Structural and Dynamic Analysis of Sulphur Dioxide Adsorption in a Series of Zirconium-Based Metal-Organic Frameworks.
Structural and Dynamic Analysis of Sulphur Dioxide Adsorption in a Series of Zirconium-Based Metal-Organic Frameworks.
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DOI：
10.1002/anie.202207259
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发表时间：
2022-09-05
影响因子：
16.6
通讯作者：
Yang, Sihai
中科院分区：
文献类型：
--
作者：
Li, Jiangnan;Smith, Gemma L.;Chen, Yinlin;Ma, Yujie;Kippax-Jones, Meredydd;Fan, Mengtian;Lu, Wanpeng;Frogley, Mark D.;Cinque, Gianfelice;Day, Sarah J.;Thompson, Stephen P.;Cheng, Yongqiang;Daemen, Luke L.;Ramirez-Cuesta, Anibal J.;Schroder, Martin;Yang, Sihai
我们报告了在坚固的Zr基金属有机框架（MOF）材料中SO2的可逆高容量吸附。Zr‐bptc（H4 bptc =联苯-3，3 ′，5，5 ′-四羧酸）在0.1 bar和298 K下显示出6.2 mmol g−1的高SO2吸收率，反映了优异的捕获能力和在低浓度（2500 ppm）下的SO2去除能力。 动态穿透实验证实，在孔中引入胺、原子分散的CuII或杂原子硫位点可增强低浓度下的SO2捕获。捕获的SO2可以定量转化为药物中间体，芳基N-氨基磺酰胺，从而将废物转化为化学价值。原位X射线衍射、红外显微光谱和非弹性中子散射能够在原子水平上可视化吸附的SO2分子的结合域和这些材料中的主客体结合动力学。孔隙环境的细化在设计高效吸附剂材料中起着关键作用。已经研究了一系列基于Zr的金属-有机骨架材料用于可逆的SO2吸收。原子分散的CuII、胺或杂原子硫位点的掺入增强了低浓度下的SO2吸收。这项工作证实，孔隙环境的控制是一个重要的方法，优化吸附的SO2在低浓度。
We report reversible high capacity adsorption of SO2 in robust Zr‐based metal–organic framework (MOF) materials. Zr‐bptc (H4bptc=biphenyl‐3,3′,5,5′‐tetracarboxylic acid) shows a high SO2 uptake of 6.2 mmol g−1 at 0.1 bar and 298 K, reflecting excellent capture capability and removal of SO2 at low concentration (2500 ppm). Dynamic breakthrough experiments confirm that the introduction of amine, atomically‐dispersed CuII or heteroatomic sulphur sites into the pores enhance the capture of SO2 at low concentrations. The captured SO2 can be converted quantitatively to a pharmaceutical intermediate, aryl N‐aminosulfonamide, thus converting waste to chemical values. In situ X‐ray diffraction, infrared micro‐spectroscopy and inelastic neutron scattering enable the visualisation of the binding domains of adsorbed SO2 molecules and host–guest binding dynamics in these materials at the atomic level. Refinement of the pore environment plays a critical role in designing efficient sorbent materials. A series of Zr‐based metal–organic framework materials have been investigated for reversible SO2 uptake. The incorporation of atomically‐dispersed CuII, amine or heteroatomic sulphur sites enhances the uptake of SO2 at low concentrations. This work confirms that control of pore environments is an important approach for optimising the adsorption of SO2 at low concentrations.
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超刚性金属有机物中客体控制的不相称调制
影响因子：
15
作者：
Li J;Zhou Z;Han X;Zhang X;Yan Y;Li W;Smith GL;Cheng Y;McCormick McPherson LJ;Teat SJ;Frogley MD;Rudić S;Ramirez-Cuesta AJ;Blake AJ;Sun J;Schröder M;Yang S
通讯作者：
Yang S
DOI：
10.1039/c0cc02990d
发表时间：
2010-11-07
期刊：
Chemical communications (Cambridge, England)
影响因子：
--
作者：
Garibay SJ;Cohen SM
通讯作者：
Cohen SM
影响因子：
11.9
作者：
Martinez-Ahumada, Eva;Diaz-Ramirez, Mariana L.;Ibarra, Ilich A.
通讯作者：
Ibarra, Ilich A.
影响因子：
9.5
作者：
Glomb, Sebastian;Woschko, Dennis;Janiak, Christoph
通讯作者：
Janiak, Christoph
影响因子：
15
作者：
Cavka, Jasmina Hafizovic;Jakobsen, Soren;Lillerud, Karl Petter
通讯作者：
Lillerud, Karl Petter