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Ultra-small Mo2C nanodots encapsulated in nitrogen-doped porous carbon for pH-universal hydrogen evolution: insights into the synergistic enhancement of HER activity by nitrogen doping and structural defects

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Abstract

Herein, ultra-small molybdenum carbide nanodots encapsulated in nitrogen-doped porous carbon (Mo2C/N-PC) were synthesized by a facile one-pot method. Ammonium molybdate and low-cost starch were used as precursors of Mo2C and C. Ammonium nitrate was selected as a nitrogen dopant, which played multiple roles in the reduction of MoC to Mo2C, nitrogen doping of carbon, and formation of a porous structure with abundant structural defects, thus avoiding the high-temperature reduction by H2/Ar. The optimized Mo2C/N-PC hybrid has a remarkable catalytic activity towards the HER over a wide pH range (0–14). Especially, under alkaline conditions, an overpotential as small as −100 mV vs. RHE could be achieved at 10 mA cm−2, comparable to that of the best Mo2C-based materials. The density functional theory (DFT) calculations revealed that a decreased Gibbs free energy for H* adsorption (ΔGH*) could be obtained by combining Mo2C with N-PC, proving the synergistic enhancement mechanism of nitrogen doping and structural defects. This material contains no noble metals and can be easily synthesized on a large scale; thus, it should have significant potential in hydrogen production.

Graphical abstract: Ultra-small Mo2C nanodots encapsulated in nitrogen-doped porous carbon for pH-universal hydrogen evolution: insights into the synergistic enhancement of HER activity by nitrogen doping and structural defects

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Publication details

The article was received on 19 Nov 2018, accepted on 29 Jan 2019 and first published on 29 Jan 2019


Article type: Paper
DOI: 10.1039/C8TA11098K
Citation: J. Mater. Chem. A, 2019, Advance Article

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    Ultra-small Mo2C nanodots encapsulated in nitrogen-doped porous carbon for pH-universal hydrogen evolution: insights into the synergistic enhancement of HER activity by nitrogen doping and structural defects

    W. Han, L. Chen, B. Ma, J. Wang, W. Song, X. Fan, Y. Li, F. Zhang and W. Peng, J. Mater. Chem. A, 2019, Advance Article , DOI: 10.1039/C8TA11098K

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