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Cucurbit[6]uril@MIL-101-Cl: loading polar porous cages in mesoporous stable host for enhanced SO2 adsorption at low pressures
Nanoscale ( IF 5.8 ) Pub Date : 2021-09-07 , DOI: 10.1039/d1nr04432j
Yangyang Sun 1 , Jun Liang 1, 2 , Philipp Brandt 1 , Alex Spieß 1 , Secil Öztürk 1 , Christoph Janiak 1, 2
Affiliation  

The robust cucurbituril-MOF composite CB6@MIL-101-Cl was synthesized by a wet impregnation method and a concomitant OH-to-Cl ligand exchange {CB6 = cucurbit[6]uril, 31 wt% content in the composite, MIL-101-Cl = [Cr3(O)Cl(H2O)2(BDC)3], BDC = benzene-1,4-dicarboxylate}. MIL-101-Cl was formed postsynthetically from standard fluorine-free MIL-101 where Cr-OH ligands were substituted by Cl during treatment with HCl. CB6@MIL-101-Cl combines the strong SO2 affinity of the rigid CB6 macrocycles and the high SO2 uptake capacity of MIL-101, and shows a high SO2 uptake of 438 cm3 g−1 (19.5 mmol g−1) at 1 bar and 293 K (380 cm3 g−1, 17.0 mmol g−1 at 1 bar and 298 K). The captured SO2 amount is 2.2 mmol g−1 for CB6@MIL-101-Cl at 0.01 bar and 293 K (2.0 mmol g−1 at 298 K), which is three times higher than that of the parent MIL-101 (0.7 mmol g−1) under the same conditions. The near zero-coverage SO2 adsorption enthalpies of MIL-101 and CB6@MIL-101-Cl are −35 kJ mol−1 and −50 kJ mol−1, respectively, reflecting the impact of the incorporated CB6 macrocycles, having higher affinity towards SO2. FT-IR spectroscopy confirms the interactions of the SO2 with the cucurbit[6]uril moieties of the CB6@MIL-101-Cl composite and SO2 retention for a few minutes under ambient air. Comparative experiments demonstrated loss of crystallinity and porosity after dry SO2 adsorption for MIL-101, while CB6@MIL-101-Cl exhibits nearly complete retention of crystallinity and porosity under the exposure to both dry and wet SO2. Thus, CB6@MIL-101-Cl can be an attractive adsorbent for SO2 capture because of its excellent recycling stability, high capacity and strong affinity toward SO2 at low pressure.

中文翻译:

Cucurbit[6]uril@MIL-101-Cl:在介孔稳定宿主中加载极性多孔笼以增强低压下的 SO2 吸附

坚固的葫芦脲-MOF复合材料CB6@MIL-101-Cl是通过湿浸渍法和伴随的OH-to-Cl配体交换{CB6 =葫芦脲[6]脲,复合材料中的31wt%含量合成的,MIL-101 -Cl = [Cr 3 (O)Cl(H 2 O) 2 (BDC) 3 ],BDC = 苯-1,4-二羧酸酯}。MIL-101-Cl 是从标准的无氟 MIL-101 合成后形成的,其中 Cr-OH 配体在用 HCl 处理期间被 Cl 取代。CB6 @ MIL-101-CL结合了强SO 2刚性CB6大环化合物的亲合性和高SO 2 MIL-101的吸收能力,并且显示出高的SO 2吸收438厘米3-1(19.5毫摩尔克-1) 在 1 bar 和 293 K(380 cm 3 g -1,17.0 mmol g -1在 1 bar 和 298 K)。CB6@MIL-101-Cl 在 0.01 bar 和 293 K(2.0 mmol g -1在 298 K)下捕获的 SO 2量为 2.2 mmol g -1,是母体 MIL-101 的三倍( 0.7 mmol g -1 ) 在相同条件下。MIL-101和CB6@MIL-101-Cl的接近零覆盖SO 2吸附焓分别为-35 kJ mol -1和-50 kJ mol -1,反映了掺入CB6大环的影响,具有更高的亲和力对 SO 2。FT-IR 光谱证实了 SO 的相互作用2与 CB6@MIL-101-Cl 复合材料的葫芦 [6] uril 部分和 SO 2在环境空气下保留几分钟。对比实验表明,MIL-101在干燥 SO 2吸附后结晶度和孔隙率下降,而 CB6@MIL-101-Cl 在暴露于干和湿 SO 2下几乎完全保持结晶度和孔隙率。因此,CB6@MIL-101-Cl因其优异的循环稳定性、高容量和在低压下对 SO 2 的强亲和力而成为一种有吸引力的 SO 2捕获吸附剂。
更新日期:2021-09-15
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