光热效应增强的Au/RGO/Na_(2)Ti_(3)O_(7)光催化加氢性能  

Photothermal Enhanced Photocatalytic Hydrogenation Performance of Au/RGO/Na_(2)Ti_(3)O_(7)

作　　者：孟祥钰 詹琦 武亚南 马晓双 姜靖逸 孙岳明[1] 代云茜[1] MENG Xiangyu;ZHAN Qi;WU Yanan;MA Xiaoshuang;JIANG Jingyi;SUN Yueming;DAI Yunqian(School of Chemistry and Chemical Engineering,Southeast University,Nanjing 211189,China)

机构地区：[1]东南大学化学化工学院,南京211189

出　　处：《高等学校化学学报》2022年第3期136-147,共12页Chemical Journal of Chinese Universities

基　　金：国家自然科学基金(批准号:21975042);江苏省六大人才高峰基金(批准号:XCL-082);江苏省科协青年托举人才基金资助。

摘　　要：将典型的光热等离激元石墨烯和纳米金简便地负载在钛酸钠(Na_(2)Ti_(3)O_(7))载体上,构建出具有较窄禁带宽度和较高光催化活性的Au/RGO/Na_(2)Ti_(3)O_(7)光热辅助光催化体系.研究发现,石墨烯片层与金纳米颗粒在光照下,通过局域表面等离激元共振效应诱导产生大量的热电子,以活化反应物并降低反应活化能,其引发的光热效应还可精准提升光催化体系中反应位点附近的温度,从而大幅提升光催化反应速率.通过构建特殊微支结构,进一步增强了Au/RGO/Na_(2)Ti_(3)O_(7)催化剂对光的捕获,并限域锚定高表面能催化剂以增强体系的稳定性.在光热、光催化的高效协同增强下,Au/RGO/Na_(2)Ti_(3)O_(7)催化剂体系对对硝基苯酚和肉桂醛的加氢反应均表现出增强的光催化活性.光热辅助下的Au/RGO/Na_(2)Ti_(3)O_(7)光催化剂在对硝基苯酚反应中的转换频率(TOF)值高达54.4 min^(-1),反应活化能显著降低至15.78 kJ/mol,且其在长效测试中表现出良好的稳定性(4次循环催化后,转化率的保持率近90%)Typical photothermal plasmon graphene and nano gold were simply supported on sodium titanate(Na_(2)Ti_(3)O_(7)).Thus,Au/RGO/Na_(2)Ti_(3)O_(7) photothermal-assisted photocatalytic system was constructed,featured with nar⁃row bandgap and high photocatalytic activity.Graphene sheets and gold nanoparticles could generate a large number of hot-electron for activating reactants and reducing the reaction energy,through their local surface plasmon reso⁃nance effect under light.The photothermal effect can precisely raise the temperature near the reaction site,thus great⁃ly improving the photocatalytic reaction rate.In addition,the Au/RGO/Na_(2)Ti_(3)O_(7) catalyst is endow with enhanced light-trapping performance by ably constructing special micro-branched structure.Also,the stability of catalyst was enhanced by confinement effects.Under the synergistic enhancement of photothermal effect and photocatalysis,Au/RGO/Na_(2)Ti_(3)O_(7) catalyst showed enhanced photocatalytic activity for the p-nitrophenol hydrogenation and cin-nam⁃aldehyde hydrogenation.The turnover frequency(TOF)of the p-nitrophenol reduction reaction catalyzed by the photo⁃thermal-assisted Au/RGO/Na_(2)Ti_(3)O_(7) was up to 54.4 min^(-1),and the activation energy barrier was significantly reduced to 15.78 kJ/mol.Moreover,it showed high stability in the long-term test(after 4 cycling test,the conversion retention rate was nearly 90%).

关 键 词：光热效应 光催化 热电子 加氢还原 

分 类 号：O643[理学—物理化学]