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...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(FTIR), scanning electron microscope(SEM), N_(2) 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 Al3+generating MIL-53-Al@C_(x)(x = 12, 14, 18).The MIL-53-Al@C_(x) 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_(14) 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_(14).Under the condition of 90% RH, the acetone adsorption capacity of MIL-53-Al@C_(14) was 102.98% higher than that of MIL-53-Al.Notably, MIL-53-Al@C_(14) 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_(14) would be deemed as a promising candidate for capturing acetone in high moisture environment.展开更多
基金supported by the National Key R&D Program of China(Nos.2016YFC0205300,2019YFC1904100 and 2019YFC1904102)the National Engineering Laboratory for Mobile Source Emission Control Technology of China(No.NELMS2017A03)+2 种基金the Natural National Science Foundation of China(Nos.21503144 and 21690083)the Tianjin Research Program of Ecological Environmental Treatment(Nos.18ZXSZSF00210 and 18ZXSZSF00060)the Tianjin Research Program of Application Foundation and Advanced Technique(No.16JCQNJC05400)。
文摘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(FTIR), scanning electron microscope(SEM), N_(2) 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 Al3+generating MIL-53-Al@C_(x)(x = 12, 14, 18).The MIL-53-Al@C_(x) 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_(14) 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_(14).Under the condition of 90% RH, the acetone adsorption capacity of MIL-53-Al@C_(14) was 102.98% higher than that of MIL-53-Al.Notably, MIL-53-Al@C_(14) 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_(14) would be deemed as a promising candidate for capturing acetone in high moisture environment.