Covalent Heme Framework as a Highly Active Heterogeneous Biomimetic Oxidation Catalyst

被引:80
作者
Wang, Xi-Sen [1 ]
Chrzanowski, Matthew [1 ]
Yuan, Daqiang [2 ]
Sweeting, Brandon S. [1 ]
Ma, Shengqian [1 ]
机构
[1] Univ S Florida, Dept Chem, Tampa, FL 33620 USA
[2] Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
关键词
METAL-ORGANIC FRAMEWORKS; POROUS POLYMER NETWORKS; CARBON-DIOXIDE CAPTURE; METALLOPORPHYRIN FRAMEWORKS; PORPHYRIN FRAMEWORK; HIGH-STABILITY; CO2; CAPTURE; ADSORPTION; STORAGE; PHTHALOCYANINE;
D O I
10.1021/cm403860t
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
Although the active centers of many metalloenzymes have been well-studied, the ability for chemists to imitate the iron porphyrin heme found in these enzymes remains a challenge. Herein, we report a water/chemical-stable nanoporous covalent heme framework (CHF-1) that can be synthesized via the Yamamoto homocoupling reaction. Unlike other artificial enzymes, CHF-1 neatly arranges the heme centers to form a graphene-like two-dimensional framework bearing a high surface area (1620 m(2)/g) and high density of active sites. Biomimetic catalytic reactions show that CHF-1 catalyst is an effective heterogeneous catalyst with exceptionally high binding affinities and high catalytic efficiency approaching that of natural heme-based enzymes.
引用
收藏
页码:1639 / 1644
页数:6
相关论文
共 88 条
[1]   ASSEMBLY OF PORPHYRIN BUILDING-BLOCKS INTO NETWORK STRUCTURES WITH LARGE CHANNELS [J].
ABRAHAMS, BF ;
HOSKINS, BF ;
MICHAIL, DM ;
ROBSON, R .
NATURE, 1994, 369 (6483) :727-729
[2]   Zeolite-like metal-organic frameworks as platforms for applications:: On metalloporphyrin-based catalysts [J].
Alkordi, Mohamed H. ;
Liu, Yunling ;
Larsen, Randy W. ;
Eubank, Jarrod F. ;
Eddaoudi, Mohamed .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (38) :12639-+
[3]  
[Anonymous], 2008, ACC MAT STUD REL 5 0
[4]   Targeted Synthesis of a Porous Aromatic Framework with High Stability and Exceptionally High Surface Area [J].
Ben, Teng ;
Ren, Hao ;
Ma, Shengqian ;
Cao, Dapeng ;
Lan, Jianhui ;
Jing, Xiaofei ;
Wang, Wenchuan ;
Xu, Jun ;
Deng, Feng ;
Simmons, Jason M. ;
Qiu, Shilun ;
Zhu, Guangshan .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2009, 48 (50) :9457-9460
[5]   Heme-Like Coordination Chemistry Within Nanoporous Molecular Crystals [J].
Bezzu, C. Grazia ;
Helliwell, Madeleine ;
Warren, John E. ;
Allan, David R. ;
McKeown, Neil B. .
SCIENCE, 2010, 327 (5973) :1627-1630
[6]   Stepwise Synthesis of Metal-Organic Frameworks: Replacement of Structural Organic Linkers [J].
Burnett, Brandon J. ;
Barron, Paul M. ;
Hu, Chunhua ;
Choe, Wonyoung .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2011, 133 (26) :9984-9987
[7]   Highly Efficient Activation of Molecular Oxygen with Nanoporous Metalloporphyrin Frameworks in Heterogeneous Systems [J].
Chen, Long ;
Yang, Yong ;
Guo, Zhaoqi ;
Jiang, Donglin .
ADVANCED MATERIALS, 2011, 23 (28) :3149-+
[8]   CMPs as Scaffolds for Constructing Porous Catalytic Frameworks: A Built-in Heterogeneous Catalyst with High Activity and Selectivity Based on Nanoporous Metalloporphyrin Polymers [J].
Chen, Long ;
Yang, Yong ;
Jiang, Donglin .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (26) :9138-9143
[9]   Biomimetic Catalysis of a Porous Iron-Based Metal-Metalloporphyrin Framework [J].
Chen, Yao ;
Tran Hoang ;
Ma, Shengqian .
INORGANIC CHEMISTRY, 2012, 51 (23) :12600-12602
[10]   Size-Selective Biocatalysis of Myoglobin Immobilized into a Mesoporous Metal-Organic Framework with Hierarchical Pore Sizes [J].
Chen, Yao ;
Lykourinou, Vasiliki ;
Tran Hoang ;
Ming, Li-June ;
Ma, Shengqian .
INORGANIC CHEMISTRY, 2012, 51 (17) :9156-9158