Evolution of bismuth-based metal–organic frameworks for efficient electroreduction of CO2,Journal of Materials Chemistry A

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Evolution of bismuth-based metal–organic frameworks for efficient electroreduction of CO2
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2022-08-18 , DOI: 10.1039/d2ta04485d
Lili Li ₁ , Xinchen Kang _{1,

2} , Meng He ₁ , Alena Sheveleva _{1,

3} , Kui Hu ₁ , Shaojun Xu _{4,

5} , Yiqi Zhou _{6,

7} , Jin Chen ₁ , Sergei Sapchenko ₁ , George Whitehead ₁ , Iñigo J Vitorica-Yrezabal ₁ , Laura Lopez-Odriozola ₁ , Louise S Natrajan ₁ , Eric J L McInnes _{1,

3} , Martin Schröder ₁ , Sihai Yang ₁ , Floriana Tuna _{1,

3}

Affiliation

Understanding the structural and chemical changes that reactive metal–organic frameworks (MOFs) undergo is crucial for the development of new efficient catalysts for electrochemical reduction of CO₂. Here, we describe three Bi(III) materials, MFM-220, MFM-221 and MFM-222, which are constructed from the same ligand (biphenyl-3,3′,5,5′-tetracarboxylic acid) but which show distinct porosity with solvent-accessible voids of 49.6%, 33.6% and 0%, respectively. We report the first study of the impact of porosity of MOFs on their evolution as electrocatalysts. A Faradaic efficiency of 90.4% at −1.1 V vs. RHE (reversible hydrogen electrode) is observed for formate production over an electrode decorated with MFM-220-p, formed from MFM-220 on application of an external potential in the presence of 0.1 M KHCO₃ electrolyte. In situ electron paramagnetic resonance spectroscopy confirms the presence of ·COOH radicals as a reaction intermediate, with an observed stable and consistent Faradaic efficiency and current density for production of formate by electrolysis over 5 h. This study emphasises the significant role of porosity of MOFs as they react and evolve during electroreduction of CO₂ to generate value-added chemicals.

中文翻译：

用于有效电还原二氧化碳的铋基金属有机框架的演变

了解活性金属有机框架（MOF）所经历的结构和化学变化对于开发用于电化学还原CO ₂的新型高效催化剂至关重要。在这里，我们描述了三种 Bi( III ) 材料，MFM-220、MFM-221 和 MFM-222，它们由相同的配体（联苯-3,3',5,5'-四羧酸）构建，但表现出不同的特性溶剂可及的孔隙率分别为 49.6%、33.6% 和 0%。我们首次研究了 MOF 的孔隙率对其作为电催化剂的演变的影响。在用 MFM-220-p 装饰的电极（由 MFM-220 在存在 0.1 的外部电势的情况下形成）上观察到在 -1.1 V vs. RHE（可逆氢电极）下产生甲酸盐的法拉第效率为 90.4% M KHCO ₃电解质。原位电子顺磁共振波谱证实了·COOH自由基作为反应中间体的存在，并观察到通过电解5小时以上稳定一致的法拉第效率和电流密度。这项研究强调了 MOF 的孔隙率在 CO ₂电还原过程中发生反应和演化以产生增值化学品时的重要作用。

更新日期：2022-08-18

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