Regulation of NO uptake in flexible Ru dimer chain compounds with highly electron-donating dopants
Regulation of NO uptake in flexible Ru dimer chain compounds with highly electron-donating dopants
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高给电子掺杂剂对柔性 Ru 二聚体链化合物中 NO 吸收的调节
DOI：
10.1021/acs.inorgchem.6b02349
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发表时间：
2016
期刊：
影响因子：
4.6
通讯作者：
Jun Zhang et al.
中科院分区：
文献类型：
--
作者：
Kouji Taniguchi;Nanami Shito;Hiroki Fukunaga;Hitoshi Miyasaka;Jun Zhang et al.
按需设计用于选择性捕获特定气体分子（包括有毒气体分子如一氧化氮（NO））的多孔框架是分子多孔材料研究领域中非常重要的主题。在这里，我们报告了通过在框架中化学掺杂实现高选择性NO吸附（即，固溶体方法）：高给电子单元[Ru 2（o-OMePhCO2）4]（o-OMePhCO 2-= o-茴香酸酯）被移植到结构灵活的链框架[Ru 2（4-Cl-2-OMePhCO2）4（phz）]（0分; 4-Cl-2-OMePhCO 2-= 4-氯-o-茴香酸酯和phz =吩嗪）得到一系列掺杂化合物，[{Ru 2（4-Cl-2-OMePhCO 2）4}1-x{Ru 2（o-OMePhCO 2）4}x（phz）]（x= 0.34，0.44，0.52，0.70，0.81，0.87），其中[Ru 2（o-OMePhCO 2）4（phz）]（1）asx= 1。最初的化合物1纯粹由“高电子供给单元”制成，但由于其无孔性而没有吸附气体的能力。同时，将具有电子优势的[Ru 2（o-OMePhCO 2）4]单元（x = 0.34-0.52）部分移植到0中，成功地提高了NO在相同结构的柔性骨架中的选择性吸附能力，在95 kPa下的吸附量比原始化合物高1.7-3 mol/[Ru 2]单元（121 K）。固溶体方法是设计有目的的多孔框架的有效手段。
On-demand design of porous frameworks for selective capture of specific gas molecules, including toxic gas molecules such as nitric oxide (NO), is a very important theme in the research field of molecular porous materials. Herein, we report the achievement of highly selective NO adsorption through chemical doping in a framework (i.e., solid solution approach): the highly electron donating unit [Ru2(o-OMePhCO2)4] (o-OMePhCO2–=o-anisate) was transplanted into the structurally flexible chain framework [Ru2(4-Cl-2-OMePhCO2)4(phz)] (0; 4-Cl-2-OMePhCO2–= 4-chloro-o-anisate and phz = phenazine) to obtain a series of doped compounds, [{Ru2(4-Cl-2-OMePhCO2)4}1–x{Ru2(o-OMePhCO2)4}x(phz)] (x= 0.34, 0.44, 0.52, 0.70, 0.81, 0.87), with [Ru2(o-OMePhCO2)4(phz)] (1) asx= 1. The original compound1was made purely from a “highly electron donating unit” but had no adsorption capability for gases because of its nonporosity. Meanwhile, the partial transplant of the electronically advantageous [Ru2(o-OMePhCO2)4] unit withx= 0.34–0.52 in0successfully enhanced the selective adsorption capability of NO in an identical structurally flexible framework; an uptake at 95 kPa that was 1.7–3 mol/[Ru2] unit higher than that of the original0compound was achieved (121 K). The solid solution approach is an efficient means of designing purposeful porous frameworks.