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Angew Chem Int Ed Engl. 2015 Sep 07;54(37):10752-7. doi: 10.1002/anie.201504376. Epub 2015 Jul 23.

Coupling Mo2 C with Nitrogen-Rich Nanocarbon Leads to Efficient Hydrogen-Evolution Electrocatalytic Sites.

Angewandte Chemie (International ed. in English)

Yipu Liu, Guangtao Yu, Guo-Dong Li, Yuanhui Sun, Tewodros Asefa, Wei Chen, Xiaoxin Zou

Affiliations

  1. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, International Joint Research Laboratory of Nano-Micro Architecture Chemistry, College of Chemistry, Jilin University, Changchun 130012 (P.R. China).
  2. Institute of Theoretical Chemistry, International Joint Research Laboratory of Nano-Micro Architecture Chemistry, Jilin University, Changchun 130023 (P.R. China).
  3. Department of Chemistry and Chemical Biology & Department of Chemical and Biochemical Engineering, Rutgers, The State University of New Jersey, Piscataway, NJ 08854 (USA). [email protected].
  4. Institute of Theoretical Chemistry, International Joint Research Laboratory of Nano-Micro Architecture Chemistry, Jilin University, Changchun 130023 (P.R. China). [email protected].
  5. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, International Joint Research Laboratory of Nano-Micro Architecture Chemistry, College of Chemistry, Jilin University, Changchun 130012 (P.R. China). [email protected].

PMID: 26212796 DOI: 10.1002/anie.201504376

Abstract

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 Mo2 C@NC that is composed of ultrasmall molybdenum carbide (Mo2 C) nanoparticles embedded within nitrogen-rich carbon (NC) nanolayers. The Mo2 C@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 Mo2 C 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.

© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Keywords: catalytically active site; composite material; electrocatalysis; molybdenum carbide; water splitting

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