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环己二胺四乙酸对NiMo/Al2O3催化剂加氢脱硫活性的促进作用
李彦鹏,张婷婷,刘大鹏,刘宾,柴永明,刘晨光
(中国石油大学(华东)化学工程学院,山东青岛 266580)
摘要:
以二苯并噻吩(DBT)为加氢脱硫(HDS)反应模型化合物,研究有机配体环己二胺四乙酸(CyDTA)对NiMo催化剂HDS活性的促进效果,考察不同Mo与有机配体物质的量比以及热处理温度等因素对催化剂HDS活性的影响,以TEM、XPS等表征手段研究CyDTA的促进作用。结果表明:使用CyDTA后可大幅度提高NiMo催化剂的HDS活性与氢解脱硫选择性,其中CyDTA配比(物质的量比)影响最为显著,Mo∶CyDTA=3∶2时kHDS增加约1.15倍; CyDTA的使用会使催化剂中MoS2活性相的平均堆垛层数略有提高,平均片晶长度略有增加,Mo原子暴露率有所降低,但活性位转换频率(TOF)大幅度提高,催化剂活性相的本质发生了变化; CyDTA与Ni助剂存在相互作用,可有效促进Ni助剂对Mo组分的协同效应,增加催化剂中NiMoS活性相的含量,最终大幅提高NiMo催化剂的催化活性。
关键词:  加氢脱硫  NiMo催化剂  环己二胺四乙酸  活性相
DOI:10.3969/j.issn.1673-5005.2019.06.018
分类号::TE 624.43
文献标识码:A
基金项目:山东省自然科学基金项目(ZR2017MB031);中央高校基本科研业务费专项(17CX02051)
Effect of cyclohexanediamine tetraacetic acid on hydrodesulfurization performance of NiMo/Al2O3 catalyst
LI Yanpeng, ZHANG Tingting, LIU Dapeng, LIU Bin, CHAI Yongming, LIU Chenguang
(College of Chemical Engneering in China University of Petroleum(East China), Qingdao 266580, China)
Abstract:
The effect of cyclohexanediamine tetraacetic acid (CyDTA) on the hydrodesulfurization (HDS) performance of NiMo/Al2O3 catalyst was studied using dibenzothiophene (DBT) as model compound for HDS evaluation. The influence of molar ratio of Mo:CyDTA and heat treatment temperature on the HDS were investigated, and TEM and XPS were applied to interpret the promotion effect of CyDTA on NiMo catalyst. Evaluation results prove that the CyDTA could significantly increase the HDS activity as well as the direct-desulfurization selectivity of NiMo catalyst, and the molar ratio of Mo:CyDTA affects the most. The kHDS could be increased by 1.15 times with Mo∶CyDTA of 3∶2. The CyDTA could lead to a small increase of mean stacking number of MoS2 active phase, meanwhile the mean slab length is also increased thus the dispersion of MoS2 phase is declined. However the turnover frequency (TOF) of the active sites is substantially increased, which indicates that the nature of active phase might be changed. It is also found that there is interaction between CyDTA and Ni promotor, facilitating the synergy effect between Ni promoter and active MoS2 phase. Thus the concentration of active NiMoS phase could be promoted and finally the HDS performance of NiMo catalyst could be enhanced.
Key words:  hydrodesulfurization  NiMo catalysts  CyDTA  active phase
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