Stepwise Synthesis of Robust Metal-Organic Frameworks via Postsynthetic Metathesis and Oxidation of Metal Nodes in a Single-Crystal to Single-Crystal Transformation

被引:241
作者
Liu, Tian-Fu [1 ]
Zou, Lanfang [1 ]
Feng, Dawei [1 ]
Chen, Ying-Pin [1 ]
Fordham, Stephen [1 ]
Wang, Xuan [1 ]
Liu, Yangyang [1 ]
Zhou, Hong-Cai [1 ]
机构
[1] Texas A&M Univ, Dept Chem, College Stn, TX 77842 USA
关键词
GIANT PORES; ADSORPTION; REACTIVITY; SEPARATION; STABILITY; CHEMISTRY; EXCHANGE; DESIGN; CO2;
D O I
10.1021/ja5023283
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Utilizing PCN-426-Mg as a template, two robust metal-organic frameworks (MOFs), PCN-426-Fe(III) and PCN-426-Cr(III), have been synthesized through a strategy of postsynthetic metathesis and oxidation (PSMO) of the metal nodes step by step. The frameworks remained in their single crystal form throughout. Furthermore, the stability and porosity of the frameworks were significantly improved after PSMO. By taking advantage of both the kinetically labile metal-ligand exchange reactions prior to oxidation and the kinetically inert metal-ligand bonds after oxidation, robust MOFs, which would otherwise be difficult to synthesize, can be readily prepared.
引用
收藏
页码:7813 / 7816
页数:4
相关论文
共 42 条
[1]   [VIII(H2O)]3O(O2CC6H4CO2)3•(Cl, 9H2O) (MIL-59):: a rare example of vanadocarboxylate with a magnetically frustrated three-dimensional hybrid framework [J].
Barthelet, K ;
Riou, D ;
Férey, G .
CHEMICAL COMMUNICATIONS, 2002, (14) :1492-1493
[2]  
Base C.F., 1976, The hydrolysis of cations
[3]   Hydrocarbon Separations in a Metal-Organic Framework with Open Iron(II) Coordination Sites [J].
Bloch, Eric D. ;
Queen, Wendy L. ;
Krishna, Rajamani ;
Zadrozny, Joseph M. ;
Brown, Craig M. ;
Long, Jeffrey R. .
SCIENCE, 2012, 335 (6076) :1606-1610
[4]   High capacity CO2 adsorption in a Mg(II)-based phosphine oxide coordination material [J].
Bohnsack, Alisha M. ;
Ibarra, Ilich A. ;
Hatfield, Peter W. ;
Yoon, Ji Woong ;
Hwang, Young Kyu ;
Chang, Jong-San ;
Humphrey, Simon M. .
CHEMICAL COMMUNICATIONS, 2011, 47 (17) :4899-4901
[5]   Ti3+-, V2+/3+-, Cr2+/3+-, Mn2+-, and Fe2+-Substituted MOF-5 and Redox Reactivity in Cr- and Fe-MOF-5 [J].
Brozek, Carl K. ;
Dinca, Mircea .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2013, 135 (34) :12886-12891
[6]   Quantification of Site-Specific Cation Exchange in Metal-Organic Frameworks Using Multi-Wavelength Anomalous X-ray Dispersion [J].
Brozek, Carl K. ;
Cozzolino, Anthony F. ;
Teat, Simon J. ;
Chen, Yu-Sheng ;
Dinca, Mircea .
CHEMISTRY OF MATERIALS, 2013, 25 (15) :2998-3002
[7]  
Burgess J., 1978, Metal ions in solution, P264
[8]   A new zirconium inorganic building brick forming metal organic frameworks with exceptional stability [J].
Cavka, Jasmina Hafizovic ;
Jakobsen, Soren ;
Olsbye, Unni ;
Guillou, Nathalie ;
Lamberti, Carlo ;
Bordiga, Silvia ;
Lillerud, Karl Petter .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (42) :13850-13851
[9]   High-enthalpy hydrogen adsorption in cation-exchanged variants of the microporous metal-organic framework Mn3[(Mn4Cl)3(BTT)8(CH3OH)10]2 [J].
Dinca, Mircea ;
Long, Jeffrey R. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (36) :11172-11176
[10]  
EIGEN M, 1963, PURE APPL CHEM, V6, P105