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一种用于制备高疏水性MIL-53-Al的金属-羟基基团修饰策略,以在潮湿条件下高效捕获丙酮。

A metal-OH group modification strategy to prepare highly-hydrophobic MIL-53-Al for efficient acetone capture under humid conditions.

作者信息

Shi Jiaqi, Han Rui, Lu Shuangchun, Liu Qingling

机构信息

Tianjin Key Lab of Indoor Air Environmental Quality Control, School of Environmental Science and Technology, Tianjin University, Tianjin 300350, China; State Key Laboratory of Engines, Tianjin University, Tianjin 300350, China.

Tianjin Key Lab of Indoor Air Environmental Quality Control, School of Environmental Science and Technology, Tianjin University, Tianjin 300350, China; State Key Laboratory of Engines, Tianjin University, Tianjin 300350, China.

出版信息

J Environ Sci (China). 2021 Sep;107:111-123. doi: 10.1016/j.jes.2021.01.030. Epub 2021 Feb 13.

Abstract

A series of highly-hydrophobic MIL-53-Al (MIL = Materials of Institut Lavoisier) frameworks synthesized via decoration of the Al-OH groups by alkyl phosphonic acid were developed as adsorbents for removing acetone from humid gas streams. The newly prepared materials were characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscope (SEM), N adsorption-desorption and thermogravimetric analysis (TGA). Their adsorption behaviors toward acetone vapor under dry and wet conditions were studied subsequently. Results showed that alkyl phosphonic acid was successfully grafted into MIL-53-Al skeleton through coordinating interaction with Al generating MIL-53-Al@C (x = 12, 14, 18). The MIL-53-Al@C exhibited similar crystal structure and thermal stability to parent MIL-53-Al. Furthermore, the modified materials showed significantly enhanced hydrophobicity. The water vapor uptake of MIL-53-Al@C decreased by 72.55% at 75% relative humidity (RH). Dynamic adsorption experiments demonstrated that water vapor had almost no effect on the acetone adsorption performance of MIL-53-Al@C. Under the condition of 90% RH, the acetone adsorption capacity of MIL-53-Al@C was 102.98% higher than that of MIL-53-Al. Notably, MIL-53-Al@C presented excellent adsorption reversibility and regeneration performance in 10 adsorption-desorption cycles. Taken together, the strategy of metal-OH group modification is an attractive way to improve the acetone adsorption performance over metal-organic frameworks (MOFs) under humid conditions. Besides, MIL-53-Al@C would be deemed as a promising candidate for capturing acetone in high moisture environment.

摘要

通过用烷基膦酸修饰Al-OH基团合成了一系列高疏水性的MIL-53-Al(MIL = 拉瓦锡研究所材料)骨架,并将其开发为从潮湿气流中去除丙酮的吸附剂。通过X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、扫描电子显微镜(SEM)、N吸附-脱附和热重分析(TGA)对新制备的材料进行了表征。随后研究了它们在干燥和潮湿条件下对丙酮蒸气的吸附行为。结果表明,烷基膦酸通过与Al的配位相互作用成功接枝到MIL-53-Al骨架中,生成MIL-53-Al@C(x = 12、14、18)。MIL-53-Al@C表现出与母体MIL-53-Al相似的晶体结构和热稳定性。此外,改性材料的疏水性显著增强。在75%相对湿度(RH)下,MIL-53-Al@C的水蒸气吸附量降低了72.55%。动态吸附实验表明,水蒸气对MIL-53-Al@C的丙酮吸附性能几乎没有影响。在90%RH条件下,MIL-53-Al@C的丙酮吸附容量比MIL-53-Al高102.98%。值得注意的是,MIL-53-Al@C在10次吸附-脱附循环中表现出优异的吸附可逆性和再生性能。综上所述,金属-OH基团改性策略是在潮湿条件下提高金属有机骨架(MOF)对丙酮吸附性能的一种有吸引力的方法。此外,MIL-53-Al@C将被视为在高湿度环境中捕获丙酮的有前途的候选材料。

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