Coupling Mo2C with Nitrogen-Rich Nanocarbon Leads to Efficient Hydrogen-Evolution Electrocatalytic Sites

• Published in: Angewandte Chemie International Edition Vol. 54; no. 37; pp. 10752 - 10757
• Main Authors: Liu, Yipu, Yu, Guangtao, Li, Guo-Dong, Sun, Yuanhui, Asefa, Tewodros, Chen, Wei, Zou, Xiaoxin
• Format: Journal Article
• Language: English
• Published: Weinheim WILEY-VCH Verlag 07.09.2015; WILEY‐VCH Verlag; Wiley Subscription Services, Inc
• Edition: International ed. in English
• Subjects: catalytically active site; composite material; electrocatalysis; Hydrogen; Molybdenum; molybdenum carbide; Nitrogen; water splitting
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.201504376

In our efforts to obtain electrocatalysts with improved activity for water splitting, meticulous design and synthesis of the active sites of the electrocatalysts and deciphering how exactly they catalyze the reaction are vitally necessary. Herein, we report a one‐step facile synthesis of a novel precious‐metal‐free hydrogen‐evolution nanoelectrocatalyst, dubbed Mo2C@NC that is composed of ultrasmall molybdenum carbide (Mo2C) nanoparticles embedded within nitrogen‐rich carbon (NC) nanolayers. The Mo2C@NC hybrid nanoelectrocatalyst shows remarkable catalytic activity, has great durability, and gives about 100 % Faradaic yield toward the hydrogen‐evolution reaction (HER) over a wide pH range (pH 0–14). Theoretical calculations show that the Mo2C and N dopants in the material synergistically co‐activate adjacent C atoms on the carbon nanolayers, creating superactive nonmetallic catalytic sites for HER that are more active than those in the constituents. Hybrid catalyst: An efficient hybrid hydrogen‐evolution electrocatalyst containing molybdenum carbide nanoparticles embedded in nitrogen‐rich carbon nanolayers has been synthesized in one‐step from inexpensive precursors. The synergistic effect between Mo2C and N dopants was found to yield very active nonmetallic HER catalytic sites on the carbon nanolayers.