4.7 Article

NiS/MoS2 Mott-Schottky heterojunction-induced local charge redistribution for high-efficiency urea-assisted energy-saving hydrogen production

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 443, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136321

Keywords

Mott-Schottky electrocatalyst; Electronic structure engineering; Hydrogen evolution reaction; Urea oxidation reaction

Funding

  1. National Natural Science Foundation of China [21972068, 21875112, 22075290, 51806110]
  2. State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences [MPCS-2021-A-05]
  3. High-level Talents Project of Jinling Institute of Technology [jit-b-202164]

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By constructing NiS/MoS2 hetero-nanoflowers on a conductive carbon cloth substrate, a Mott-Schottky bifunctional electrocatalyst was formed, enabling efficient urea-assisted water electrolysis with reduced energy consumption.
Urea-assisted water electrolysis possesses the prospective prospect for high-efficiency hydrogen production by replacing oxygen evolution reaction (OER) with thermodynamically more favorable urea oxidation reaction (UOR). Modulating the electronic structure of electrocatalysts through constructing metal-semiconductor heteminterface represents an effective strategy to promote the electrochemical performances. Herein, we construct a Mott-Schottky bifunctional electrocatalyst by in-situ growth of NiS/MoS2 hetero-nanoflowers on the conductive carbon cloth (CC) substrate (abbreviated as NiS/MoS2@CC hereafter) for both hydrogen evolution reaction (HER) and urea oxidation reaction (UOR). Thanks to the Mott-Schottky effect, the self-driven charge transfer occurs across the NiS/MoS2 heterointerfaces, which results in the built-in electric field, the accelerated charge transfer rate, and the modified chemisorption free energies for reaction intermediates, ultimately expediting the dissociation of water and urea molecules. Consequently, the as-fabricated NiS/MoS2@CC electrode only requires an overpotential of 87 mV for hydrogen evolution reaction (HER) in 1.0 M KOH and a potential of 1.36 V for UOR in 1.0 M KOH solution with 0.5 M urea to attain a current density of 10 mA cm(-2), respectively. Moreover, when served as the free-standing anode and cathode simultaneously, the NiS/MoS2@CC-assembled urea electrolyzer requires a cell voltage of 1.46 V at 10 mA cm(-2), which is 200 mV smaller than that of the pure water splitting counterpart. This study may deepen the understanding of electronic modulation via Mott-Schottky establishment.

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