Density Gradation of Open Metal Sites in the Mesospace of Porous Coordination Polymers

被引:132
作者
Duan, Jingui [1 ,2 ]
Higuchi, Masakazu [2 ]
Zheng, Jiajia [2 ,5 ]
Noro, Shin-ichiro [3 ]
Chang, I-Ya [4 ]
Hyeon-Deuk, Kim [4 ]
Mathew, Simon [2 ,7 ]
Kusaka, Shinpei [2 ]
Sivaniah, Easan [2 ]
Matsuda, Ryotaro [2 ]
Sakaki, Shigeyoshi [5 ]
Kitagawa, Susumu [2 ,6 ]
机构
[1] Nanjing Tech Univ, State Key Lab Mat Oriented Chem Engn, Coll Chem Engn, Jiangsu Natl Synerget Innovat Ctr Adv Mat, Nanjing 210009, Jiangsu, Peoples R China
[2] Kyoto Univ, Inst Integrated Cell Mat Sci, Sakyo Ku, Kyoto 6068501, Japan
[3] Hokkaido Univ, Res Inst Elect Sci, Sapporo, Hokkaido 0010020, Japan
[4] Kyoto Univ, Dept Chem, Kyoto 6068502, Japan
[5] Kyoto Univ, Fukui Inst Fundamental Chem, Sakyo Ku, Nishi Hiraki Cho, Kyoto 6068103, Japan
[6] Kyoto Univ, Dept Synthet Chem & Biol Chem, Grad Sch Engn, Nishikyo Ku, Kyoto 6158510, Japan
[7] Univ Amsterdam, Vant Hoff Inst Mol Sci, Sci Pk 904, NL-1098 XH Amsterdam, Netherlands
基金
美国国家科学基金会; 日本科学技术振兴机构;
关键词
EFFECTIVE CORE POTENTIALS; ORGANIC FRAMEWORKS; SEPARATION; C2H2/CO2; STORAGE; SERIES; WATER; UNITS;
D O I
10.1021/jacs.7b05702
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The prevalence of the condensed phase, interpenetration, and fragility of ruesoporous coordination polymers (meso-PCPs) featuring dense open metal sites (OMSs) place strict limitations en their preparation, as revealed by experimental and `theoretical reticular chemistry investigations. Herein, we propose a rational design of stabilized high-porosity meso-PCPs, employing a 'low-symmetry ligand in combination with the shortest linker, formic acid. The resulting dimeric dusters (PCP-31 and PCP-32) exhibit high surface areas, ultrahigh porosities, and high OMS derisities (3.76 and 3.29 nmol g(-1) respectively), enabling highly selective- and effective separation of C2H2 from C2H2/CO2 mixtures at 298 K, as verified by binding energy (BE) and electrostatic potentials (ESP) calculations.
引用
收藏
页码:11576 / 11583
页数:8
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