Boosting electrosynthesis of ammonia on surface-engineered MXene Ti3C2

被引:111
作者
Xia, Jiexiang [1 ,2 ]
Yang, Shi-Ze [3 ]
Wang, Bin [1 ]
Wu, Peiwen [1 ,2 ]
Popovs, Ilja [2 ]
Li, Huaming [1 ]
Irle, Stephan [2 ]
Dai, Sheng [2 ]
Zhu, Huiyuan [2 ,4 ]
机构
[1] Jiangsu Univ, Sch Chem & Chem Engn, Inst Energy Res, 301 Xuefu Rd, Zhenjiang 212013, Jiangsu, Peoples R China
[2] Oak Ridge Natl Lab, Chem Sci Div, POB 2009, Oak Ridge, TN 37830 USA
[3] Oak Ridge Natl Lab, Mat Sci & Technol Div, POB 2009, Oak Ridge, TN 37830 USA
[4] Virginia Polytech Inst & State Univ, Dept Chem Engn, Blacksburg, VA 24061 USA
关键词
Nitrogen fixation; MXene; Electrocatalysis; Surface engineering; Ti3C2; ATMOSPHERIC-PRESSURE; HYDROGEN EVOLUTION; NITROGEN; CARBON; NANOCRYSTALS; TEMPERATURE; NANOSHEETS; REDUCTION; MECHANISM; OXIDATION;
D O I
10.1016/j.nanoen.2020.104681
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Seeking a breakthrough in the development of efficient nitrogen fixation catalysts has become the frontier of energy and chemical conversion schemes. Here, we report that the MXene Ti3C2 can serve as a promising catalyst for the electrochemical N-2 reduction reaction (NRR) under ambient conditions. The electrocatalytic performance of Ti3C2 can be further optimized through surface engineering. Specifically, Ti3C2 with the increased surface hydroxyl moieties demonstrates enhanced production of NH3 with a yield rate of 1.71 mu g h(-1) cm(-2), a Faradaic efficiency of 7.01% at 0.2 V vs. RHE at 20 degrees C and an even higher yield rate of 12.46 mu g h(-1) cm(-2) together with a Faradaic efficiency of 9.03% at 0.2 V vs. RHE at 60 degrees C. The detailed electrochemical analysis suggests that the surface hydroxyl modification can effectively facilitate the electron transfer, surface adsorption and activation of dinitrogen. Our work sheds light on the development of efficient NRR catalysts based on earth-abundant elements.
引用
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页数:7
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