Simultaneous oxidation of alcohols and hydrogen evolution in a hybrid system under visible light irradiation

被引:79
作者
Li, Fei [1 ]
Wang, Yong [1 ]
Du, Jian [1 ]
Zhu, Yong [1 ]
Xu, Congying [1 ]
Sun, Licheng [1 ,2 ]
机构
[1] Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China
[2] KTH Royal Inst Technol, Sch Chem Sci & Engn, Dept Chem, S-10044 Stockholm, Sweden
基金
中国国家自然科学基金;
关键词
Photocatalysis; Selective oxidation of alcohol; Hydrogen evolution; Molecular catalyst; Hybrid system; CARBON NITRIDE SEMICONDUCTORS; SELECTIVE OXIDATION; ENERGY-CONVERSION; BENZYL ALCOHOL; CO2; REDUCTION; WATER; PHOTOCATALYST; BIOMASS; DEHYDROGENATION; OXYGENATION;
D O I
10.1016/j.apcatb.2017.11.072
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Water oxidation as a multi-electron transfer and endothermal reaction has been considered to be the bottleneck of solar-driven water splitting into oxygen and hydrogen. Herein, an alternative approach for solar energy conversion is developed by coupling Hy generation with the selective oxidation of alcohol. In a closed redox system containing molecular ruthenium catalyst (RuCat) and Pt modified g-C3N4 (Pt-g-C3N4) composite, hydrogen production is concomitant with the oxidation of benzyl alcohols to aldehydes with over 99% selectivity in the presence of visible light and pure water. By contrary, the system lacking molecular catalyst only exhibits low to moderate selectivities towards aldehydes. The remarkably improved selectivity is attributed to the formation of highly active Ru(IV) = O intermediate through efficient hole transfer from g-C3N4 to RuCat.
引用
收藏
页码:258 / 263
页数:6
相关论文
共 38 条
[1]   Hydrogen Storage and Energy Recovery Using Aldehydes and Ketones: A Key Role for Catalysis [J].
Angelici, Robert J. .
ACS CATALYSIS, 2011, 1 (07) :772-776
[2]   Visible-light-driven selective oxidation of benzyl alcohol and thioanisole by molecular ruthenium catalyst modified hematite [J].
Bai, Lichen ;
Li, Fei ;
Wang, Yong ;
Li, Hua ;
Jiang, Xiaojuan ;
Sun, Licheng .
CHEMICAL COMMUNICATIONS, 2016, 52 (62) :9711-9714
[3]  
Cha HG, 2015, NAT CHEM, V7, P328, DOI [10.1038/NCHEM.2194, 10.1038/nchem.2194]
[4]   Ferrites boosting photocatalytic hydrogen evolution over graphitic carbon nitride: a case study of (Co, Ni)Fe2O4 modification [J].
Chen, Jie ;
Zhao, Daming ;
Diao, Zhidan ;
Wang, Miao ;
Shen, Shaohua .
SCIENCE BULLETIN, 2016, 61 (04) :292-301
[5]   Molecular and textural engineering of conjugated carbon nitride catalysts for selective oxidation of alcohols with visible light [J].
Chen, Yan ;
Zhang, Jinshui ;
Zhang, Mingwen ;
Wang, Xinchen .
CHEMICAL SCIENCE, 2013, 4 (08) :3244-3248
[6]   Making Oxygen with Ruthenium Complexes [J].
Concepcion, Javier J. ;
Jurss, Jonah W. ;
Brennaman, M. Kyle ;
Hoertz, Paul G. ;
Patrocinio, Antonio Otavio T. ;
Murakami Iha, Neyde Yukie ;
Templeton, Joseph L. ;
Meyer, Thomas J. .
ACCOUNTS OF CHEMICAL RESEARCH, 2009, 42 (12) :1954-1965
[7]   Catalysts made of earth-abundant elements (Co, Ni, Fe) for water splitting: Recent progress and future challenges [J].
Du, Pingwu ;
Eisenberg, Richard .
ENERGY & ENVIRONMENTAL SCIENCE, 2012, 5 (03) :6012-6021
[8]  
Fukuzumi S, 2011, NAT CHEM, V3, P38, DOI [10.1038/nchem.905, 10.1038/NCHEM.905]
[9]   Photocatalytic Oxidation of Hydrocarbons in Water by Ruthenium Complexes [J].
Kalita, Diganta ;
Radaram, Bhasker ;
Brooks, Brandon ;
Kannam, Pooja Priyanka ;
Zhao, Xuan .
CHEMCATCHEM, 2011, 3 (03) :571-573
[10]   Solar-Driven Reduction of Aqueous Protons Coupled to Selective Alcohol Oxidation with a Carbon Nitride-Molecular Ni Catalyst System [J].
Kasap, Hatice ;
Caputo, Christine A. ;
Martindale, Benjamin C. M. ;
Godin, Robert ;
Lau, Vincent Wing-hei ;
Lotsch, Bettina V. ;
Durrant, James R. ;
Reisner, Erwin .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (29) :9183-9192