Chelating N‐Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry,Angewandte Chemie International Edition

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Chelating N‐Heterocyclic Carbene Ligands Enable Tuning of Electrocatalytic CO2 Reduction to Formate and Carbon Monoxide: Surface Organometallic Chemistry
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2018-03-23 , DOI: 10.1002/anie.201800367
Zhi Cao ₁ , Jeffrey S. Derrick _{1,

2} , Jun Xu ₃ , Rui Gao _{4,

5} , Ming Gong _{1,

2} , Eva M. Nichols _{1,

2} , Peter T. Smith _{1,

2} , Xingwu Liu _{4,

5} , Xiaodong Wen _{4,

5} , Christophe Copéret ₃ , Christopher J. Chang _{1,

2,

6}

Affiliation

Reported here is the chelate effect as a design principle for tuning heterogeneous catalysts for electrochemical CO₂ reduction. Palladium functionalized with a chelating tris‐N‐heterocyclic carbene (NHC) ligand (Pd‐timtmb^Me) exhibits a 32‐fold increase in activity for electrochemical reduction of CO₂ to C1 products with high Faradaic efficiency (FE_C1=86 %) compared to the parent unfunctionalized Pd foil (FE=23 %), and with sustained activity relative to a monodentate NHC‐ligated Pd electrode (Pd‐mimtmb^Me). The results highlight the contributions of the chelate effect for tailoring and maintaining reactivity at molecular‐materials interfaces enabled by surface organometallic chemistry.

中文翻译：

螯合的N-杂环碳配体可实现电催化CO2还原成甲酸酯和一氧化碳的调节：表面有机金属化学

此处报道的螯合效应作为调整多相催化剂以减少电化学CO ₂的设计原理。与螯合的Tris-N-杂环卡宾（NHC）配体（Pd-timtmb ^Me）官能化的钯在电化学法下将CO ₂还原为C1产品的活性提高了32倍，而法拉第效率较高（FE _C1 = 86％）到母体未官能化的Pd箔（FE = 23％），并且相对于单齿NHC连接的Pd电极（Pd-mimtmb ^Me）具有持续的活性。结果突出了螯合效应对通过表面有机金属化学实现的分子材料界面的剪裁和维持反应性的贡献。

更新日期：2018-03-23

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