Abstract

Hydrogen production through water splitting has been considered as a green, pure and high-efficient technique. As an important half-reaction involved, hydrogen evolution reaction is a complex electrochemical process involving liquid-solid-gas three-phase interface behaviour. Therefore, new concepts and strategies of material design are needed to smooth each pivotal step. Here we report a multiscale structural and electronic control of molybdenum disulfide foam to synergistically promote the hydrogen evolution process. The optimized three-dimensional molybdenum disulfide foam with uniform mesopores, vertically aligned two-dimensional layers and cobalt atoms doping demonstrated a high hydrogen evolution activity and stability. In addition, density functional theory calculations indicate that molybdenum disulfide with moderate cobalt doping content possesses the optimal activity. This study demonstrates the validity of multiscale control in molybdenum disulfide via overall consideration of the mass transport, and the accessibility, quantity and capability of active sites towards electrocatalytic hydrogen evolution, which may also be extended to other energy-related processes.

Highlights

  • Hydrogen production through water splitting has been considered as a green, pure and highefficient technique

  • Unlike the flexibility of carbon atoms skeleton in graphene and organic small molecules in polymers, MoS2 with single-crystal layer composed of three molecular layers (S–Mo–S) appears much more inflexible, which leads to such engineering still remaining a great challenge

  • We present a multiscale structural and electronic control of MoS2 foam for highly efficient hydrogen evolution reaction (HER) process: (i) the macro-scale: a uniform mesoporous MoS2 foam facilitate the transport of H3O þ and H2, and increases the accessibility of MoS2 surface; (ii) the nanoscale: oriented vertical growth of MoS2 nanosheets around the mesopores increase the number of edges as the active sites; (iii) the atomic-scale: further chemical doping with transition metal Co atoms into the mPF-MoS2 framework enhance the intrinsic HER activity

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Summary

Introduction

Hydrogen production through water splitting has been considered as a green, pure and highefficient technique. Owing to its natural abundance, low cost and good catalytic performance, recently MoS2 has become a representative non-precious material for electrocatalytic hydrogen evolution reaction (HER) of water splitting[14,15,16,17,18,19,20,21] Such liquid-to-gas electrochemical conversion, with a complex reaction process at the interface of liquid (H þ ), solid (catalyst) and gas (H2), require a multiscale structural and electronic control of MoS2 to make each involved reaction step to proceed smoothly. The strategies, introduced in the present work, may open new opportunities for the rational design of MoS2 through a multiscale structural and electronic control to strengthen the electrocatalytic HER and other energyrelated process, and possibly for the structural control of other 2D materials

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