Highly Dispersed HKUST-1 on Milimeter-Sized Mesoporous γ-Al2O3 Beads for Highly Effective Adsorptive Desulfurization
Highly Dispersed HKUST-1 on Milimeter-Sized Mesoporous γ-Al2O3 Beads for Highly Effective Adsorptive Desulfurization
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毫米级介孔 γ-Al2O3 珠上高度分散的 HKUST-1 用于高效吸附脱硫
DOI：
10.1021/acs.iecr.6b01001
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发表时间：
2016-07-13
影响因子：
4.2
通讯作者：
Mu, Cuncun
中科院分区：
文献类型：
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作者：
Qin, Libo;Zhou, Yunshan;Mu, Cuncun
在水热条件下，将HKUST-1有效地浸渍在毫米级介孔γ-Al 2 O3微球上，形成了高比表面积、机械强度、化学稳定性和热稳定性显著提高、成本低廉的复合材料HKUST-1@ γ-Al 2 O3。该复合材料表现出优异的性能与吸附脱硫容量为59.7 mg S/g MOF（与裸HKUST-1的49.1 mg S/g MOF）的二苯并噻吩（初始硫含量为1000 ppmwS）和正辛烷组成的模型油。实验结果还表明，HKUST-1@ gamma-Al 2 O3可以降低35 ppmwS的硫含量低于9.6 ppmwS的模型油在HKUST-1@ gamma-Al 2 O3的比例超过30重量%，表明深度吸附脱硫的有效性。HKUST-1@ gamma-Al_2 O_3吸附DBT的吉布斯自由能小于HKUST-1，这是由于HKUST-1在gamma-Al_2 O_3通道/孔的受限环境下形成的纳米颗粒有效地利用了活性中心、较短的扩散通道和较大的比表面积。值得注意的是，使用后的HKUST-1@ γ-Al_2 O_3珠可以很容易地通过丙酮洗涤再生，并且吸附脱硫容量在经历5次循环后仅略有下降。结果表明，HKUST-1@ gamma-Al 2 O3微球作为吸附脱硫剂具有很好的应用前景。
HKUST-1 was impregnated effectively on millimeter-sized mesoporous gamma-Al2O3 beads under hydrothermal conditions, resulting in formation of a composite material HKUST-1@gamma-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 ppmwS) and n-octane. Experimental results also revealed that HKUST-1@gamma-Al2O3 could reduce 35 ppmwS sulfur content of the model oil lower than 9.6 ppmwS at a ratio of HKUST-1@gamma-Al2O3 to oil over 30 wt %, indicating effectiveness for deep adsorptive desulfurization. The Gibbs free energy for DBT adsorption by HKUST-1@gamma-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 gamma-Al2O3 channels/pores. Remarkably, the used HKUST-1@gamma-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@gamma-Al2O3 beads have great potential as an adsorbent for adsorptive desulfurization in practical applications.