Highly Efficient and Stable Hydrogen Production in All pH Range by Two-Dimensional Structured Metal-Doped Tungsten Semicarbides

被引:48
作者
Ang, Edison H. [1 ,2 ]
Dinh, Khang N. [1 ,2 ]
Sun, Xiaoli [2 ,3 ]
Huang, Ying [2 ]
Yang, Jun [2 ,4 ]
Dong, Zhili [2 ]
Dong, Xiaochen [4 ]
Huang, Wei [4 ]
Wang, Zhiguo [3 ]
Zhang, Hua [2 ,5 ]
Yan, Qingyu [1 ,2 ]
机构
[1] Nanyang Technol Univ, Interdisciplinary Grad Sch, Energy Res Inst, Singapore 637553, Singapore
[2] Nanyang Technol Univ, Sch Mat Sci & Engn, Ctr Programmable Mat, Singapore 639798, Singapore
[3] Nanjing Tech Univ, Inst Adv Mat, Nanjing 210000, Peoples R China
[4] Univ Elect Sci & Technol China, Sch Phys Elect, Chengdu 610054, Peoples R China
[5] City Univ Hong Kong, Dept Chem, Kowloon, Hong Kong, Peoples R China
关键词
OXYGEN REDUCTION; NICKEL PHOSPHIDE; CARBIDE; ELECTROCATALYSTS; NANOPARTICLES; NANOSHEETS; W2C; NI; CO; STABILITY;
D O I
10.34133/2019/4029516
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
Transition-metal-doped tungsten semicarbide nanosheets (M-doped W2C NSs, M=Fe, Co, and Ni) have been synthesized through carburization of the mixture of tungsten trioxide, poly vinylpyrrolidone, and metal dopant. The nanosheets grow directly on the W mesh and have the lateral dimension of several hundreds of nm to a few ym with a thickness of few tens nm. It is demonstrated that the M-doped W2C NSs exhibit superior electrocatalytic activity for hydrogen evolution reaction (HER). Impressively, the Ni-doped W2C NSs (2 at% Ni) with the optimized HER activity show extremely low onset overpotentials of 4, 9, and 19 mV and modest Tafel slopes of 39, 51, and 87 mV dec(-1) in acidic (pH=0), neutral (pH 7.2), and basic (pH=14) solutions, respectively, which is close to the commercial Pt/C catalyst. Density functional theory (DFT) calculations also demonstrate that the Gibbs free energy for H adsorption of Ni-W2C is much closer to the optimal value Delta G(H*) = -0.073 eV as compared to -0.16 eV of W2C. Furthermore, nearly 100% Faradaic efficiency and long-term stability are obtained in those environments. This realization of highly tolerant metal semicarbide catalyst performing on par with commercial Pt/C in all range of pH offers a key step towards industrially electrochemical water splitting.
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页数:14
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