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Atomic Sulfur Filling Oxygen Vacancies Optimizes H Absorption and Boosts the Hydrogen Evolution Reaction in Alkaline Media
Author(s) -
Jin Jing,
Yin Jie,
Liu Hongbo,
Huang Bolong,
Hu Yang,
Zhang Hong,
Sun Mingzi,
Peng Yong,
Xi Pinxian,
Yan ChunHua
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202104055
Subject(s) - overpotential , electrocatalyst , chemistry , hydrogen , dissociation (chemistry) , raman spectroscopy , inorganic chemistry , oxygen , sulfur , absorption spectroscopy , spinel , materials science , electrochemistry , electrode , physics , optics , metallurgy , quantum mechanics , organic chemistry
The hydrogen evolution reaction (HER) usually has sluggish kinetics in alkaline solution due to the difficulty in forming binding protons. Herein we report an electrocatalyst in which sulfur atoms are doping in the oxygen vacancies (V O ) of inverse spinel NiFe 2 O 4 (S‐NiFe 2 O 4 ) to create active sites with enhanced electron transfer capability. This electrocatalyst has an ultralow overpotential of 61 mV at the current density of 10 mA cm −2 and long‐term stability of 60 h at 1.0 Acm −2 in 1.0 M KOH media. In situ Raman spectroscopy revealed that S sites adsorb hydrogen adatom (H*) and in situ form S‐H*, which favor the production of hydrogen and boosts HER in alkaline solution. DFT calculations further verified that S introduction lowered the energy barrier of H 2 O dissociation. Both experimental and theoretical investigations confirmed S atoms are active sites of the S‐NiFe 2 O 4 .