物理化学学报2023，Vol.39Issue(4)：67-75,9.DOI:10.3866/PKU.WHXB202205039
阳离子镍基MOF自组装CdS/PFC-8催化剂用于可见光光催化选择性苯甲醇氧化耦合产氢
Cationic Ni-MOF-Assembled CdS/PFC-8 Catalyst for Photocatalytic Hydrogen Production with Selective Benzyl Alcohol Oxidation under Visible Light
摘要
Abstract
Visible-light-driven photocatalytic H2 evolution coupled with oxidative organic synthesis is attracting extensive attention owing to the environmental friendliness and sustainability of these processes,which can coproduce clean H2 fuel and high-value chemicals under mild conditions without requiring sacrificial agents.Semiconductor materials and metal-organic framework(MOF)materials have been widely used in photocatalys owing to their properties and advantages.In this work,we successfully synthesized a novel effective catalyst(named CdS/PFC-8)by electrostatic self-assembly.Among the components of the CdS/PFC-8 composite,PFC-8 was a nickel-based MOF.The CdS/PFC-8 composite,as a noble metal-free catalyst,enabled excellent photocatalytic H2 evolution and benzyl alcohol oxidation under visible light.A series of catalytic characterizations were performed with the CdS/PFC-8 composite.X-ray diffraction(XRD)and scanning electron microscopy(SEM)results demonstrated the successful synthesis of the CdS/PFC-8 composite.X-ray photoelectron spectroscopy(XPS)results demonstrated the existence of an interfacial interaction between CdS nanorods and PFC-8.The optoelectronic performance was characterized by ultraviolet-visible diffuse reflectance spectroscopy(UV-Vis DRS),photoluminescence(PL)spectroscopy,and electrochemical tests,and the results demonstrated the visible-light response and photocatalytic feasibility of the CdS/PFC-8 composite.The photocatalytic results obtained with different catalysts were compared.Under visible light,the CdS/PFC-8 composite enabled the generation of H2 with the selective oxidation of benzyl alcohol in a single reaction.It exhibited a remarkable H2 production rate of 3376 μmol·g-1·h-1;further,the benzaldehyde yield was 4120 μmol·g-1·h-1,which is higher than that of CdS alone.Photocatalytic cycling reactions were carried out to verify the activity and stability of the catalysts.The changes in the catalysts before and after the reaction were analyzed,and the results suggested that the nickel in PFC-8 could be used as a catalytically active site to improve the catalytic activity.In addition,the possible photocatalytic reaction mechanism was discussed.This work highlights the advantages of combining the functionalities of semiconductors and MOFs to enhance the photocatalytic activity.关键词
光催化/金属有机框架/硫化镉/氢气/苯甲醇Key words
Photocatalytic/Metal-organic frameworks/Cadmium sulfide/Hydrogen/Benzyl alcohol分类
化学化工引用本文复制引用
项景超,李静君,杨雪,高水英,曹荣..阳离子镍基MOF自组装CdS/PFC-8催化剂用于可见光光催化选择性苯甲醇氧化耦合产氢[J].物理化学学报,2023,39(4):67-75,9.基金项目
This work was supported by the National Key Research and Development Program of China(2021YFA1501500,2017YFA0700102),the National Natural Science Foundation of China(22033008,21871263,22071245,22171265),Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZZ103).国家重点研究开发计划(2021YFA1501500,2017YFA0700102),国家自然科学基金(22033008,21871263,22071245,22171265)与中国福建光电信息科学与技术创新实验室(2021ZZ103)资助项目 （2021YFA1501500,2017YFA0700102）
