V2O5/CeO2 催化剂上甲醇氧化一步法合成二甲氧基甲烷

doi:10.3724/SP.J.1088.2012.11015

催化学报 ›› 2012, Vol. 33 ›› Issue (5): 813-818.DOI: 10.3724/SP.J.1088.2012.11015

V₂O₅/CeO₂ 催化剂上甲醇氧化一步法合成二甲氧基甲烷

郭荷芹1, 李德宝1,b, 陈从标1, 范志宏1,2, 孙予罕1,3,a

1中国科学院山西煤炭化学研究所煤转化国家重点实验室, 山西太原 030001; 2中国科学院研究生院, 北京 100049; 3中国科学院上海高等研究院, 上海 201203

收稿日期:2011-10-21 修回日期:2011-12-13 出版日期:2012-05-09 发布日期:2012-05-09

One-Step Oxidation of Methanol to Dimethoxymethane on V₂O₅/CeO₂ Catalyst

GUO Heqin1, LI Debao1,b, CHEN Congbiao1, FAN Zhihong1,2, SUN Yuhan1,3,a

1State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China; 2Graduate University of Chinese Academy of Sciences, Beijing 100049, China; 3Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201203, China

Received:2011-10-21 Revised:2011-12-13 Online:2012-05-09 Published:2012-05-09

摘要/Abstract

摘要： 采用溶胶-凝胶法制备了 V₂O₅/CeO₂ 催化剂, 并用于甲醇氧化一步法合成二甲氧基甲烷 (DMM) 反应中. 考察了 V₂O₅含量对钒氧化物的存在状态、催化剂表面酸性、氧化-还原性及其催化甲醇氧化反应性能的影响. 结果表明, V₂O₅含量为 15% 时钒氧化物呈单层分散, 小于 15% 时以孤立或聚合态存在, 大于 20% 时出现 V₂O₅ 晶体, 达到 30% 时出现 CeVO₄. 当 V₂O₅含量为 15% 时, 较高的钒氧化物分散度使催化剂具有较强的氧化还原能力和较多的酸性中心, 从而使催化剂具有较高的活性和 DMM 选择性.

关键词: 氧化钒, 氧化铈, 甲醇氧化, 酸性, 氧化-还原性, 二甲氧基甲烷

Abstract: The V₂O₅/CeO₂ catalyst samples were prepared by the sol-gel method and applied in the methanol partly oxidation. The influence of V₂O₅ content on the existing state of vanadia and surface properties as well as the catalytic performance was studied. The results showed that the vanadia was monolayer dispersed with V₂O₅ content was 15%, aggregated as V₂O₅ crystalline with above 20%, and formed CeVO₄ with 30%. The higher dispersion of vanadia can lead to stronger reducibility and more acidic sites, which were closely related to the higher methanol conversion and dimethoxymethane selectivity.

Key words: vanadia, ceria, methanol oxidation, acidity, redox, dimethoxymethane

郭荷芹, 李德宝, 陈从标, 范志宏, 孙予罕. V₂O₅/CeO₂ 催化剂上甲醇氧化一步法合成二甲氧基甲烷[J]. 催化学报, 2012, 33(5): 813-818.

GUO He-Qin, LI De-Bao, CHEN Cong-Biao, FAN Zhi-Hong, SUN Yu-Han. One-Step Oxidation of Methanol to Dimethoxymethane on V₂O₅/CeO₂ Catalyst[J]. Chinese Journal of Catalysis, 2012, 33(5): 813-818.

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V₂O₅/CeO₂ 催化剂上甲醇氧化一步法合成二甲氧基甲烷

One-Step Oxidation of Methanol to Dimethoxymethane on V₂O₅/CeO₂ Catalyst

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