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Effects of toluene on thiophene adsorption over NaY and Ce(IV)Y zeolites

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Journal of Natural Gas Chemistry 2012年第4期21卷 421-425页

作者： Yanchun Shi Xiaojian Yang Fuping Tian Cuiying Jia Yongying Chen School of Chemistry&State Key Laboratory of Fine Chemicals Dalian University of TechnologyDalian 116024LiaoningChina

Zeolites NaY and Ce（IV）Y were employed as adsorbents to remove organic sulfur compounds from model gasoline （MG） solutions with and without toluene in static adsorption experiments at room temperature （RT） and atmospheric pressure. The adsorbents were characterized by XRD, XRF and pyridine infrared spectrum （IR）. The adsorption experiments show that the desulfurization performance of Ce（IV）Y is much better than that of NaY. The sulfur removal over both NaY and Ce（IV）Y decreases with the increase of toluene concentration in MG, however, the decline tendency on Ce（IV）Y is smooth, and it is steep on NaY. FT-IR spectra of thiophene adsorption indicate that thiophene molecules are mainly adsorbed on NaY via π electron interaction, but on Ce（IV）Y, in addition to the π electron interaction, both Ce^4＋-S direct interaction and protonation of thiophene also play important roles. Toluene molecules are adsorbed on NaY also via π electron interaction. Although the amount of Bronsted acid sites is increased due to the introduction of Ce^4＋ ions into NaY zeolite, it is not found to influence the adsorption mode of toluene over Ce（IV）Y. Compared with NaY zeolite, the improved desulfurization performance over Ce（IV）Y for removing organic sulfur compounds from MG solution, especially those containing large amount of aromatics, may be ascribed to the direct Ce（IV）-S interaction, which is much resistant to the influence resulted from toluene adsorption.

关键词： toluene Ce(IV)Y adsorption desulfurization thiophene Ce^4+-S interaction

Bio-regeneration of p-complexation desulfurization adsorbents

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Science China Chemistry 2005年第6期48卷 538-544页

作者： LI Wangliang1,2, XING Jianmin1, XIONG Xiaochao1,2, SHAN Guobin1,2 & LIU Huizhou1 1. Laboratory of Separation Science and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100080, China 2. Graduate School of the Chinese Academy of Sciences,Beijing 100039, China 1. Laboratory of Separation Science and Engineering Institute of Process Engineering Chinese Academy of Sciences 100080 Beijing China 2. Graduate School of the Chinese Academy of Sciences 100039 Beijing China

The coupling of adsorption desulfurization and biodesulfurization is a new approach to produce clean fuels. Sulfur compounds are firstly adsorbed on adsorbents, and then the ad-sorbents are regenerated by microbial conversion. p-Complexation adsorbent, Cu(I)-Y, was ob-tained by ion exchanging Y-type zeolite with Cu2+ and then by auto-reduction in helium at 450℃ for 3 h. Dibenzothiophene (DBT) was used as a model compound. The effects of cell concentra-tion, volume of oil phase, the ratio of aqueous phase to adsorbent on DBT desorption by a bac-terium were studied. The amounts of DBT desorbed and 2-HBP produced can be apparently increased with addition of n-octane. BDS activity can be improved by increasing cell concentra-tion and the ratio of water-to-adsorbent. 89% of DBT desorbed from the adsorbents can be converted to 2-HBP within 6 h and almost 100% within 24 h, when the volume ratio of oil-to-water was 1/5 mL/mL, the cell concentration was 60 g·L?1, and the ratio of adsorbent-to-oil was 0.03 g·mL?1. The amount of 2-HBP produced was strongly dependent on the volume ratio of oil-to- water, cell concentration and amount of adsorbent. adsorption capacity of the regenerated ad-sorbent is 95% that of the fresh one after being desorbed with Pseudomonas delafieldii R-8, washed with n-octane, dried at 100℃ for 24 h and auto-reduced in He.

关键词： adsorption desulfurization p-complexation adsorbents bio-regeneration Pseudomonas delafieldii desorption.

Ultra-deep adsorptive removal of thiophenic sulfur compounds from FCC gasoline over the specific active sites of CeHY zeolite

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Journal of Energy Chemistry 2019年第12期28卷 256-267页

作者： Yun Zu Chang Zhang Yucai Qin Xiaotong Zhang Li Zhang Honghai Liu Xionghou Gao Lijuan Song College of Chemistry and Chemical Engineering China University of Petroleum(East China)Qingdao 266555ShandongChina Key Laboratory of Petrochemical Catalytic Science and Technology Liaoning Shihua UniversityFushun 113001LiaoningChina Lanzhou Petrochemical Research Center Petrochemical Research InstitutePetro China Company LimitedLanzhou 730060GansuChina

adsorption desulfurization performance of Na Y,HY and Ce HY zeolites is evaluated in a miniature fixedbed flow by model gasoline containing with thiophene,tetrahydrothiophene,2-methylthiophene,benzothiophene or mixed sulfur *** structural properties of adsorbents are characterized by XRD,N2-adsorption and XPS *** desulfurization mechanisms of these sulfur compounds over the specific active sites of adsorbents as a major focus of this work,have been systematically investigated by using in situ FT-IR spectroscopy with single and double probing *** experimental results show that the Ce HY adsorbent exhibits superior adsorption sulfur capacity at breakthrough point of zero sulfur for ultra-deep removal of each thiophenic sulfur compound,especially in the capture of aromatic 2-methylthiophene(about ca.28.6 mgS/gadsorbent).The results of in situ FT-IR with single probing molecule demonstrate an important finding that high oligomerization ability of thiophene or 2-methylthiophene on the CeHY can promote the breakthrough adsorption sulfur capacity,mainly resulting from the synergy between Br?nsted acid sites and Ce(III)hydroxylated species active sites located in the supercages of Ce ***,the result of in situ FT-IR with double probing molecules further reveals the essence of oligomerization reactions of thiophene and 2-methylthiophene molecules on those specific active *** contrast,the oligomerization reaction of benzothiophene molecules on the active sites of Ce HY cannot occur due to the restriction of cavity size of supercages,but they can be adsorbed on the Br?nsted acid sites via protonation,and on Ce(III)hydroxylated species and extra-framework aluminum hydroxyls species via direct"S-M"bonding *** to the tetrahydrothiophene,adsorption mechanism is similar to that of benzothiophene,except in the absence of *** paper can provide a new design idea of specific adsorption active sites in

关键词： CeHY zeolite Active sites Thiophenic sulfur compounds adsorption desulfurization Oligomerization ability In situ FT-IR spectroscopy