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原子间距调控诱导光催化氧-氧耦合生成过氧化氢（英文）

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

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【作者】 张开莲； 陈铧畅； 王雷刚； 唐华； 刘兆清；

【Author】 Kai-Lian Zhang;Hua-Chang Chen;Leigang Wang;Hua Tang;Zhao-Qing Liu;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;School of Materials Science and Engineering, Jiangsu University;School of Environmental Science and Engineering, Qingdao University;

【通讯作者】 刘兆清;

【机构】 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； School of Materials Science and Engineering, Jiangsu University； School of Environmental Science and Engineering, Qingdao University；

【摘要】 Photocatalytic hydrogen peroxide（H2O2） generation is largely subject to the sluggish conversion kinetics of the superoxide radical(O2.-) intermediate, which has relatively low reactivity and requires high energy.Here, we present a lattice-strain strategy to accelerate the conversion of O2.-to highly active singlet oxygen（1O2） by optimizing the distance between two adjacent active sites, thereby stimulating H2O2generation via low-barrier oxygen-oxygen coupling. As the initial demonstration, the defect-induced strain in Zn In2S4nanosheet optimizes the distance of two adjacent Zn sites from 3.85 to 3.56 ?, resulting in that Zn In2S4with 0.7% compressive strain affords 3086.00 μmol g-1h-1yield of H2O2with 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 active1O2intermediate. This finding paves the way for atomic-scale manipulation of reactive sites, offering a promising approach for efficient H2O2photosynthesis.

【Abstract】 Photocatalytic hydrogen peroxide（H2O2） generation is largely subject to the sluggish conversion kinetics of the superoxide radical(O2.-) intermediate, which has relatively low reactivity and requires high energy.Here, we present a lattice-strain strategy to accelerate the conversion of O2.-to highly active singlet oxygen（1O2） by optimizing the distance between two adjacent active sites, thereby stimulating H2O2generation via low-barrier oxygen-oxygen coupling. As the initial demonstration, the defect-induced strain in Zn In2S4nanosheet optimizes the distance of two adjacent Zn sites from 3.85 to 3.56 ?, resulting in that Zn In2S4with 0.7% compressive strain affords 3086.00 μmol g-1h-1yield of H2O2with 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 active1O2intermediate. This finding paves the way for atomic-scale manipulation of reactive sites, offering a promising approach for efficient H2O2photosynthesis.

【关键词】 Superoxide radical； Singlet oxygen； Oxygen-Oxygen Coupling； Hydrogen Peroxide；
【Key words】 Superoxide radical； Singlet oxygen； Oxygen-Oxygen Coupling； Hydrogen Peroxide；
【基金】 supported by the National Natural Science Foundation of China (U24A20541 and 22278094);the Guangdong Graduate Education Innovation Program (2023JGXM_102);the ‘‘Double Thousand Plano Initiative of Jiangxi Province (jxsq2023102142);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)
  • 【文献出处】 Science Bulletin ,科学通报(英文版) , 编辑部邮箱 ,2025年04期
  • 【分类号】O643.36;O644.1;TQ123.6
  • 【下载频次】30
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