氧掺杂和中空结构介导效应在高效光催化过氧化氢生产中实现快速电子转移

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中文摘要：因其安全、绿色、低成本的特点,利用太阳能光催化生产过氧化氢是解决能源危机的环境友好型方案,但其效率低下,严重阻碍了其规模化可行性.在这项工作中,通过使用简单的两步水热法在O掺杂的空心g-C3N4纳米球表面生长In2S3超薄纳米片,成功构建了空心核壳结构OCN@In2S3复合光催化剂.独特的中空结构提供了更大的比表面积,增强了光吸收.O掺杂增加了活性位点的数量,异质结的存在促进了光生载流子的快速分离和转移.在可见光照射下,OCN@In2S3的H2O2产率达到632.5 μmolh-1 g-1,是普通g-C3N4的5.7倍,是In2S3的12.3倍,高于大多数g-C3N4基光催化剂.淬灭实验和电子顺磁共振光谱表明,·O2-是光催化产生H2O2的中间产物,并且反应过程主要遵循两步单电子反应路径.Koutecky-Levich图证实了合成的OCN@In2S3在催化反应中保持了较高的两电子ORR选择性(n=1.67).通过光致发光、电化学阻抗谱和紫外光电子能谱等表征手段阐明了可能的光催化机理,证实了OCN@In2S3有效抑制光生载流子的复合.这项工作为开发高活性的能量转换光催化剂提供了一种简单而有吸引力的策略.

外文标题：Oxygen doping and hollow structure-mediated effects to enable rapid electron transfer during photocatalytic hydrogen peroxide production

外文摘要：The photocatalytic production of hydrogen peroxide using solar energy is an environment-friendly solu-tion to the energy crisis,but fits low eficiency hinders its scale-up feasibility.In this work,a hollow core-shell structure OCN@In2S3 composite photocatalyst was constructed by growing In2S3 ultrathin nanosheets on the surface of O-doped hollow g-C3N4 nanospheres using a two-step hydrothermal method.The hollow structure provided a high specific surface area and enhanced light absorption.O doping increased the number of active sites,and the heterojunction promoted the rapid separation and transfer of photogenerated carriers.Under visible light irradiation,the H2O2 yield of OCN@In2S3 reached 632.5 μmol h-1 g-1,which was 5.7 times higher than that of g-C3N4 and 12.3 times that of In2S3,as well as higher than most g-C3N4-based photocatalysts.Quenching experi-ments and electron paramagnetic resonance spectroscopy showed that·O2-was an intermediate product formed during photocatalytic H2O2 generation.The reaction primarily fol-lowed a two-step single-electron pathway.The Koutecky-Le-vich diagram confirmed that the synthesized OCN@In2S3 maintained a high two-electron ORR selectivity during the catalytic reaction(n=1.67).The photocatalytic mechanism was elucidated by photoluminescence,electrochemical im-pedance spectroscopy,and ultraviolet photoelectron spectro-scopy,which confirmed that OCN@In2S3 inhibited the recombination of photogenerated carriers.This work provides a simple and attractive strategy for developing highly active energy-conversion photocatalysts.

外文关键词：

photocatalytic productionO-dopinghollow-shell structurerapid separation and transferhigh activity

作者：

徐燕东、台婉玉、王沚睿、张琳琳、王德欣、廖建军

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作者单位：

Key Laboratory of Agro-Forestry Environmental Processes and Ecological Regulation of Hainan Province,School of Ecology and Environment,Hainan University,Haikou 570228,China

关键词：

photocatalytic production O-doping hollow-shell structure rapid separation and transfer high activity

基金：

Hainan Province Science and Technology Special FundHaikou City Science and Technology Plan ProjectNational Natural Science Foundation of ChinaHainan Provincial Natural Science Foundation of ChinaScientific Research Project of Hainan Higher Education InstitutionsHainan University Research Startup Fund

项目编号：

ZDYF2022SHFZ0942023-01252100038420RC530Hnky2023-9kyqdzr22185

出版年：

2024

DOI：

10.1007/s40843-023-2659-9

中国科学:材料科学(英文)

CSTPCD

ISSN：

年,卷(期)：2024.67(1)

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