现代化工2024,Vol.44Issue(6) :101-106.DOI:10.16606/j.cnki.issn0253-4320.2024.06.021

Al2O3基材作载体制备MoP加氢脱硫催化剂的研究

Preparation of Al2O3-based material supported MoP catalyst for hydrodesulfurization

邹洁 李翔 盛强 尚森森 王伟
现代化工2024,Vol.44Issue(6) :101-106.DOI:10.16606/j.cnki.issn0253-4320.2024.06.021

Al2O3基材作载体制备MoP加氢脱硫催化剂的研究

Preparation of Al2O3-based material supported MoP catalyst for hydrodesulfurization

邹洁 1李翔 2盛强 2尚森森 2王伟1
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作者信息

  • 1. 银川能源学院,宁夏银川 750105
  • 2. 天津科技大学化工与材料学院,天津 300457
  • 折叠

摘要

采用低温燃烧法和溶剂热法分别合成了富含五配位Al3+物种的氧化铈改性Al2O3(Ce-Al2O3)和介孔-大孔Al2O3(M-Al2O3);通过程序升温还原浸渍法负载的Mo的磷酸盐前驱体制备了 MoP催化剂.以二苯并噻吩(DBT)为模型含硫化合物评价了其加氢脱硫(HDS)性能.结果表明,M-Al2O3上制备纯相MoP所需磷酸盐前驱体的P/Mo摩尔比在1~1.2之间.DBT 在 MoP 催化剂上转化率大小为 MoP(1)/SiO2>MoP(1)/Ce-Al2O3>MoP(1.2)/M-Al2O3.动力学研究表明,DBT 在 MoP(1)/Ce-Al2O3和MoP(1.2)/M-Al2O3上的HDS反应活化能几乎相同,显著小于MoP(1)/SiO2上的活化能.在MoP催化剂上,直接脱硫(DDS)路径选择性随温度的增加而增加.在较低的温度下(如280℃),DBT主要通过加氢(HYD)反应路径脱硫;在较高的温度下(如360℃),DDS和HYD两条反应路径并重.

Abstract

A cerium oxide modified Al2O3(Ce-Al2O3)and a macro-mesoporous Al2O3(M-Al2O3),which are both rich in pentahedrally coordinated Al3+,are synthesized via a low-temperature combustion method and a solvothermal method,respectively.MoP catalysts are obtained through temperature-programmed method to reduce the supported molybdenum phosphate precursors prepared via an impregnation method.The hydrodesulfurization performances of MoP catalysts are evaluated through using dibenzothiophene(DBT)as model sulfur-containing compound.It is indicated that the P/Mo molar ratio in the phosphate precursor required for the formation of phase-pure MoP over M-Al2O3 is between 1 and 1.2.The conversion of DBT over MoP catalysts drops in the order of MoP(1)/SiO2>MoP(1)/Ce-Al2O3>MoP(1.2)/M-Al2O3.It is demonstrated by the kinetic study that the hydrodesulfurization activation energy of DBT over MoP(1)/Ce-Al2O3 is nearly same as that over MoP(1.2)/M-Al2O3,both are much lower than that over MoP(1)/SiO2.Over these MoP catalysts,the selectivity of the direct desulfurization pathway increases with the rising temperature.At a relatively low temperature(e.g.280℃),the desulfurization of DBT occurs mainly through the hydrogenation pathway;while at a high temperature(e.g.360℃),both the direct desulfurization and hydrodesulfurization pathways play an equal role.

关键词

MoP/磷酸盐前驱体/程序升温还原/Al2O3/加氢脱硫/二苯并噻吩

Key words

MoP/phosphate precursors/temperature-programmed reduction/Al2O3/hydrodesulfurization/dibenzothiophene

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基金项目

宁夏回族自治区自然科学基金(2021AAC03253)

国家自然科学基金(21673029)

国家自然科学基金(22108207)

天津市自然科学基金重点项目(19JCZDJC31700)

重质油国家重点实验室开放基金(SKLHOP202202005)

出版年

2024
现代化工
中国化工信息中心

现代化工

CSTPCDCSCD北大核心
影响因子:0.553
ISSN:0253-4320
参考文献量20
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