{"title":"Hydrogen Spillover Mechanism of Superaerophobic NiSe2-Ni5P4 Electrocatalyst to Promote Hydrogen Evolution in Saline Water","authors":"Jiahui Jiang, Guancheng Xu, Bingbing Gong, Jingjing Zhu, Weiwei Wang, Ting Zhao, Yuying Feng, Qihao Wu, Shuai Liu, Li Zhang","doi":"10.1002/adfm.202412685","DOIUrl":null,"url":null,"abstract":"The hydrogen spillover mechanism of metal-supported electrocatalyst can significantly improve HER activity. However, the rational design of binary heterojunction hydrogen spillover electrocatalysts remains a challenge. Here, a NiSe<sub>2</sub>-Ni<sub>5</sub>P<sub>4</sub> heterojunction electrocatalyst with superaerophobic structure is synthesized by using a simple substrate self-derived strategy. Experimental characterization and theoretical calculation reveal the hydrogen spillover mechanism of NiSe<sub>2</sub>-Ni<sub>5</sub>P<sub>4</sub> heterogeneous electrocatalyst. NiSe<sub>2</sub> and Ni<sub>5</sub>P<sub>4</sub> synergistically promote the adsorption/dissociation of H<sub>2</sub>O and the adsorption of H<sup>*</sup>, respectively. The smaller Δ<i>Φ</i> effectively reduced the electron density at the interface, weakening the proton adsorption at the interface and promoting the migration of H<sup>*</sup> from NiSe<sub>2</sub> to Ni<sub>5</sub>P<sub>4</sub>. The NiSe<sub>2</sub>-Ni<sub>5</sub>P<sub>4</sub> exhibits excellent HER activity in alkaline electrolyte, requiring only a potential of 65, 270 mV to achieve a current density of 10, 500 mA cm<sup>−2</sup>, respectively, and a stability of up to 200 h. Moreover, the design of NiSe<sub>2</sub>-Ni<sub>5</sub>P<sub>4</sub> with superaerophobic structure can reduce the deposition of impurity ions on the electrode surface and avoid Cl<sup>−</sup> corrosion of the electrode, which results in NiSe<sub>2</sub>-Ni<sub>5</sub>P<sub>4</sub> showing better HER activity and stability than commercial Pt/C in brackish water. This study deepens the understanding of hydrogen spillover mechanism of binary heterojunction electrocatalysts, broadens the application of hydrogen production in complex water quality.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":18.5000,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Functional Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adfm.202412685","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
The hydrogen spillover mechanism of metal-supported electrocatalyst can significantly improve HER activity. However, the rational design of binary heterojunction hydrogen spillover electrocatalysts remains a challenge. Here, a NiSe2-Ni5P4 heterojunction electrocatalyst with superaerophobic structure is synthesized by using a simple substrate self-derived strategy. Experimental characterization and theoretical calculation reveal the hydrogen spillover mechanism of NiSe2-Ni5P4 heterogeneous electrocatalyst. NiSe2 and Ni5P4 synergistically promote the adsorption/dissociation of H2O and the adsorption of H*, respectively. The smaller ΔΦ effectively reduced the electron density at the interface, weakening the proton adsorption at the interface and promoting the migration of H* from NiSe2 to Ni5P4. The NiSe2-Ni5P4 exhibits excellent HER activity in alkaline electrolyte, requiring only a potential of 65, 270 mV to achieve a current density of 10, 500 mA cm−2, respectively, and a stability of up to 200 h. Moreover, the design of NiSe2-Ni5P4 with superaerophobic structure can reduce the deposition of impurity ions on the electrode surface and avoid Cl− corrosion of the electrode, which results in NiSe2-Ni5P4 showing better HER activity and stability than commercial Pt/C in brackish water. This study deepens the understanding of hydrogen spillover mechanism of binary heterojunction electrocatalysts, broadens the application of hydrogen production in complex water quality.
期刊介绍:
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