Density Gradation of Open Metal Sites in the Mesospace of Porous Coordination Polymers
Density Gradation of Open Metal Sites in the Mesospace of Porous Coordination Polymers
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多孔配位聚合物介观空间中开放金属位点的密度分级
DOI：
10.1021/jacs.7b05702
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发表时间：
2017-08-23
影响因子：
15
通讯作者：
Kitagawa, Susumu
中科院分区：
文献类型：
--
作者：
Duan, Jingui;Higuchi, Masakazu;Kitagawa, Susumu
实验和理论网格化学研究表明，以致密的开放金属中心(OMS)为特征的介孔配位聚合物(Meso-PCP)的凝聚相、互穿和脆性的普遍存在，对其制备提出了严格的限制。在这里，我们提出了一种稳定的高孔率介孔分子筛的合理设计，使用了低对称性的配体和最短的连接物甲酸。由此得到的二聚体除尘器(PCP-31和PCP-32)具有高比表面积、超高孔隙率和高OMS导数(分别为3.76和3.29nmolg(-1))，通过结合能(BE)和静电势(ESP)计算证实，在298K下能够高选择性地有效地从C2H2/CO2混合物中分离C2H2。
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.