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Preferential SOx Adsorption in Mg-MOF-74 from a Humid Acid Gas Stream
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-02-03 , DOI: 10.1021/acsami.0c21298 Susan E. Henkelis 1 , Patrick T. Judge 2, 3 , Sophia E. Hayes 2 , Tina M. Nenoff 4
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-02-03 , DOI: 10.1021/acsami.0c21298 Susan E. Henkelis 1 , Patrick T. Judge 2, 3 , Sophia E. Hayes 2 , Tina M. Nenoff 4
Affiliation
The preferential adsorption of SOx versus water in Mg-MOF-74 from a humid SOx gas stream has been investigated via materials studies and nuclear magnetic resonance (NMR). Mg-MOF-74 has been synthesized and subsequently loaded simultaneously with water vapor and SOx (62–96 ppm) in an adsorption chamber at room temperature over a time period of 4 days with a sample taken every 24 h. Each sample was analyzed by powder X-ray diffraction (PXRD), Fourier transform infrared spectroscopy, thermogravimetric analysis (TGA)–mass spectrometry, and scanning electron microscopy–energy-dispersive spectroscopy. The metal–organic framework (MOF) showed retained crystallinity and peak intensity in PXRD, and after 2 days, it showed no obvious degradation to the structure. Use of multiple techniques, including TGA, identified 10% by weight of SOx species, specifically H2S and SO2, within the MOF. 1H solid-state NMR shows a substantial reduction of H2O when SOx is present, which is consistent with SOx preferentially binding to the oxophilic metal site of the framework. After 14 weeks aging, the sulfur remains present in the three-dimensional MOF, with only half being desorbed after 23 weeks in air.
中文翻译:
优惠SO X吸附在Mg的MOF-74从潮湿酸性气体流
通过材料研究和核磁共振(NMR)研究了潮湿的SO x气流中Mg-MOF-74中SO x相对于水的优先吸附。已合成Mg-MOF-74,随后同时装载水蒸气和SO x(62-96 ppm)在室温下于吸附室中放置4天,每24小时取样一次。通过粉末X射线衍射(PXRD),傅立叶变换红外光谱,热重分析(TGA)–质谱和扫描电子显微镜–能量色散光谱对每个样品进行分析。金属有机骨架(MOF)在PXRD中显示出保留的结晶度和峰强度,并且在2天后,没有显示出对结构的明显降解。使用多种技术(包括TGA)可确定MOF中10%重量的SO x物质,特别是H 2 S和SO 2。1 H固态NMR显示,当SO x时,H 2 O大量还原存在SO 3,这与SO x优先结合至框架的亲氧金属位点相一致。老化14周后,硫保留在三维MOF中,在空气中23周后只有一半被解吸。
更新日期:2021-02-17
中文翻译:
优惠SO X吸附在Mg的MOF-74从潮湿酸性气体流
通过材料研究和核磁共振(NMR)研究了潮湿的SO x气流中Mg-MOF-74中SO x相对于水的优先吸附。已合成Mg-MOF-74,随后同时装载水蒸气和SO x(62-96 ppm)在室温下于吸附室中放置4天,每24小时取样一次。通过粉末X射线衍射(PXRD),傅立叶变换红外光谱,热重分析(TGA)–质谱和扫描电子显微镜–能量色散光谱对每个样品进行分析。金属有机骨架(MOF)在PXRD中显示出保留的结晶度和峰强度,并且在2天后,没有显示出对结构的明显降解。使用多种技术(包括TGA)可确定MOF中10%重量的SO x物质,特别是H 2 S和SO 2。1 H固态NMR显示,当SO x时,H 2 O大量还原存在SO 3,这与SO x优先结合至框架的亲氧金属位点相一致。老化14周后,硫保留在三维MOF中,在空气中23周后只有一半被解吸。