B助剂对Ni2P/SBA-15催化剂结构及其加氢脱硫性能的影响

doi:10.3866/PKU.WHXB20110728

物理化学学报 >> 2011, Vol. 27 >> Issue (07): 1737-1742.doi: 10.3866/PKU.WHXB20110728

B助剂对Ni₂P/SBA-15催化剂结构及其加氢脱硫性能的影响

赵鹏飞, 季生福, 魏妮, 马倩, 刘辉, 李成岳

北京化工大学, 化工资源有效利用国家重点实验室, 北京 100029

收稿日期:2010-12-29 修回日期:2011-04-05 发布日期:2011-06-28
通讯作者: 季生福 E-mail:jisf@mail.buct.edu.cn
基金资助:
国家基础研究重大项目计划(973) (2006CB202503)基金资助

Effect of Boron Promoter on the Structure and Hydrodesulfurization Activity of Ni₂P/SBA-15 Catalysts

ZHAO Peng-Fei, JI Sheng-Fu, WEI Ni, MA Qian, LIU Hui, LI Cheng-Yue

State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, P. R. China

Received:2010-12-29 Revised:2011-04-05 Published:2011-06-28
Contact: JI Sheng-Fu E-mail:jisf@mail.buct.edu.cn
Supported by:
The project was supported by the National Key Basic Research Program of China (973) (2006CB202503).

摘要/Abstract

摘要：

以介孔分子筛SBA-15为载体, 磷酸氢二铵为磷源, 硝酸镍为镍源, 硼酸为硼源, 采用共浸渍法制备了B-Ni₂P/SBA-15催化剂前驱体, 然后采用程序升温氢气还原法, 制备了n_P/n_Ni=0.8, B含量为0.35%-2.10%(w)的一系列B-Ni₂P/SBA-15催化剂. 用X射线衍射(XRD)、N₂吸附脱附、透射电子显微镜(TEM)和氨气程序升温脱附(NH₃-TPD)等表征技术对催化剂的结构进行了研究, 以1%(w)二苯并噻吩(DBT)/十氢萘溶液为模型化合物, 在微型固定床反应器上对催化剂的加氢脱硫(HDS)性能进行了评价. 结果表明, B-Ni₂P/SBA-15催化剂仍具有介孔结构, Ni₂P为主要的活性物相. 适量B助剂的加入可促使Ni₂P晶粒减小, 催化剂比表面积增加. 此外, 随着B含量的增加, B-Ni₂P/SBA-15催化剂的总酸量也增加. 当反应压力为3.0 MPa, 反应温度由300 ℃升高至360 ℃时, B含量对Ni₂P/SBA-15催化剂活性有明显的影响, B含量为1.40%(w)的B-Ni₂P/SBA-15催化剂加氢脱硫活性最高. B-Ni₂P/SBA-15催化剂上二苯并噻吩的加氢脱硫的反应机理以直接脱硫为主.

关键词: 加氢脱硫, SBA-15, Ni₂P, 二苯并噻吩, 硼

Abstract:

The catalyst precursors of B-Ni₂P/SBA-15 were synthesized by co-impregnation using (NH₄)₂HPO₄ as the source of phosphorus, Ni(NO)₃ as the source of nickel and H₃BO₃ as the source of boron. The B-Ni₂P/SBA-15 catalysts with an initial P/Ni molar ratio of 0.8 and a boron content from 0.35% to 2.10%(w) were prepared by temperature-programmed reduction in a H₂ flow. The structure of the catalysts was characterized by X-ray diffraction (XRD), N₂ adsorption-desorption, transmission electron microscopy (TEM) and NH₃ temperature-programmed desorption (NH₃-TPD). The catalytic performances of hydrodesulfurization (HDS) were evaluated in a fixed-bed microreactor using dibenzothiophene (DBT) as a model compound. The results showed that the B-Ni₂P/SBA-15 catalysts still retained mesoporous structure. The Ni₂P phase was mainly active phases in all the catalysts. The proper addition of boron reduced the Ni₂P active phases but increased the specific surface area of the catalysts. The amount of acid in B-Ni₂P/SBA-15 also increased with addition of boron. When the reaction temperature was increased from 300 to 360 ℃, the HDS conversion of DBT over the catalyst clearly improved with an increase in the content of boron. The B-Ni₂P/SBA-15 catalyst with a boron content of 1.40%(w) had the best catalytic activity. The mechanism of the HDS of DBT consisted of main direct desulfurization (DDS) over the B-Ni₂P/SBA-15 catalysts.

Key words: Hydrodesulfurization, SBA-15, Ni₂P, Dibenzothiophene, Boron

赵鹏飞, 季生福, 魏妮, 马倩, 刘辉, 李成岳. B助剂对Ni₂P/SBA-15催化剂结构及其加氢脱硫性能的影响[J]. 物理化学学报, 2011, 27(07): 1737-1742.

ZHAO Peng-Fei, JI Sheng-Fu, WEI Ni, MA Qian, LIU Hui, LI Cheng-Yue. Effect of Boron Promoter on the Structure and Hydrodesulfurization Activity of Ni₂P/SBA-15 Catalysts[J]. Acta Phys. -Chim. Sin., 2011, 27(07): 1737-1742.

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB20110728

https://www.whxb.pku.edu.cn/CN/Y2011/V27/I07/1737

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B助剂对Ni₂P/SBA-15催化剂结构及其加氢脱硫性能的影响

Effect of Boron Promoter on the Structure and Hydrodesulfurization Activity of Ni₂P/SBA-15 Catalysts

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