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Vertically aligned Ni/NiO nanocomposites with abundant oxygen deficient hetero-interfaces for enhanced overall water splitting

引用

Science China Chemistry 2022年第10期65卷 1885-1894页

作者： Hongxia Wang Meiyan Cui Gaoliang Fu Jiaye Zhang Xingyu Ding Irene Azaceta matthew bugnet Demie M.Kepaptsoglou Vlado K.Lazarov Victor Ade la Peña O’Shea Freddy E.Oropeza Kelvin H.L.Zhang State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Henan Provincial Key Laboratory of Nanocomposites and Applications Institute of Nanostructured Functional MaterialsHuanghe Science and Technology CollegeZhengzhou 450006China Department of Physics University of YorkHeslingtonYorkYO105DDUK SuperSTEM Laboratory SciTech Daresbury CampusDaresbury WA44ADUK School of Chemical and Process Engineering Univeristy of LeedsLeeds LS29JTUK Univ Lyon CNRSINSA LyonUCBLMATEISUMR 551069621 VilleurbanneFrance Photoactivated Processes Unit IMDEA Energy InstituteParque Tecnológico de MóstolesAvda.Ramón de la Sagra 328935 MóstolesMadridSpain

The design of heterostructured transition metal-based electrocatalysts with controlled composition and interfaces is key to increasing the efficiency of the water electrolysis and the elucidation of reaction *** this work,we report the synthesis of well-controlled vertically aligned Ni/NiO nanocomposites consisting of Ni nanoclusters embedded in NiO,which result in highly efficient electrocatalysts for overall water *** show that such a high catalytic efficiency toward both the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER)originates from a synergetic effect at Ni/NiO interfaces that significantly reduces the energy barrier for water dissociation,and favours the formation of reactive H*intermediates on the Ni side of the interface,and OH_(ads) on the NiO side of the interface.A study of water chemisorption based on near-ambient pressure photoelectron spectroscopy indicates that the abundant hetero-interfaces in Ni/NiO nanocomposite promote the dissociation of water with a three-fold increase in the surface concentration of OH_(ads) compared with pure *** functional theory calculations indicate that Ni/NiO interface leads to the reduction of the water dissociation energy barrier due to a high concentration of oxygen vacancies at NiO side of the interface,whereas the formation of highly active metallic Ni sites with an optimal value of Gibbs free energy of H*(ΔG_(H*)=−0.16 eV)owes to a favourable adjustment of the electron energetics at the interface,thus accelerating the overall electrochemical water splitting.

关键词： water splitting hydrogen evolution reaction electronic structure heterostructure vertically aligned nanocomposites

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