Tang Yongan, Lin Lu, Kumar Anil, Guo Min, Sevilla Michael, Zeng Xiangqun
Department of Chemistry, Oakland University, Rochester, Michigan 48309, United States.
J Phys Chem C Nanomater Interfaces. 2017 Mar 9;121(9):5161-5167. doi: 10.1021/acs.jpcc.7b00335. Epub 2017 Feb 13.
Hydrogen electrooxidation via a "hydrogen abstraction" mechanism in an aprotic ionic liquid 1-butyl-1-methylpyrrolidinium bis-(trifluoromethylsulfonyl) [Bmpy][NTf] under anaerobic conditions was investigated using cyclic voltammetry and density functional theory (DFT). It is found that a platinum bound NTf radical (NTf) formed by the oxidation of NTf at anodic potential can catalyze the oxidation of hydrogen and enhance its reaction rate. Both experimental and theoretical studies (DFT) have supported a mechanism involving a NTf radical intermediate that catalyzes the hydrogen redox processes.
采用循环伏安法和密度泛函理论（DFT），研究了在厌氧条件下，质子惰性离子液体1-丁基-1-甲基吡咯烷双（三氟甲基磺酰）亚胺（[Bmpy][NTf₂]）中通过“氢提取”机制进行的氢电氧化反应。研究发现，在阳极电位下，通过NTf₂氧化形成的铂结合NTf自由基（NTf•）可以催化氢的氧化并提高其反应速率。实验和理论研究（DFT）均支持涉及NTf自由基中间体催化氢氧化还原过程的机制。
