物理化学学报2025，Vol.41Issue(7)：103-113,11.DOI:10.1016/j.actphy.2025.100081
具有富电子Ptδ-壳层的空心AgPt@Pt核壳催化剂:提升光催化H2O2生成选择性与活性
Hollow AgPt@Pt core-shell cocatalyst with electron-rich Ptδ-shell for boosting selectivity of photocatalytic H2O2 production for faceted BiVO4
摘要
Abstract
Platinum(Pt)is an excellent oxygen reduction cocatalyst with great potential for the photocatalytic production of H2O2.However,its catalytic efficiency is limited by the strong adsorption of O2,which facilitates O―O bond cleavage and reduces selectivity for the 2-electron oxygen reduction reaction(ORR).Fortunately,the strength of the Pt―O bond can be weakened by adjusting the structure of the cocatalyst to modify the electronic structure of Pt.In this paper,Pt and Ag cocatalysts are successively modified on the(010)facet of BiVO4 through a two-step photodeposition method.Due to the occurrence of a displacement reaction during the process,a synergistic catalyst with a hollow AgPt alloy core and an electron-rich Ptδ-shell(AgPt@Pt)structure is ultimately synthesized.Photocatalytic experiments demonstrated that the H2O2 production from BiVO4 modified with hollow AgPt@Pt reached an impressive 1021.5 μmol∙L-1.This corresponds to an AQE of 5.1%,which is 28.6 times higher than that of the Pt/BiVO4 photocatalyst with only 35.7 μmol∙L-1.Furthermore,research results show that AgPt can transfer electrons to the Pt shell to generate electron-rich Ptδ-active sites,thus increasing the antibonding orbital occupancy of Pt―Oads in AgPt@Pt catalysts.This electron redistribution weakens the adsorption strength of O2 on Pt,promoting the 2-electron ORR and facilitating the efficient generation of H2O2.This synthesis strategy offers a versatile approach for preparing other Pt-based nano-alloy cocatalysts with improved activity for the selective reduction of O2 to H2O2.关键词
光催化/富电子Ptδ-/O2吸附/H2O2/BiVO4Key words
Photocatalysis/Electron-rich Ptδ-/O2-adsorption/H2O2/BiVO4分类
化学化工引用本文复制引用
王玉,石海洋,陈子涵,陈峰,王苹,王雪飞..具有富电子Ptδ-壳层的空心AgPt@Pt核壳催化剂:提升光催化H2O2生成选择性与活性[J].物理化学学报,2025,41(7):103-113,11.基金项目
This work was supported by the National Natural Science Foundation of China(22178276),the Postdoctoral Fellowship Program of CPSF(GZC20240888),the National College Students'Innovation and Entrepreneurship Training Program at Wuhan University of Technology(S202410497023).国家自然科学基金(22178276),国家资助博士后研究人员计划(GZC20240888)和武汉理工大学国家大学生创新创业训练计划(S202410497023)资助 （22178276）
