Acid-Base Bifunctional Periodic Mesoporous Metal Phosphonates for Synergistically and Heterogeneously Catalyzing CO2 Conversion

被引:85
作者
Ma, Tian Yi [1 ]
Qiao, Shi Zhang [1 ]
机构
[1] Univ Adelaide, Sch Chem Engn, Adelaide, SA 5005, Australia
来源
ACS CATALYSIS | 2014年 / 4卷 / 11期
基金
澳大利亚研究理事会;
关键词
phosphonate; bifunction; synergistic effect; heterogeneous catalysis; Co-2; conversion; ORGANIC FRAMEWORK; CARBON-DIOXIDE; ADSORPTION PROPERTIES; SELECTIVE SYNTHESIS; TITANIUM PHOSPHATE; AZIRIDINES; EFFICIENT; CATALYSTS; AMINE; SILICA;
D O I
10.1021/cs501124d
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
Integrating multiple functions into one host for improved catalytic performance is challenging and promising for both catalysis and material science. Herein a new acidbase bifunctional periodic mesoporous titanium phosphonate hybrid material is synthesized by a facile one-pot hydrothermal method, using alendronate sodium trihydrate as a coupling molecule. The new material possesses highly periodic mesopores with a large specific surface area of 540 m(2) g(-1) and pore volume of 0.43 cm(3) g(-1), favoring the smooth mass transport of reactants and products during the catalytic reaction. It also has an organicinorganic hybrid framework with homogeneously incorporated phosphonate groups, in which a large number of accessible acidic POH and basic -NH2 sites can, respectively, activate aziridine and CO2, synergistically leading to the high conversion (>99%), yield (98%), and regioselectivity (98:2) for the CO2 cycloaddition reaction. The catalytic activity is better than that of the scarcely reported heterogeneous catalysts for aziridine and CO2 cycloaddition and even comparable to that of the state-of-the-art homogeneous ones. Moreover, being superior to the other catalysts, the metal phosphonate materials can be easily separated and reused repeatedly without activity loss, and no hazardous halogen ions, organic solvents, or cocatalysts are needed for the catalytic process. In comparison with previously reported multifunctional catalysts synthesized by complicated multistep fabrications, the facile one-pot preparation of mesoporous metal phosphonates with dual active sites makes it more practical for high-performance heterogeneous catalysis.
引用
收藏
页码:3847 / 3855
页数:9
相关论文
共 56 条
[1]   High and Selective CO2 Uptake in a Cobalt Adeninate Metal-Organic Framework Exhibiting Pyrimidine- and Amino-Decorated Pores [J].
An, Jihyun ;
Geib, Steven J. ;
Rosi, Nathaniel L. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (01) :38-+
[2]   Designed Catalysts from Pt Nanoparticles Supported on Macroporous Oxides for Selective Isomerization of n-Hexane [J].
An, Kwangjin ;
Alayoglu, Selim ;
Musselwhite, Nathan ;
Na, Kyungsu ;
Somorjai, Gabor A. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (19) :6830-6833
[3]   Frontiers, Opportunities, and Challenges in Biochemical and Chemical Catalysis of CO2 Fixation [J].
Appel, Aaron M. ;
Bercaw, John E. ;
Bocarsly, Andrew B. ;
Dobbek, Holger ;
DuBois, Daniel L. ;
Dupuis, Michel ;
Ferry, James G. ;
Fujita, Etsuko ;
Hille, Russ ;
Kenis, Paul J. A. ;
Kerfeld, Cheal A. ;
Morris, Robert H. ;
Peden, Charles H. F. ;
Portis, Archie R. ;
Ragsdale, Stephen W. ;
Rauchfuss, Thomas B. ;
Reek, Joost N. H. ;
Seefeldt, Lance C. ;
Thauer, Rudolf K. ;
Waldrop, Grover L. .
CHEMICAL REVIEWS, 2013, 113 (08) :6621-6658
[4]   Mesoporous titanium phosphate molecular sieves with ion-exchange capacity [J].
Bhaumik, A ;
Inagaki, S .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2001, 123 (04) :691-696
[5]   KINETICS OF CARBAMATE FORMATION AND BREAKDOWN [J].
CAPLOW, M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1968, 90 (24) :6795-&
[6]   Synthesis of Hierarchical Sn-MFI as Lewis Acid Catalysts for Isomerization of Cellulosic Sugars [J].
Cho, Hong Je ;
Dornath, Paul ;
Fan, Wei .
ACS CATALYSIS, 2014, 4 (06) :2029-2037
[7]   Tuning the Adsorption Properties of Isoreticular Pyrazolate-Based Metal-Organic Frameworks through Ligand Modification [J].
Colombo, Valentina ;
Montoro, Carmen ;
Maspero, Angelo ;
Palmisano, Giovanni ;
Masciocchi, Norberto ;
Galli, Simona ;
Barea, Elisa ;
Navarro, Jorge A. R. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (30) :12830-12843
[8]   Mesostructured Hybrid Organic-Silica Materials: Ideal Supports for Well-Defined Heterogeneous Organometallic Catalysts [J].
Conley, Matthew P. ;
Coperet, Christophe ;
Thieuleux, Chloe .
ACS CATALYSIS, 2014, 4 (05) :1458-1469
[9]   An Amine-Functionalized MIL-53 Metal-Organic Framework with Large Separation Power for CO2 and CH4 [J].
Couck, Sarah ;
Denayer, Joeri F. M. ;
Baron, Gino V. ;
Remy, Tom ;
Gascon, Jorge ;
Kapteijn, Freek .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (18) :6326-+
[10]   Sequestering CO2 for Short-Term Storage in MOFs: Copolymer Synthesis with Oxiranes [J].
Darensbourg, Donald J. ;
Chung, Wan-Chun ;
Wang, Kecheng ;
Zhou, Hong-Cai .
ACS CATALYSIS, 2014, 4 (05) :1511-1515