金属有机骨架
锆
吸附
吸附剂
硫黄
材料科学
分子
金属
非弹性中子散射
化学
化学工程
无机化学
物理化学
中子散射
散射
有机化学
工程类
物理
光学
作者
Jiangnan Li,Gemma L. Smith,Yinlin Chen,Yujie Ma,Meredydd Kippax-Jones,Mengtian Fan,Wanpeng Lu,Mark D. Frogley,Gianfelice Cinque,Sarah Day,Stephen P. Thompson,Yongqiang Cheng,Luke L. Daemen,Anibal J. Ramírez-Cuesta,Martin Schröder,Sihai Yang
标识
DOI:10.1002/anie.202207259
摘要
We report reversible high capacity adsorption of SO2 in robust Zr-based metal-organic framework (MOF) materials. Zr-bptc (H4 bptc=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.
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