NH2-MIL-125(Ti)/TiO2 composites as superior visible-light photocatalysts for selective oxidation of cyclohexane

被引:122
作者
Zhao, Xiaoxia [2 ]
Zhang, Ying [1 ,2 ]
Wen, Ping [2 ]
Xu, Guang [2 ]
Ma, Di [2 ]
Qiu, Ping [2 ]
机构
[1] State Key Lab Heavy Oil Proc, Beijing, Peoples R China
[2] China Univ Petr, Dept Mat Sci & Engn, Beijing 102249, Peoples R China
基金
中国国家自然科学基金;
关键词
NH2-MIL-125(T)/TiO2; Visible light; Photocatalysis; Cyclohexane oxidation; METAL-ORGANIC FRAMEWORK; C-H BONDS; DRIVEN PHOTOCATALYST; AEROBIC OXIDATION; SOLVENT; REDUCTION; GRAPHENE; POLYMER; OXYGEN; STATES;
D O I
10.1016/j.mcat.2018.04.004
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
Semiconductor-metal-organic framework (MOF) hybrid photocatalysts have aroused increasing interest because of their enhanced photocatalytic activity. In this work, NH2-MIL-125(Ti)/TiO2 composites with different molar ratios were successfully prepared by a facile one-pot solvothermal method and used for visible-light driven photocatalytic selective oxidation of cyclohexane. The as-prepared NH2-MIL-125(Ti)/TiO2 composites presented better catalytic performances compared with NH2-MIL-125(Ti). This is due to the energy bands coupling and intimate interfacial contact between NH2-MIL-125(Ti) and TiO2, which can improve the photon-generated carrier transfer and minimize the recombination of electron-hole pairs. For the optimum composite photo catalyst, the activity was three times higher than that of NH2-MIL-125(Ti) in visible-light driven photocatalytic cyclohexane oxidation using molecular oxygen as oxidant at room temperature and under ambient pressure. Additionally, the effects of illumination time on the photocatalytic performance and reusability of the optimum composite photocatalyst were investigated in detail. Finally, a possible reaction mechanism has been proposed based on controlling experiments using different radical scavenger techniques, which prove that the photo-generated holes are significantly involved in the oxidation process.
引用
收藏
页码:175 / 183
页数:9
相关论文
共 53 条
[1]   Luminescent metal-organic frameworks [J].
Allendorf, M. D. ;
Bauer, C. A. ;
Bhakta, R. K. ;
Houk, R. J. T. .
CHEMICAL SOCIETY REVIEWS, 2009, 38 (05) :1330-1352
[2]   The photo-oxidation of cyclohexane on titanium dioxide: an investigation of competitive adsorption and its effects on product formation and selectivity [J].
Almquist, CB ;
Biswas, P .
APPLIED CATALYSIS A-GENERAL, 2001, 214 (02) :259-271
[3]   Photocatalytic oxygenation of cyclohexane on titanium dioxide suspensions: Effect of the solvent and of oxygen [J].
Boarini, P ;
Carassiti, V ;
Maldotti, A ;
Amadelli, R .
LANGMUIR, 1998, 14 (08) :2080-2085
[4]   Titanium dioxide nanomaterials: Synthesis, properties, modifications, and applications [J].
Chen, Xiaobo ;
Mao, Samuel S. .
CHEMICAL REVIEWS, 2007, 107 (07) :2891-2959
[5]   Tunability of electronic band gaps from semiconducting to metallic states via tailoring Zn ions in MOFs with Co ions [J].
Choi, Jung Hoon ;
Choi, Yoon Jeong ;
Lee, Jung Woo ;
Shin, Weon Ho ;
Kang, Jeung Ku .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2009, 11 (04) :628-631
[6]   Ab-initio prediction of materials properties with CRYSTAL:: MOF-5 as a case study [J].
Civalleri, Bartolomeo ;
Napoli, Francesco ;
Noel, Yves ;
Roetti, Carla ;
Dovesi, Roberto .
CRYSTENGCOMM, 2006, 8 (05) :364-371
[7]   The nitrogen-boron paramagnetic center in visible light sensitized N-B co-doped TiO2. Experimental and theoretical characterization [J].
Czoska, A. M. ;
Livraghi, S. ;
Paganini, M. C. ;
Giamello, E. ;
Di Valentin, C. ;
Pacchioni, G. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2011, 13 (01) :136-143
[8]   A New Photoactive Crystalline Highly Porous Titanium(IV) Dicarboxylate [J].
Dan-Hardi, Meenakshi ;
Serre, Christian ;
Frot, Theo ;
Rozes, Laurence ;
Maurin, Guillaume ;
Sanchez, Clement ;
Ferey, Gerard .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (31) :10857-+
[9]   Selective photo(catalytic)-oxidation of cyclohexane:: Effect of wavelength and TiO2 structure on product yields [J].
Du, P ;
Moulijn, JA ;
Mul, G .
JOURNAL OF CATALYSIS, 2006, 238 (02) :342-352
[10]   An Amine-Functionalized Titanium Metal-Organic Framework Photocatalyst with Visible-Light-Induced Activity for CO2 Reduction [J].
Fu, Yanghe ;
Sun, Dengrong ;
Chen, Yongjuan ;
Huang, Renkun ;
Ding, Zhengxin ;
Fu, Xianzhi ;
Li, Zhaohui .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2012, 51 (14) :3364-3367