期刊
ADVANCED FUNCTIONAL MATERIALS
卷 32, 期 14, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202109731
关键词
hydrogen evolution reaction; seawater splitting; sulfur vacancy
类别
资金
- National Key R&D Program of China [2019YFC1907602]
- National Natural Science Foundation of China [51572295, 21273285, 21003157]
- Australian Research Council (ARC) Future Fellowship [FT210100298]
- CSIRO Energy Centre
- Kick-Start Project
- Victorian Government's support through the provision of a grant from veski - Study Melbourne Research Partnerships (SMRP) project
Metal Ru and vacancy engineering are used to enhance the activity of NiCo2S4 electrocatalysts for both oxygen evolution and hydrogen evolution reactions. Decorated with Ru single atoms and nanoclusters, the electrocatalysts exhibit significantly improved OER and HER performance, outperforming most reported materials in overall water splitting. Bader charge analysis reveals the promotion of electron interactions, contributing to the enhanced electrochemical performance.
Metal Ru and vacancy engineering play an important role in oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). However, there are few reports targeted on electrocatalysts by simultaneously employing these two strategies. Herein, theoretical calculation firstly predicts that Ru and V-S can regulate the adsorption energy of OER/HER intermediates for NiCo2S4 electrocatalysts. Then, a facile solvothermal-photochemical strategy is utilized to synthesis series NiCo2S4 samples: through filling the solvothermal-created V-S in NiCo2S4-x with Ru single atoms (Ru-NiCo2S4-x) under ultraviolet irradiation as OER catalysts. Besides, Ru nanoclusters are introduced into NiCo2S4 without V-S (Ru-NiCo2S4) for HER. As a result, the OER exchange current density of NiCo2S4-x is prominently boosted after decoration of Ru single atom, which possesses an eminently low overpotential of 190 mV@50 mA cm(-2), while Ru-NiCo2S4 shows superior HER performance (32 mV@10 mA cm(-2)) compared with Ru-NiCo2S4-x, surpassing most reported electrocatalytic materials. Moreover, Ru-NiCo2S4-x//Ru-NiCo2S4 exhibits remarkable stability and catalytic performance in the overall water splitting, with a cell voltage value of 1.46 V at 10 mA cm(-2) in 1.0 m KOH. Bader charge analysis unravels the restricted-delocalized-restricted phenomenon between electrons promote the electron interactions, which in turn improves electrochemical performance.
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