亚基之间的协同通讯负责观察到的光催化和电催化性能的增强。确认两个[Ru（dmbpy）（CO）2 Cl 2之间的电子通信]亚基以及对可能机制的阐明得到了电化学，红外光谱电化学和DFT研究的支持。
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