Title: Phase Modulation of (1T‐2H)‐MoSe2/TiC‐C Shell/Core Arrays via Nitrogen Doping for Highly Efficient Hydrogen Evolution Reaction

Abstract

Abstract Tailoring molybdenum selenide electrocatalysts with tunable phase and morphology is of great importance for advancement of hydrogen evolution reaction (HER). In this work, phase‐ and morphology‐modulated N‐doped MoSe ₂ /TiC‐C shell/core arrays through a facile hydrothermal and postannealing treatment strategy are reported. Highly conductive TiC‐C nanorod arrays serve as the backbone for MoSe ₂ nanosheets to form high‐quality MoSe ₂ /TiC‐C shell/core arrays. Impressively, continuous phase modulation of MoSe ₂ is realized on the MoSe ₂ /TiC‐C arrays. Except for the pure 1T‐MoSe ₂ and 2H‐MoSe ₂ , mixed (1T‐2H)‐MoSe ₂ nanosheets are achieved in the N‐MoSe ₂ by N doping and demonstrated by spherical aberration electron microscope. Plausible mechanism of phase transformation and different doping sites of N atom are proposed via theoretical calculation. The much smaller energy barrier, longer HSe bond length, and diminished bandgap endow N‐MoSe ₂ /TiC‐C arrays with substantially superior HER performance compared to 1T and 2H phase counterparts. Impressively, the designed N‐MoSe ₂ /TiC‐C arrays exhibit a low overpotential of 137 mV at a large current density of 100 mA cm ⁻² , and a small Tafel slope of 32 mV dec ⁻¹ . Our results pave the way to unravel the enhancementmore » mechanism of HER on 2D transition metal dichalcogenides by N doping.« less

Authors:

Deng, Shengjue ^[1]; Yang, Fan ^[2]; Zhang, Qinghua ^[3]; Zhong, Yu ^[1]; Zeng, Yinxiang ^[4]; Lin, Shiwei ^[2]; Wang, Xiuli ^[1]; Lu, Xihong ^[4]; Wang, Cai‐Zhuang ^[5]; Gu, Lin ^[3]; Xia, Xinhui  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-5976-5337"

Tu, Jiangping ^[1]

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+ Show Author Affiliations

1. State Key Laboratory of Silicon Materials Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province and Department of Materials Science and Engineering Zhejiang University Hangzhou 310027 P. R. China
2. State Key Laboratory of Marine Resource Utilization in South China Sea Hainan University Haikou 570228 P. R. China
3. Institute of Physics Chinese Academy of Sciences Beijing 100190 China
4. MOE of the Key Laboratory of Bioinorganic and Synthetic Chemistry KLGHEI of Environment and Energy Chemistry School of Chemistry Sun Yat‐sen University Guangzhou 510275 China
5. Ames Laboratory U. S. Department of Energy and Department of Physics and Astronomy Iowa State University Ames IA 50011 USA

Publication Date:

Thu Jul 05 00:00:00 EDT 2018

Sponsoring Org.:

USDOE

OSTI Identifier:

1459052

Grant/Contract Number:  

DE‐AC02‐07CH11358

Resource Type:

Publisher's Accepted Manuscript

Journal Name:

Advanced Materials

Additional Journal Information:

Journal Name: Advanced Materials Journal Volume: 30 Journal Issue: 34; Journal ID: ISSN 0935-9648

Publisher:

Wiley Blackwell (John Wiley & Sons)

Country of Publication:

Germany

Language:

English