Compressive interatomic distance stimulates photocatalytic oxygen-oxygen coupling to hydrogen peroxide  

原子间距调控诱导光催化氧-氧耦合生成过氧化氢

作　　者：Kai-Lian Zhang Hua-Chang Chen Leigang Wang Hua Tang Zhao-Qing Liu 张开莲;陈铧畅;王雷刚;唐华;刘兆清

机构地区：[1]School of Chemistry and Chemical Engineering/Institute of Clean Energy and Materials/Guangzhou Key Laboratory for Clean Energy and Materials/Huangpu Hydrogen Innovation Center,Guangzhou University,Guangzhou 510006,China [2]School of Materials Science and Engineering,Jiangsu University,Zhenjiang 212013,China [3]School of Environmental Science and Engineering,Qingdao University,Qingdao 266071,China

出　　处：《Science Bulletin》2025年第4期536-545,共10页科学通报(英文版)

基　　金：supported by the National Natural Science Foundation of China(U24A20541 and 22278094);the Guangdong Graduate Education Innovation Program(2023JGXM_102);the Basic and Applied Basic Research Program of Guangzhou(SL2024A03J00499);the University Innovation Team Scientific Research Project of Guangzhou(202235246);the Undergraduate Innovation Training Program of Guangzhou University(202211078121).

摘　　要：Photocatalytic hydrogen peroxide(H2O2)generation is largely subject to the sluggish conversion kinetics of the superoxide radical(O_(2)⋅^(-))intermediate,which has relatively low reactivity and requires high energy.Here,we present a lattice-strain strategy to accelerate the conversion of O_(2)⋅^(-)to highly active singlet oxygen(1O2)by optimizing the distance between two adjacent active sites,thereby stimulating H2O2 generation via low-barrier oxygen-oxygen coupling.As the initial demonstration,the defect-induced strain in ZnIn2S4 nanosheet optimizes the distance of two adjacent Zn sites from 3.85 to 3.56Å,resulting in that ZnIn2S4 with 0.7%compressive strain affords 3086.00μmol g^(-1)h^(-1)yield of H2O2 with sacrificial agent.This performance is attributed to the strain-induced enhancement of electron coupling between the compressed adjacent Zn sites,which promotes low-barrier oxygen-oxygen coupling to active 1O2 intermediate.This finding paves the way for atomic-scale manipulation of reactive sites,offering a promising approach for efficient H2O2 photosynthesis.

关 键 词：Superoxide radical Singlet oxygen lOxygen-Oxygen Couplingl Hydrogen Peroxide 

分 类 号：O64[理学—物理化学]