Solid-state reaction mechanism of ammonium molybdate with LaHY

ZHANG Weiqing; GUO Wenguang; CHU Lili; KONG Lingpeng; JIN Guangzhou

doi:10.11949/j.issn.0438-1157.20160403

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Solid-state reaction mechanism of ammonium molybdate with LaHY

更新时间：2025-12-10

- Solid-state reaction mechanism of ammonium molybdate with LaHY
- CIESC Journal Issue 8, Pages: 3380-3386(2016)
- 作者机构：
  
  北京石油化工学院化学工程系,北京,102617
- 作者简介：
- 基金信息：
- DOI：10.11949/j.issn.0438-1157.20160403
  CLC： 643
- Online First：05 August 2016，
  
  Published：05 August 2016
- 稿件说明：
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ZHANG Weiqing, GUO Wenguang, CHU Lili, et al. Solid-state reaction mechanism of ammonium molybdate with LaHY[J]. CIESC Journal, 2016, (8): 3380-3386.
DOI：

ZHANG Weiqing, GUO Wenguang, CHU Lili, et al. Solid-state reaction mechanism of ammonium molybdate with LaHY[J]. CIESC Journal, 2016, (8): 3380-3386. DOI： 10.11949/j.issn.0438-1157.20160403.

摘要

采用TG-DSC技术研究了钼酸铵和LaHY在空气气氛中的失重行为，考察了钼酸铵与LaHY的固相反应机理，用XRD、BET和NH3-TPD对其物相结构、比表面积和表面酸性进行了表征。结果表明，（NH4）6Mo7O24·4H2O分解产生的表相Mo物种借助固相反应以金属-氧簇定位在LaHY分子筛体相笼中形成nMoOx·LaHY单相复合体，引起分子筛的晶胞收缩，晶胞参数a0减小，比表面积下降。制备的nMoOx·LaHY较相应LaHY分子筛的弱酸中心变化较小，中强酸中心增加，强酸中心略有减少，总酸量增加。以质量分数为0.6%的二苯并噻吩/正癸烷溶液为模型反应物，评价了制备的nMoOx·LaHY催化剂的加氢脱硫性能。负载Mo质量分数为5.0%制得的nMoOx·LaHY催化剂在反应压力4.0 MPa，反应液时空速20 h-1，H2/原料液体积比500:1的实验条件下，290℃和310℃的二苯并噻吩加氢脱硫转化率达到了56.38%和88.79%，较相应负载Mo质量分数为20.0%制备的MoO3/Al2O3催化剂分别提高了约12个百分点和28个百分点，表现出了较高的二苯并噻吩加氢脱硫反应活性。

Abstract

Mass loss behavior in air and solid-state reaction mechanism of ammonium molybdate with LaHY were investigated by TG-DSC technique

and the physical structure

specific surface area

and surface acid sites by XRD

BET and NH3-TPD techniques. It showed that surface speicies of Mo arising from decomposition of (NH4)6Mo7O24·4H2O

over solid-state reaction of (NH4)6Mo7O24·4H2O with LaHY

allocates in LaHY molecular sieve cage as molybdenum-oxygen clusters to form a single-phase complex nMoOx·LaHY. The single-phase complex contributes to the lattice shrinkage

the reduced lattice parameter a0

and the decrease in specific surface area. The as-prepared nMoOx·LaHY possesses a slightly variation of weak acid center sites

an increase in medium strong acid center sites

a slightly decrease in strong acid center sites

and an increase in total acid sites

in comaprision with LaHY. The hydrodesulfulrization (HDS) performance of the single-phase complex nMoOx·LaHY was evaluated by using 0.6% (mass) dibenzothiophene(DBT)/decane as the representative reactants. The conversion of DBT in HDS process at 290℃ and 310℃ over nMoOx·LaHY catalyst with 5.0% (mass) of Mo loading

reached 56.38% and 88.79% under conditions of 4.0 MPa

20 h-1 of space velocity and 500:1 of H2/oil volumetric ratio

which increased 12 and 28 percentage than that of MoO3/Al2O3 with 20% (mass) of Mo loading

respectively. The nMoOx·LaHY catalyst exhibited higher activity for DBT HDS reaction.

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