Spontaneous Redox Approach to the Self-Assembly Synthesis of Au/CeO2 Plasmonic Photocatalysts with Rich Oxygen Vacancies for Selective Photocatalytic Conversion of Alcohols

被引:76
作者
Cui, Zhiqing [1 ,2 ]
Wang, Weikang [1 ,2 ]
Zhao, Cuijiao [1 ,2 ]
Chen, Chun [1 ]
Han, Miaomiao [1 ]
Wang, Guozhong [1 ]
Zhang, Yunxia [1 ]
Zhang, Haimin [1 ]
Zhao, Huijun [1 ,3 ]
机构
[1] Chinese Acad Sci, Ctr Environm & Energy Nanomat, Anhui Key Lab Nanomat & Nanotechnol, Key Lab Mat Phys,CAS Ctr Excellence Nanosci,Inst, Hefei 230031, Anhui, Peoples R China
[2] Univ Sci & Technol China, Hefei 230026, Anhui, Peoples R China
[3] Griffith Univ, Ctr Clean Environm & Energy, Gold Coast Campus, Southport, Qld 4222, Australia
基金
国家重点研发计划;
关键词
spontaneous redox approach; self-assembly synthesis; Au/CeO2; selective oxidation of alcohols; visible light activity; VISIBLE-LIGHT; AEROBIC OXIDATION; BENZYL ALCOHOL; CATALYTIC APPLICATIONS; ULTRATHIN NANOSHEETS; AROMATIC ALCOHOLS; TIO2; CEO2; OPTIMIZATION; ACTIVATION;
D O I
10.1021/acsami.8b10705
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
We present the self-assembly synthesis of core shell structure Au/CeO2 composites with different Au loadings through a spontaneous chemical redox approach at an ambient temperature utilizing HAuCl4. and Ce(NO3)(3) as reaction substrates in an alkaline environment. The results demonstrate that the as-synthesized Au/CeO2 composites exhibit spherical shape morphologies with porous structures, composed of Au nanoparticle (similar to 10 rim) cores and CeO2 nanoparticle shells with abundant oxygen vacancies. The introduction of Au nanoparticles in CeO2 not only effectively improves the visible light utilization efficiency but also provides rich surface catalytic active sites for highly efficient visible light photocatalysis. As visible light photocatalysts (lambda > 400 nm), the as-synthesized Au/CeO2 composites with the Au loading amount wt >= 4.0% exhibit high conversion and selectivity (similar to 100%) of benzyl alcohol to benzaldehyde under the given experimental conditions. Moreover, Au/CeO2 also shows a general applicability as a visible light photocatalyst for the selective oxidation of other alcohols to corresponding aldehydes or ketones. The photocatalytic mechanism studies indicate that the photoelectrons/holes produced from the photoexcited Au and the formed superoxide radicals in the oxygen vacancies of CeO2 synergistically contribute to the high performance of the selective photocatalytic oxidation of alcohols to aldehydes or ketones.
引用
收藏
页码:31394 / 31403
页数:10
相关论文
共 45 条
[1]   Solvent-free oxidation of primary alcohols to aldehydes using Au-Pd/TiO2 catalysts [J].
Enache, DI ;
Edwards, JK ;
Landon, P ;
Solsona-Espriu, B ;
Carley, AF ;
Herzing, AA ;
Watanabe, M ;
Kiely, CJ ;
Knight, DW ;
Hutchings, GJ .
SCIENCE, 2006, 311 (5759) :362-365
[2]   A mild and environmentally benign strategy towards hierarchical CeO2/Au nanoparticle assemblies with crystal facet-enhanced catalytic effects for benzyl alcohol aerobic oxidation [J].
Gong, Xia ;
Liu, Baocang ;
Zhang, Geng ;
Xu, Guangran ;
Zhao, Tuo ;
Shi, Dichao ;
Wang, Qin ;
Zhang, Jun .
CRYSTENGCOMM, 2016, 18 (27) :5110-5120
[3]   Recent advances in heterogeneous selective oxidation catalysis for sustainable chemistry [J].
Guo, Zhen ;
Liu, Bin ;
Zhang, Qinghong ;
Deng, Weiping ;
Wang, Ye ;
Yang, Yanhui .
CHEMICAL SOCIETY REVIEWS, 2014, 43 (10) :3480-3524
[4]   Aerosol-Sprayed Gold/Ceria Photocatalyst with Superior Plasmonic Hot Electron-Enabled Visible-Light Activity [J].
Jia, Henglei ;
Zhu, Xiao-Ming ;
Jiang, Ruibin ;
Wang, Jianfang .
ACS APPLIED MATERIALS & INTERFACES, 2017, 9 (03) :2560-2571
[5]   Insights into the Surface-Defect Dependence of Photoreactivity over CeO2 Nanocrystals with Well-Defined Crystal Facets [J].
Jiang, Dong ;
Wang, Wenzhong ;
Zhang, Ling ;
Zheng, Yali ;
Wang, Zhong .
ACS CATALYSIS, 2015, 5 (08) :4851-4858
[6]   Equilibrating the Plasmonic and Catalytic Roles of Metallic Nanostructures in Photocatalytic Oxidation over Au-Modified CeO2 [J].
Jiang, Dong ;
Wang, Wenzhong ;
Sun, Songmei ;
Zhang, Ling ;
Zheng, Yali .
ACS CATALYSIS, 2015, 5 (02) :613-621
[7]   Metal/Semiconductor Hybrid Nanostructures for Plasmon-Enhanced Applications [J].
Jiang, Ruibin ;
Li, Benxia ;
Fang, Caihong ;
Wang, Jianfang .
ADVANCED MATERIALS, 2014, 26 (31) :5274-5309
[8]   Palladium Nanoparticles Supported in the Nanospaces of Imidazolium-Based Bifunctional PMOs: The Role of Plugs in Selectivity Changeover in Aerobic Oxidation of Alcohols [J].
Karimi, Babak ;
Khorasani, Mojtaba ;
Vali, Hojatollah ;
Vargas, Carolina ;
Luque, Rafael .
ACS CATALYSIS, 2015, 5 (07) :4189-4200
[9]   Nanostructured Ceria-Silver Synthesized in a One-Pot Redox Reaction Catalyzes Carbon Oxidation [J].
Kayama, Tomoyuki ;
Yamazaki, Kiyoshi ;
Shinjoh, Hirofumi .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (38) :13154-13155
[10]   Advanced Nanoarchitectures for Solar Photocatalytic Applications [J].
Kubacka, Anna ;
Fernandez-Garcia, Marcos ;
Colon, Gerardo .
CHEMICAL REVIEWS, 2012, 112 (03) :1555-1614