In situ synchrotron IR microspectroscopy of CO2 adsorption on single crystals of the functionalized MOF Sc2(BDC-NH2)3.
In situ synchrotron IR microspectroscopy of CO2 adsorption on single crystals of the functionalized MOF Sc2(BDC-NH2)3.
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DOI：
10.1002/anie.201408369
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发表时间：
2014-12-01
期刊：
影响因子：
--
通讯作者：
Wright PA
中科院分区：
文献类型：
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作者：
Greenaway A;Gonzalez-Santiago B;Donaldson PM;Frogley MD;Cinque G;Sotelo J;Moggach S;Shiko E;Brandani S;Howe RF;Wright PA
同步辐射（SR）红外显微光谱学已经能够确定的热力学，动力学和分子取向的CO2吸附在单一微晶的功能化金属有机框架（MOF）的条件下，从烟道气中的碳捕获。 在298-373 K、分压为0.025-0.2 bar的CO2吸收过程中研究了具有明确晶形的小孔MOF单晶Sc2（BDC-NH 2）3（BDC-NH 2 =2-氨基-1，4-苯二甲酸酯）。 从单个单晶确定的吸附的焓和扩散系数是一致的，从散装样品的测量获得的值。明亮的SR IR光源允许快速收集偏振光谱。 在不同取向的晶体相对于偏振的IR光的NH 2基团的MOF和吸附的CO2的不对称拉伸的对称拉伸的吸光度的强烈变化表明，CO2分子排列沿着在MOF的通道。
Synchrotron radiation (SR) IR microspectroscopy has enabled determination of the thermodynamics, kinetics, and molecular orientation of CO2 adsorbed in single microcrystals of a functionalized metal–organic framework (MOF) under conditions relevant to carbon capture from flue gases. Single crystals of the small-pore MOF, Sc2(BDC-NH2)3, (BDC-NH2=2-amino-1,4-benzenedicarboxylate), with well-defined crystal form have been investigated during CO2 uptake at partial pressures of 0.025-0.2 bar at 298–373 K. The enthalpy and diffusivity of adsorption determined from individual single crystals are consistent with values obtained from measurements on bulk samples. The brilliant SR IR source permits rapid collection of polarized spectra. Strong variations in absorbance of the symmetric stretch of the NH2 groups of the MOF and the asymmetric stretch of the adsorbed CO2 at different orientations of the crystals relative to the polarized IR light show that CO2 molecules align along channels in the MOF.