Immobilization of a Molecular Re Complex on MOF‐derived Hierarchical Porous Carbon for CO2 Electroreduction in Water/Ionic Liquid Electrolyte,ChemSusChem

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Immobilization of a Molecular Re Complex on MOF‐derived Hierarchical Porous Carbon for CO2 Electroreduction in Water/Ionic Liquid Electrolyte
ChemSusChem ( IF 7.5 ) Pub Date : 2020-09-25 , DOI: 10.1002/cssc.202002014
Domenico Grammatico _{1,

2} , Huan Ngoc Tran ₃ , Yun Li ₃ , Silvia Pugliese _{1,

3} , Laurent Billon ₂ , Bao‐Lian Su ₁ , Marc Fontecave ₃

Affiliation

The development of molecular catalysts for CO₂ electroreduction within electrolyzers requests their immobilization on the electrodes. While a variety of methods have been explored for the heterogenization of homogeneous complexes, a novel approach using a hierarchical porous carbon material, derived from a metal–organic framework, is reported as a support for the well‐known molecular catalyst [Re(bpy)(CO)₃Cl] (bpy=2,2’‐bipyridine). This cathodic hybrid material, named Re@HPC (HPC=hierarchical porous carbon), has been tested for CO₂ electroreduction using a mixture of an ionic liquid (1‐ethyl‐3‐methylimidazolium tetrafluoroborate, EMIM) and water as the electrolyte. Interestingly, it catalyzes the conversion of CO₂ into a mixture of carbon monoxide and formic acid, with a selectivity that depends on the applied potential. The present study thus reveals that Re@HPC is a remarkable catalyst, enjoying excellent activity (turnover numbers for CO₂ reduction of 7835 after 2 h at −1.95 V vs. Fc/Fc⁺ with a current density of 6 mA cm⁻²) and good stability. These results emphasize the advantages of integrating molecular catalysts onto such porous carbon materials for developing novel, stable and efficient, catalysts for CO₂ reduction.

中文翻译：

MOF衍生的多孔碳上分子复合物的固定化，用于水/离子液体电解质中CO2的电还原

电解槽内用于CO ₂电解还原的分子催化剂的开发要求将其固定在电极上。尽管已经探索了多种方法来均相复合物的异质化，但据报道，一种使用由金属-有机骨架衍生的分级多孔碳材料的新方法可为著名的分子催化剂提供支持[Re（bpy）（CO）₃ Cl]（bpy = 2,2'-联吡啶）。这种阴极杂化材料名为Re @ HPC（HPC =多级多孔碳），已通过使用离子液体（1-乙基-3-甲基咪唑四氟硼酸盐，EMIM）和水作为电解质的混合物进行了CO ₂电还原测试。有趣的是，它催化CO ₂的转化形成一氧化碳和甲酸的混合物，其选择性取决于所施加的电势。因此，本研究表明，Re @ HPC是一种出色的催化剂，具有出色的活性（在-1.95 V下2小时后，相对于Fc / Fc ⁺电流密度为6 mA cm ^-2，CO ₂还原数为7835 ）稳定性好这些结果强调了将分子催化剂整合到这种多孔碳材料上以开发新颖，稳定和有效的CO ₂还原催化剂的优点。

更新日期：2020-09-25

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