Pd/TiO Nanocatalyst with Strong Metal-Support Interaction for Highly Efficient Durable Heterogeneous Hydrogenation

被引:95
作者
Imran, M. [1 ]
Yousaf, Ammar B. [1 ]
Zhou, Xiao [1 ]
Jiang, Yi-Fan [1 ]
Yuan, Cheng-Zong [1 ]
Zeb, Akif [1 ]
Jiang, Nan [1 ]
Xu, An-Wu [1 ]
机构
[1] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Div Nanomat & Chem, Hefei 230026, Anhui, Peoples R China
基金
中国国家自然科学基金;
关键词
RAY PHOTOELECTRON-SPECTROSCOPY; CATALYTIC-ACTIVITY; TITANIUM MONOXIDE; CO2; HYDROGENATION; NANOPARTICLES; OXIDES; PHOTOCATALYSIS; OXIDATION; VACANCIES; METHANOL;
D O I
10.1021/acs.jpcc.6b10274
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
Developing heterogeneous catalysts that promote activation of hydrogen and adsorption of reactants on the surface is crucial to improve the activity of hydrogenation reactions. Herein, we present the use of highly reduced TiO support for loading noble metal nanoparticles, which provides a synergistic effect on boosting catalytic activity. The lowtemperature polymorph of titanium monoxide is used as support and promoter, which contains vacancies in both the Ti and 0 sublattices with ordered distribution. The lattice vacancies increase the donor density and enhance the adsorption of substrate and hydrogen and subsequently lower the activation energy required for the hydrogen dissociation. Moreover, the existence of strong metal support interactions in Pd/TiO ascertained from HRTEM and XPS analysis is responsible for both the strong binding of Pd nanoparticles and improved electronic conductivity, resulting in enhanced catalytic performance. The as synthesized Pd/TiO catalyst has been evaluated for the hydrogenation of styrene and 4-nitrophenol (4NP) and shows excellent performance. The rate constant for 4 NP reduction over Pd/TiO is 0.05 s(-1), which is higher than the previously reported data; moreover, the catalyst shows good stability up to 10 successive cycles. Hydrogenation of styrene is conducted at ambient conditions using Pd/TiO as catalyst, which exhibits remarkably high turnover frequency (TOP) of 4838 h(-1). The catalyst can be recovered and recycled several times without a marked loss of activity. The results show that our Pd/TiO catalyst is one of the highest activity among reported heterogeneous hydrogenation catalysts. The obtained Pd/TiO catalyst may hold great potential in catalysis for organic transformations and other reactions.
引用
收藏
页码:1162 / 1170
页数:9
相关论文
共 52 条
[1]  
[Anonymous], 1992, HDB XRAY PHOTOELECTR
[2]   Structural and magnetic properties of mechanochemically synthesized nanocrystalline titanium monoxide [J].
Barudzija, Tanja ;
Gusev, Alexey A. ;
Jugovic, Dragana ;
Dramicanin, Miroslav ;
Zdujic, Miodrag ;
Jovalekic, Cedomir ;
Mitric, Miodrag .
HEMIJSKA INDUSTRIJA, 2012, 66 (02) :181-186
[3]   Selective and regular localization of accessible Pt nanoparticles inside the walls of an ordered silica: Application as a highly active and well-defined heterogeneous catalyst for propene and styrene hydrogenation reactions [J].
Boualleg, M. ;
Norsic, S. ;
Baudouin, D. ;
Sayah, R. ;
Quadrelli, E. A. ;
Basset, J. -M. ;
Candy, J. -P. ;
Delichere, P. ;
Pelzer, K. ;
Veyre, L. ;
Thieuleux, C. .
JOURNAL OF CATALYSIS, 2011, 284 (02) :184-193
[4]   Control of Metal Nanocrystal Size Reveals Metal-Support Interface Role for Ceria Catalysts [J].
Cargnello, Matteo ;
Doan-Nguyen, Vicky V. T. ;
Gordon, Thomas R. ;
Diaz, Rosa E. ;
Stach, Eric A. ;
Gorte, Raymond J. ;
Fornasiero, Paolo ;
Murray, Christopher B. .
SCIENCE, 2013, 341 (6147) :771-773
[5]   Influence of the strong metal support interaction effect (SMSI) of Pt/TiO2 and Pd/TiO2 systems in the photocatalytic biohydrogen production from glucose solution [J].
Colmenares, Juan C. ;
Magdziarz, Agnieszka ;
Aramendia, Maria A. ;
Marinas, Alberto ;
Marinas, Jose M. ;
Urbano, Francisco J. ;
Navio, Jose A. .
CATALYSIS COMMUNICATIONS, 2011, 16 (01) :1-6
[6]   Support effect in high activity gold catalysts for CO oxidation [J].
Comotti, M ;
Li, WC ;
Spliethoff, B ;
Schüth, F .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (03) :917-924
[7]   C2H2 Treatment as a Facile Method to Boost the Catalysis of Pd Nanoparticulate Catalysts [J].
Dai, Yan ;
Liu, Shengjie ;
Zheng, Nanfeng .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (15) :5583-5586
[8]   Polymer-templated synthesis of hollow Pd-CeO2 nanocomposite spheres and their catalytic activity and thermal stability [J].
Du, Chenhao ;
Guo, Yun ;
Guo, Yanglong ;
Gong, Xue-qing ;
Lu, Guanzhong .
JOURNAL OF MATERIALS CHEMISTRY A, 2015, 3 (46) :23230-23239
[9]   Ceria Maintains Smaller Metal Catalyst Particles by Strong Metal-Support Bonding [J].
Farmer, Jason A. ;
Campbell, Charles T. .
SCIENCE, 2010, 329 (5994) :933-936
[10]   Oxygen vacancies in transition metal and rare earth oxides: Current state of understanding and remaining challenges [J].
Ganduglia-Pirovano, M. Veronica ;
Hofmann, Alexander ;
Sauer, Joachim .
SURFACE SCIENCE REPORTS, 2007, 62 (06) :219-270