Rational Design and Synthesis of Porous Polymer Networks: Toward High Surface Area

被引:69
作者
Lu, Weigang [1 ]
Wei, Zhangwen [1 ]
Yuan, Daqiang [2 ]
Tian, Jian [1 ]
Fordham, Stephen [1 ]
Zhou, Hong-Cai [1 ]
机构
[1] Texas A&M Univ, Dept Chem, College Stn, TX 77842 USA
[2] Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Peoples R China
基金
美国国家科学基金会;
关键词
METAL-ORGANIC FRAMEWORKS; CARBON-DIOXIDE CAPTURE; HYDROGEN-STORAGE; GAS-STORAGE; METHANE STORAGE; POLY(ARYLENEETHYNYLENE) NETWORKS; INTRINSIC MICROPOROSITY; TORSIONAL BARRIERS; NATURAL-GAS; PHYSISORPTION;
D O I
10.1021/cm501922h
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
Head-on polymerization of tetrahedral monomers inherently imparts interconnected diamond cages to the resulting framework with each strut widely exposed. We have designed and synthesized a series of 3,3',5,5'-tetraethynylbiphenyl monomers, in which the two phenyl rings are progressively locked into a nearly perpendicular position by adding substituents of different size at 2, 2', 6, and 6' positions, as evident from single crystal structures. Computational simulation suggests that these monomers, though not perfectly regular tetrahedra, could still be self-polymerized into three-dimensional frameworks with the same topology. Indeed, five porous polymer networks (PPNs) have been successfully synthesized with these newly designed monomers through Cu(II)-promoted Eglinton homocoupling reaction. Among them, PPN-13 shows exceptionally high Brunauer-Emmett-Teller (BET) surface area of 3420 m(2)/g. The total hydrogen uptake is 52 mg/g at 40 bar and 77 K, and the total methane uptake is 179 mg/g at 65 bar and 298 K.
引用
收藏
页码:4589 / 4597
页数:9
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