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通过调整沸石中的微环境增强Cu(I)的抗氧化性以实现高效吸附脱硫

Enhancing oxidation resistance of Cu(I) by tailoring microenvironment in zeolites for efficient adsorptive desulfurization.

作者信息

Li Yu-Xia, Shen Jia-Xin, Peng Song-Song, Zhang Jun-Kai, Wu Jie, Liu Xiao-Qin, Sun Lin-Bing

机构信息

State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering, Nanjing Tech University, 30 South Puzhu Road, 211816, Nanjing, China.

出版信息

Nat Commun. 2020 Jun 25;11(1):3206. doi: 10.1038/s41467-020-17042-6.

DOI:10.1038/s41467-020-17042-6
PMID:32587404
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7316705/
Abstract

The zeolite Cu(I)Y is promising for adsorptive removal of thiophenic sulfur compounds from transportation fuels. However, its application is seriously hindered by the instability of Cu(I), which is easily oxidized to Cu(II) even under atmospheric environment due to the coexistence of moisture and oxygen. Here, we report the adjustment of zeolite microenvironment from hydrophilic to superhydrophobic status by coating polydimethylsiloxane (yielding Cu(I)Y@P), which isolates moisture entering the pores and subsequently stabilizes Cu(I) despite the presence of oxygen. Cu(I) in Cu(I)Y@P is stable upon exposure to humid atmosphere for 6 months, while almost all Cu(I) is oxidized to Cu(II) in Cu(I)Y for only 2 weeks. The optimized Cu(I)Y@P material after moisture exposure can remove 532 μmol g of thiophene and is much superior to Cu(I)Y (116 μmol g), regardless of similar uptakes for unexposed adsorbents. Remarkably, Cu(I)Y@P shows excellent adsorption capacity of desulfurization for water-containing model fuel.

摘要

沸石Cu(I)Y有望用于从运输燃料中吸附去除噻吩类含硫化合物。然而,其应用受到Cu(I)不稳定性的严重阻碍,由于水分和氧气的共存,即使在大气环境下Cu(I)也容易被氧化为Cu(II)。在此,我们报道了通过涂覆聚二甲基硅氧烷(得到Cu(I)Y@P)将沸石微环境从亲水性调整为超疏水性状态,这可隔绝进入孔道的水分,进而在有氧存在的情况下使Cu(I)稳定。Cu(I)Y@P中的Cu(I)在潮湿大气中暴露6个月仍保持稳定,而Cu(I)Y中的几乎所有Cu(I)在仅2周内就被氧化为Cu(II)。暴露于湿气后的优化Cu(I)Y@P材料可去除532 μmol g的噻吩,无论未暴露的吸附剂的吸附量相似与否,其性能都远优于Cu(I)Y(116 μmol g)。值得注意的是,Cu(I)Y@P对含水模型燃料显示出优异的脱硫吸附容量。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/01b7/7316705/7dbc05f984ab/41467_2020_17042_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/01b7/7316705/c6f92b5b6b9b/41467_2020_17042_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/01b7/7316705/51646d022307/41467_2020_17042_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/01b7/7316705/ee40b879b431/41467_2020_17042_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/01b7/7316705/7dbc05f984ab/41467_2020_17042_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/01b7/7316705/c6f92b5b6b9b/41467_2020_17042_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/01b7/7316705/51646d022307/41467_2020_17042_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/01b7/7316705/ee40b879b431/41467_2020_17042_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/01b7/7316705/7dbc05f984ab/41467_2020_17042_Fig4_HTML.jpg

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