Single Atoms of Iron on MoS2Nanosheets for N2Electroreduction into Ammonia

被引:181
作者
Su, Hongyang [1 ]
Chen, Lanlan [2 ,3 ]
Chen, Yizhen [1 ]
Si, Rui [4 ]
Wu, Yuting [1 ]
Wu, Xiaonan [1 ]
Geng, Zhigang [1 ]
Zhang, Wenhua [2 ,3 ]
Zeng, Jie [1 ]
机构
[1] Univ Sci & Technol China, Anhui Higher Educ Inst,Dept Chem Phys, Key Lab Surface & Interface Chem & Energy Catalys, Hefei Natl Lab Phys Sci Microscale,CAS Key Lab St, Hefei 230026, Anhui, Peoples R China
[2] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, CAS Key Lab Mat Energy Convers, Hefei 230026, Anhui, Peoples R China
[3] Univ Sci & Technol China, Synerget Innovat Ctr Quantum Informat & Quantum P, Hefei 230026, Anhui, Peoples R China
[4] Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai 201210, Peoples R China
关键词
ammonia; electrochemistry; heterogeneous catalysis; iron; nanostructures; ACTIVE EDGE SITES; NITROGEN-FIXATION; REDUCTION; MOS2; EVOLUTION; CO2;
D O I
10.1002/anie.202009217
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Efforts have been devoted to achieving a highly efficient artificial synthesis of ammonia (NH3). Reported herein is a novel Fe-MoS(2)catalyst with Fe atomically dispersed onto MoS(2)nanosheets, imitating natural nitrogenase, to boost N(2)electroreduction into NH(3)at room temperature. The Fe-MoS(2)nanosheets exhibited a faradic efficiency of 18.8 % with a yield rate of 8.63 mu gNH3 mg(cat.)(-1) h(-1)for NH(3)at -0.3 V versus the reversible hydrogen electrode. The mechanism study revealed that the electroreduction of N(2)was promoted and the competing hydrogen evolution reaction was suppressed by decorating the edge sites of S in MoS(2)with the atomically dispersed Fe, resulting in high catalytic performance for the electroreduction of N(2)into NH3. This work provides new ideas for the design of catalysts for N(2)electroreduction and strengthens the understanding about N(2)activation over Mo-based catalysts.
引用
收藏
页码:20411 / 20416
页数:6
相关论文
共 46 条
[1]   A rigorous electrochemical ammonia synthesis protocol with quantitative isotope measurements [J].
Andersen, Suzanne Z. ;
Colic, Viktor ;
Yang, Sungeun ;
Schwalbe, Jay A. ;
Nielander, Adam C. ;
McEnaney, Joshua M. ;
Enemark-Rasmussen, Kasper ;
Baker, Jon G. ;
Singh, Aayush R. ;
Rohr, Brian A. ;
Statt, Michael J. ;
Blair, Sarah J. ;
Mezzavilla, Stefano ;
Kibsgaard, Jakob ;
Vesborg, Peter C. K. ;
Cargnello, Matteo ;
Bent, Stacey F. ;
Jaramillo, Thomas F. ;
Stephens, Ifan E. L. ;
Norskov, Jens K. ;
Chorkendorff, Ib .
NATURE, 2019, 570 (7762) :504-+
[2]   In situ XANES and EXAFS Analysis of Redox Active Fe Center Ionic Liquids [J].
Apblett, Christopher A. ;
Stewart, David M. ;
Fryer, Robert T. ;
Sell, Julia C. ;
Harry, Pratt D., III ;
Anderson, Travis M. ;
Meulenberg, Robert W. .
ELECTROCHIMICA ACTA, 2015, 185 :156-161
[3]   Electrochemical Reduction of N2 under Ambient Conditions for Artificial N2 Fixation and Renewable Energy Storage Using N2/NH3 Cycle [J].
Bao, Di ;
Zhang, Qi ;
Meng, Fan-Lu ;
Zhong, Hai-Xia ;
Shi, Miao-Miao ;
Zhang, Yu ;
Yan, Jun-Min ;
Jiang, Qing ;
Zhang, Xin-Bo .
ADVANCED MATERIALS, 2017, 29 (03)
[4]   Doping strain induced bi-Ti3+ pairs for efficient N2 activation and electrocatalytic fixation [J].
Cao, Na ;
Chen, Zheng ;
Zang, Ketao ;
Xu, Jie ;
Zhong, Jun ;
Luo, Jun ;
Xu, Xin ;
Zheng, Gengfeng .
NATURE COMMUNICATIONS, 2019, 10 (1)
[5]   Molybdenum Carbide Nanodots Enable Efficient Electrocatalytic Nitrogen Fixation under Ambient Conditions [J].
Cheng, Hui ;
Ding, Liang-Xin ;
Chen, Gao-Feng ;
Zhang, Lili ;
Xue, Jian ;
Wang, Haihui .
ADVANCED MATERIALS, 2018, 30 (46)
[6]  
deB Darwent B., 1970, NBS, V31
[7]   The nitrogen industry. [J].
Desch, CH .
NATURE, 1922, 110 :670-671
[8]   How a century of ammonia synthesis changed the world [J].
Erisman, Jan Willem ;
Sutton, Mark A. ;
Galloway, James ;
Klimont, Zbigniew ;
Winiwarter, Wilfried .
NATURE GEOSCIENCE, 2008, 1 (10) :636-639
[9]   Achieving a Record-High Yield Rate of 120.9 μgNH3 mgcat-1. h-1 for N2 Electrochemical Reduction over Ru Single-Atom Catalysts [J].
Geng, Zhigang ;
Liu, Yan ;
Kong, Xiangdong ;
Li, Pai ;
Li, Kan ;
Liu, Zhongyu ;
Du, Junjie ;
Shu, Miao ;
Si, Rui ;
Zeng, Jie .
ADVANCED MATERIALS, 2018, 30 (40)
[10]   Boosting Electrochemical Nitrogen Reduction Performance over Binuclear Mo Atoms on N-Doped Nanoporous Graphene: A Theoretical Investigation [J].
Guo, Ruijie ;
Hu, Min ;
Zhang, Weiqing ;
He, Jia .
MOLECULES, 2019, 24 (09)