过渡金属改性Y型分子筛吸附脱除低碳烃中二甲基二硫醚

doi:10.16085/j.issn.1000-6613.2017.06.032

化工进展 ›› 2017, Vol. 36 ›› Issue (06): 2190-2196.DOI: 10.16085/j.issn.1000-6613.2017.06.032

过渡金属改性Y型分子筛吸附脱除低碳烃中二甲基二硫醚

赵亚伟, 沈本贤, 孙辉, 詹国雄, 侯柯

华东理工大学化工学院石油加工研究所, 上海 200237

收稿日期:2016-11-08 修回日期:2017-02-07 出版日期:2017-06-05 发布日期:2017-06-05
通讯作者: 孙辉
作者简介:赵亚伟(1989—),男,博士研究生,研究方向为油品清洁化。E-mail:zhaoyawei1113@163.com。
基金资助:
中央高校基本科研业务费专项资金（22A201514010）、上海市自然科学基金（16ZR1408100）、国家自然科学基金重大研究计划培育项目（91634112）及化学工程联合国家重点实验室开放课题（SKL-ChE-16C01）项目。

Study on adsorption removal of DMDS from light hydrocarbons using transition metal ions modified Y zeolite

ZHAO Yawei, SHEN Benxian, SUN Hui, ZHAN Guoxiong, HOU Ke

Research Institute of Petroleum Processing, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China

Received:2016-11-08 Revised:2017-02-07 Online:2017-06-05 Published:2017-06-05

摘要/Abstract

摘要： 采用离子交换法制备了CoY、CuY、NiY分子筛，并在固定床吸附器上考察了工艺条件及原料烯烃含量对改性分子筛吸附脱除二甲基二硫醚性能的影响。采用密度泛函理论计算二甲基二硫醚及异丁烯在CoY、CuY、NiY分子筛上的竞争吸附行为。最后考察了高温水蒸气对吸附剂的再生效果。结果表明，CoY、CuY和NiY分子筛对二甲基二硫醚的动态饱和吸附硫容分别为47.5mg/g、36.3mg/g和40.2mg/g；其中CoY和NiY分子筛硫容量受烯烃含量的影响较大，CuY分子筛受影响较小。计算结果表明，吸附过程中S—S键的Mayer键级变化不大，烯烃中C=C键双键性质减弱。二甲基二硫醚在CoY、CuY和NiY分子筛上的吸附能分别为-59.5kJ/mol、-22.2kJ/mol和-30.4kJ/mol，与实验数据吻合。吸附饱和后的分子筛经160℃水蒸气脱附60min后能够有效再生，且多次再生后吸附剂硫容仍保持在新鲜吸附剂的97%以上。

关键词: 脱硫, 烯烃, 竞争吸附, 密度泛函理论

Abstract: CoY,CuY and NiY zeolites were prepared by ion-exchange method. Influences of operation conditions and olefin content on adsorption desulfurization performances were investigated by dynamic adsorption experiments. Adsorption behaviors of dimethyl disulfide(DMDS)and isobutene onto CoY,CuY and NiY zeolites were calculated using density function theory. Saturated adsorbents were regenerated in superheated steam. Results show that adsorption desulfurization capacities of CoY,NiY and CuY are 47.5mg/g、36.3mg/g and 40.2mg/g,respectively,and CoY and NiY were more easily to be influenced by olefin competitive adsorption. The Mayer bond order of S—S is not much changed after adsorption while the double bond property was weakened. The adsorption energies of CoY,CuY and NiY are -59.5kJ/mol,-22.2kJ/mol and -30.4kJ/mol,respectively,which were consistent with the experimental results. Saturated adsorbents could be effectively regenerated in steam at 160℃ for 60min.

Key words: desulfurization, olefin, competitive adsorption, density function theory(DFT)

中图分类号:

TE622

赵亚伟, 沈本贤, 孙辉, 詹国雄, 侯柯. 过渡金属改性Y型分子筛吸附脱除低碳烃中二甲基二硫醚[J]. 化工进展, 2017, 36(06): 2190-2196.

ZHAO Yawei, SHEN Benxian, SUN Hui, ZHAN Guoxiong, HOU Ke. Study on adsorption removal of DMDS from light hydrocarbons using transition metal ions modified Y zeolite[J]. Chemical Industry and Engineering Progress, 2017, 36(06): 2190-2196.

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过渡金属改性Y型分子筛吸附脱除低碳烃中二甲基二硫醚

Study on adsorption removal of DMDS from light hydrocarbons using transition metal ions modified Y zeolite

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