摘要
构建较强氧化还原能力与较高电荷转移效率的阶梯型(S型)异质结光催化剂是提高光催化性能的有效策略。通过溶剂热法在棒状苝酰亚胺(PDI)表面原位生长了ZnIn_(2)S_(4)S纳米片,得益于良好的界面接触与匹配的能带结构,PDI/ZnIn_(2)S_(4)S异质结展现出优异的光催化性能。此外,在同步光催化产氢与苯甲醇氧化全反应体系中,5%PDI/ZnIn_(2)S_(4)S光催化剂表现出较高的产氢性能[21.66mmol/(g·h)]与苯甲醛产率[1.02mmol/(g·h)]分别是纯ZnIn_(2)S_(4)S的2.12倍和3.00倍。基于X射线光电子能谱、瞬态光致发光光谱和电子顺磁共振信号等分析,证实了PDI与ZnIn_(2)S_(4)S之间内建电场的形成与S型电子转移路径。该电荷转移机制保留了复合催化剂较高的氧化还原电位,促进了界面电荷分离与转移,进而提升了光催化性能。该有机-无机S型异质结光催化剂的设计应用为新型双功能催化剂的开发提供了新思路。
The construction of step scheme(S-scheme)heterojunction with a great redox ability and a high charge transfer efficiency is an effective strategy to enhance the photocatalytic activity.ZnIn_(2)S_(4) nanosheets were grown in-situ on the surface of perylenimide(PDI)rods via a solvothermal method.A PDI/ZnIn_(2)S_(4) heterojunction exhibits an excellent photocatalytic performance due to its tight interfacial contact and matched band structures.Moreover,the 5%PDI/ZnIn_(2)S_(4) affords high H_(2)/benzaldehyde production rates of 21.66 mmol/(g·h)and 1.02 mmol/(g·h),respectively,which is 2.12 and 3.00 folds of pristine ZnIn_(2)S_(4),respectively when coupling the photocatalytic H_(2) evolution and the benzyl alcohol oxidation in the reaction system.Based on the results by X-ray photoelectron spectroscopy,transient photoluminescence spectroscopy and electron paramagnetic resonance analysis,the formation of the built-in electric field at the interface of PDI/ZnIn_(2)S_(4) and the S-scheme electron transfer path was confirmed.The enhanced photocatalytic performance and stability can be attributed to the close contact and rich active sites of PDI/ZnIn_(2)S_(4),and the charge carrier migration and increased photoredox properties were improved by a S-scheme charge-transfer route.This organic-inorganic PDI/ZnIn_(2)S_(4) S-scheme heterojunction photocatalyst can be used as a novel bifunctional photocatalyst in converting solar light into clean fuel and chemicals.
作者
唐华
刘玥
王乐乐
刘芹芹
TANG Hua;LIU Yue;WANG Lele;LIU Qinqin(School of Materials Science and Engineering,Jiangsu University,Zhenjiang 212013,Jiangsu,China;School of Environmental Science and Engineering,Qingdao University,Qingdao 266100,Shandong,China)
出处
《硅酸盐学报》
EI
CAS
CSCD
北大核心
2023年第1期14-22,共9页
Journal of The Chinese Ceramic Society
基金
光催化产氧磷酸银基S型可见光光催化剂的设计、制备及机理研究(21975110)
非金属等高激元/氮化碳耦合杂化体系的构建及全光谱响应的光催化制氢性能和机理研究(21972058)
自组装金属配合物纳米颗粒近红外光催化活性本质与乙酰化反应机理探究(22102064)。
关键词
异质结
苝酰亚胺
光催化制氢
苯甲醇氧化
scheme
perylenimide
H_(2) production
benzyl alcohol oxidation
作者简介
第一作者:唐华(1979-),男,博士,教授,E-mail:huatang79@163.com;通信作者:刘芹芹(1981-),女,博士,教授,E-mail:qqliu@ujs.edu.cn。
