Ruthenium atomically dispersed in carbon outperforms platinum toward hydrogen evolution in alkaline media

被引:537
作者
Lu, Bingzhang [1 ]
Guo, Lin [1 ,2 ]
Wu, Feng [1 ]
Peng, Yi [1 ]
Lu, Jia En [1 ]
Smart, Tyler J. [3 ]
Wang, Nan [4 ]
Finfrock, Y. Zou [5 ,6 ]
Morris, David [7 ]
Zhang, Peng [7 ]
Li, Ning [8 ,9 ]
Gao, Peng [8 ,9 ,10 ]
Ping, Yuan [1 ]
Chen, Shaowei [1 ,4 ]
机构
[1] Univ Calif Santa Cruz, Dept Chem & Biochem, 1156 High St, Santa Cruz, CA 95064 USA
[2] Chinese Acad Sci, Key Lab Photochem Convers & Optoelect Mat, Tech Inst Phys & Chem, Beijing 100190, Peoples R China
[3] Univ Calif Santa Cruz, Dept Phys, 1156 High St, Santa Cruz, CA 95064 USA
[4] South China Univ Technol, New Energy Res Inst, Sch Environm & Energy, Guangzhou Higher Educ Mega Ctr, Guangzhou 510006, Guangdong, Peoples R China
[5] Canadian Light Source Inc, Div Sci, 44 Innovat Blvd, Saskatoon, SK S7N 2V3, Canada
[6] Argonne Natl Lab, CLS APS, Sect 20, Adv Photon Source, 9700 Cass Ave, Lemont, IL 60439 USA
[7] Dalhousie Univ, Dept Chem, 6274 Coburg Rd, Halifax, NS B3H 4R2, Canada
[8] Peking Univ, Int Ctr Quantum Mat, Beijing 100871, Peoples R China
[9] Peking Univ, Electron Microscopy Lab, Sch Phys, Beijing 100871, Peoples R China
[10] Collaborat Innovat Ctr Quantum Matter, Beijing 100871, Peoples R China
基金
美国国家科学基金会;
关键词
HIGH-PERFORMANCE CATALYSTS; OXYGEN REDUCTION REACTION; DOPED CARBON; EFFICIENT; NANOPARTICLES; ELECTROCATALYST; NITROGEN; PH; DESIGN; ENERGY;
D O I
10.1038/s41467-019-08419-3
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Hydrogen evolution reaction is an important process in electrochemical energy technologies. Herein, ruthenium and nitrogen codoped carbon nanowires are prepared as effective hydrogen evolution catalysts. The catalytic performance is markedly better than that of commercial platinum catalyst, with an overpotential of only -12 mV to reach the current density of 10 mV cm(-2) in 1M KOH and -47 mV in 0.1M KOH. Comparisons with control experiments suggest that the remarkable activity is mainly ascribed to individual ruthenium atoms embedded within the carbon matrix, with minimal contributions from ruthenium nanoparticles. Consistent results are obtained in first-principles calculations, where RuCxNy moieties are found to show a much lower hydrogen binding energy than ruthenium nanoparticles, and a lower kinetic barrier for water dissociation than platinum. Among these, RuC2N2 stands out as the most active catalytic center, where both ruthenium and adjacent carbon atoms are the possible active sites.
引用
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页数:11
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