载体制备方法对MoO3/ZrO2耐硫甲烷化催化剂的影响

doi:10.16085/j.issn.1000-6613.2017.04.018

化工进展 ›› 2017, Vol. 36 ›› Issue (04): 1288-1293.DOI: 10.16085/j.issn.1000-6613.2017.04.018

载体制备方法对MoO₃/ZrO₂耐硫甲烷化催化剂的影响

杨霞, 秦绍东, 李加波, 孙守理

北京低碳清洁能源研究所, 北京 102209

收稿日期:2016-09-18 修回日期:2016-12-21 出版日期:2017-04-05 发布日期:2017-04-05
通讯作者: 杨霞
作者简介:杨霞(1981-),女,博士,高级工程师。E-mail:yangxia@nicenergy.com。

Effect of preparation method of ZrO₂ support on catalytic performance of MoO₃/ZrO₂ for sulfur-resistant methanation

YANG Xia, QIN Shaodong, LI Jiabo, SUN Shouli

National Institute of Clean and Low Carbon Energy, Beijing 102209, China

Received:2016-09-18 Revised:2016-12-21 Online:2017-04-05 Published:2017-04-05

摘要/Abstract

摘要： 采用沉淀法制备了ZrO₂载体并进一步制备用于耐硫甲烷化反应的MoO₃/ZrO₂催化剂，考察了沉淀过程中增加醇洗以及醇溶液中高温老化处理对ZrO₂织构性质、晶相结构和形貌的影响。利用N₂物理吸附、X射线衍射、透射电子显微镜和X射线光电子能谱等手段对载体的结构与表面性质和催化剂活性相的形态与分布进行了表征。结果表明，醇洗和高温老化过程可以显著改善ZrO₂的结构特征，获得比表面积较大且晶粒尺寸更小更均匀的ZrO₂载体；进而有利于促进相应Mo基催化剂中MoS₂活性相的分散，使催化剂表现出优异的甲烷化活性。

关键词: 一氧化碳, 耐硫甲烷化, 氧化锆, 钼基催化剂, 天然气

Abstract: ZrO₂ was prepared via precipitation method and then used as the support of Mo catalysts for CO methanation in the presence of H₂S. The impact of post precipitation procedures of ethanol-washing and digestion(aging in hot ethanol) on the evolution of textural,structural and morphological properties of zirconia was investigated. The physicochemical properties of ZrO₂ supports and MoO₃/ZrO₂ catalysts were characterized by nitrogen adsorption-desorption,XRD,TEM and XPS. The results indicated that the post precipitation treatment was an effective means to achieve zirconia support with large specific surface area,and uniform and small particle size. The catalytic performance of the MoO₃/ZrO₂ catalysts was improved with ZrO₂ prepared by digesting at high temperature,which could be related to the degree of sulfidation of Mo species and the enhancement of dispersed MoS₂ active sites.

Key words: carbon monoxide, sulfur-resistant methanation, zirconia, Mo-based catalyst, natural gas

中图分类号:

O643
TQ426

杨霞, 秦绍东, 李加波, 孙守理. 载体制备方法对MoO₃/ZrO₂耐硫甲烷化催化剂的影响[J]. 化工进展, 2017, 36(04): 1288-1293.

YANG Xia, QIN Shaodong, LI Jiabo, SUN Shouli. Effect of preparation method of ZrO₂ support on catalytic performance of MoO₃/ZrO₂ for sulfur-resistant methanation[J]. Chemical Industry and Engineering Progress, 2017, 36(04): 1288-1293.

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载体制备方法对MoO₃/ZrO₂耐硫甲烷化催化剂的影响

Effect of preparation method of ZrO₂ support on catalytic performance of MoO₃/ZrO₂ for sulfur-resistant methanation

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