Synthesis of high-crystallinity MIL-125 with outstanding xylene isomer separation performance

doi:10.1016/S1872-2067(21)63905-0

Abstract

Abstract:

MIL-125 is a metal-organic framework with great potential for the adsorption and separation of xylene isomers. However, MIL-125 is usually synthesized under anhydrous and anaerobic conditions. In this study, homogeneously shaped and highly crystalline MIL-125 was synthesized by introducing water-resistant titanium-containing oligomers into the synthesis process. With the assistance of the novel oligomers, MIL-125 can be synthesized in the presence of water, which meets batch-production requirements. The adsorption separation performance of the obtained highly crystalline MIL-125 was also significantly enhanced. The para-xylene/meta-xylene selectivity can reach 13.5 in mesitylene, which is higher than the selectivity values of most previously reported para-selective adsorbents. The MIL-125 xylene separation performance was verified using both batch adsorption and breakthrough experiments in the liquid phase. In addition, the influence of the solvent effect was evaluated through microcalorimetric experiments, liquid-phase adsorption experiments, and theoretical calculations.

Key words: Titanium-containing oligomers, MIL-125, Xylene isomers, Adsorption separation, Solvent effect

Liping Yang, Jiacheng Xing, Danhua Yuan, Lin Li, Yunpeng Xu, Zhongmin Liu. Synthesis of high-crystallinity MIL-125 with outstanding xylene isomer separation performance[J]. Chinese Journal of Catalysis, 2021, 42(12): 2313-2321.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63905-0

https://www.cjcatal.com/EN/Y2021/V42/I12/2313

Figures/Tables 7

Scheme 1. Depiction of the transesterification reaction.

Scheme 2. Schematic diagram of the column breakthrough set-up.

Fig. 1. (a) Synthetic illustration of the Ti-oligomer and MIL-125; TGA (b) and NMR (c) results of the raw materials used in the synthesis of MIL-125.

Fig. 2. XRD patterns and SEM images. (a) XRD patterns of simulated MIL-125 and synthesized MIL-125; (b,c) SEM images of synthesized MIL-125.

Fig. 3. Adsorbent performance tests. (a) Single-component adsorption isotherms of para-xylene (pX) (circles), meta-xylene (mX) (diamonds), and ortho-xylene (oX) (triangles) adsorbing to MIL-125 in mesitylene at 25 °C. (b,c) Binary competitive adsorption isotherms of pX/mX and pX/oX in mesitylene with MIL-125 powder at 25 °C. The uptakes (wt%, g/g) of the equimolar mixtures are shown on the left axis, and the selectivities, (α) are shown on the right axis. (d) Comparison of selectivity for pX/mX versus uptake by para-selective MOFs and molecular sieves.

Fig. 4. Dynamic separation performance. (a) Breakthrough experiments with a binary equimolar pX/mX mixture in mesitylene on a column filled with MIL-125 at a feed flow rate of 1 mL/min at 25 °C. The curves have been corrected for dead volume. (b) One cycle of the breakthrough experiment on the MIL-125 adsorbent column.

Fig. 5. Effect of different solvents on the separation of pX/mX on MIL-125. (a) Microcalorimetry experiment results of the integral dilution heat between different solvents and xylene isomers; (b) Interaction energies of pX/mX with MIL-125 in different solvents indicated by DFT calculations.

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