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What Matters to the Adsorptive Desulfurization Performance of Metal-Organic Frameworks?
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2015-09-15 00:00:00 , DOI: 10.1021/acs.jpcc.5b07546
Yu-Xia Li 1 , Wen-Juan Jiang 1 , Peng Tan 1 , Xiao-Qin Liu 1 , Dong-Yuan Zhang 1 , Lin-Bing Sun 1
Affiliation  

Metal–organic frameworks (MOFs) show high potential in adsorptive removal of aromatic sulfur compounds; however, the crucial factors affecting the adsorption performances are scarcely clarified. In the present study, three classic aromatic sulfur compounds (i.e., thiophene, benzothiophene, and 4,6-dimethyldibenzothiophene) as well as five typical MOFs (i.e., MOF-5, HKUST-1, MIL-53(Fe), MIL-53(Cr), and MIL-101(Cr)) were selected for study. The adsorptive desulfurization performances of MOFs were investigated by using a fixed-bed adsorption system. In the case of thiophene, the adsorption capacity of MOFs decreases in the order MIL-53(Cr) > HKUST-1 > MOF-5 > MIL-53(Fe) > MIL-101(Cr). For the first time, the adsorbate–adsorbent interaction was examined in detail by using infrared spectra and temperature-programmed desorption. Such an interaction was demonstrated to be the most important factor affecting adsorption performance. When the molecular size of aromatic sulfur compounds is comparable to or smaller than the window diameter of MOFs, the influence of window diameter becomes apparent. It is surprising to find that the adsorbate–adsorbent interaction plays a major role, which is responsible for the poor adsorption performance of MIL-101(Cr) with quite high porosity. Therefore, metal sites and structure that contribute to the adsorbate–adsorbent interaction should be considered to be the most significant factor aiming to develop new MOFs for adsorptive desulfurization.

中文翻译:

有什么事情对金属的吸附脱硫性能-有机骨架?

金属有机骨架(MOF)在吸附去除芳族硫化合物方面显示出很高的潜力。然而,几乎没有阐明影响吸附性能的关键因素。在本研究中,三种经典的芳族硫化合物(即噻吩,苯并噻吩和4,6-二甲基二苯并噻吩)以及五种典型的MOF(即MOF-5,HKUST-1,MIL-53(Fe),MIL-选择53(Cr)和MIL-101(Cr)进行研究。利用固定床吸附系统研究了MOFs的吸附脱硫性能。在噻吩的情况下,MOF的吸附能力按MIL-53(Cr)> HKUST-1> MOF-5> MIL-53(Fe)> MIL-101(Cr)的顺序降低。首次使用红外光谱和程序升温脱附技术对吸附物与吸附剂之间的相互作用进行了详细研究。事实证明,这种相互作用是影响吸附性能的最重要因素。当芳族硫化合物的分子大小等于或小于MOF的窗口直径时,窗口直径的影响变得明显。令人惊讶地发现,吸附物与吸附剂的相互作用起主要作用,这是导致孔隙率很高的MIL-101(Cr)吸附性能差的原因。因此,有助于吸附剂-吸附剂相互作用的金属位点和结构应被视为旨在开发用于吸附脱硫的新型MOF的最重要因素。当芳族硫化合物的分子大小等于或小于MOF的窗口直径时,窗口直径的影响变得明显。令人惊讶地发现,吸附物与吸附剂的相互作用起主要作用,这是导致孔隙率很高的MIL-101(Cr)吸附性能差的原因。因此,有助于吸附剂-吸附剂相互作用的金属位点和结构应被视为旨在开发用于吸附脱硫的新型MOF的最重要因素。当芳族硫化合物的分子大小等于或小于MOF的窗口直径时,窗口直径的影响变得明显。令人惊讶地发现,吸附物与吸附剂的相互作用起主要作用,这是导致孔隙率很高的MIL-101(Cr)吸附性能差的原因。因此,有助于吸附剂-吸附剂相互作用的金属位点和结构应被视为旨在开发用于吸附脱硫的新型MOF的最重要因素。
更新日期:2015-09-15
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