Highly Dispersed HKUST-1 on Milimeter-Sized Mesoporous γ-Al2O3 Beads for Highly Effective Adsorptive Desulfurization

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• 作者：Libo Qin ; Yunshan Zhou ; Dianqing Li ; Lijuan Zhang ; Zipeng Zhao ; Zareen Zuhra ; Cuncun Mu
• 刊名：Industrial & Engineering Chemistry Research
• 出版年：2016
• 出版时间：July 13, 2016
• 年：2016
• 卷：55
• 期：27
• 页码：7249-7258
• 全文大小：564K
• 年卷期：0
• ISSN：1520-5045

文摘

HKUST-1 was impregnated effectively on millimeter-sized mesoporous γ-Al₂O₃ beads under hydrothermal conditions, resulting in formation of a composite material HKUST-1@γ-Al₂O₃ that features high specific surface area, remarkable enhanced mechanical strength, chemical and thermal stability, and low cost. The composite material exhibited excellent performance with the adsorptive desulfurization capacity of 59.7 mg S/g MOF (versus 49.1 mg S/g MOF for bare HKUST-1) for a model oil composed of dibenzothiophene (with the initial S-content being 1000 ppmw_S) and n-octane. Experimental results also revealed that HKUST-1@γ-Al₂O₃ could reduce 35 ppmw_S sulfur content of the model oil lower than 9.6 ppmw_S at a ratio of HKUST-1@γ-Al₂O₃ to oil over 30 wt %, indicating effectiveness for deep adsorptive desulfurization. The Gibbs free energy for DBT adsorption by HKUST-1@γ-Al₂O₃ was found smaller than that by HKUST-1 due to efficient utilization of active centers, shorter diffusion channels and larger specific surface area of nanosized HKUST-1 particles formed under confined environment of γ-Al₂O₃ channels/pores. Remarkably, the used HKUST-1@γ-Al₂O₃ beads can easily be regenerated by acetone washing and the adsorptive desulfurization capacity just slightly decreased after experiencing five recycles. The results indicate that the as-synthesized HKUST-1@γ-Al₂O₃ beads have great potential as an adsorbent for adsorptive desulfurization in practical applications.