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水热合成的MoO3-SnO2催化剂催化氧化二甲醚的性能研究
引用本文:杨奇,高秀娟,冯茹,李明杰,张俊峰,张清德,韩怡卓,谭猗生. 水热合成的MoO3-SnO2催化剂催化氧化二甲醚的性能研究[J]. 燃料化学学报, 2019, 47(8): 934-941
作者姓名:杨奇  高秀娟  冯茹  李明杰  张俊峰  张清德  韩怡卓  谭猗生
作者单位:1. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China;2. University of Chinese Academy of Sciences, Beijing 100049, China
基金项目:国家自然科学基金(21773283,21373253),中国科学院创新交叉团队项目(BK2018001),中国科学院青年创新促进会人才项目(2014155)和厦门大学固体表面物理化学国家重点实验室开放课题(201624)资助
摘    要:采用无沉淀剂水热法一步合成了MoO3-SnO2复合金属氧化物催化剂,通过调变Mo/Sn物质的量比,考察了催化剂上活性组分MoOx分散程度对二甲醚(DME)低温氧化生成甲酸甲酯(MF)反应性能的影响。当Mo/Sn=1∶2,反应条件为150℃时,催化剂表现出较好的催化性能,DME转化率为22.0%,MF选择性达到77.6%。实验中采用TEM、XRD、Raman、FT-IR、NH3-TPD及H2-TPR等表征对催化剂晶体结构及表面性质进行了分析。结果发现,Mo/Sn物质的量比变化会对催化剂晶体结构产生显著影响,钼氧化物在SnO2表面形成不同分散程度的MoOx结构,这种钼氧化物结构的变化进一步影响了催化剂表面的酸性及氧化还原性,是造成催化性能差异的主要原因。

关 键 词:水热合成  二甲醚  选择氧化  甲酸甲酯  MoOx  
收稿时间:2019-03-26

MoO3-SnO2 catalyst prepared by hydrothermal synthesis method for dimethyl ether catalytic oxidation
YANG Qi,GAO Xiu-juan,FENG Ru,LI Ming-jie,ZHANG Jun-feng,ZHANG Qing-de,HAN Yi-zhuo,TAN Yi-sheng. MoO3-SnO2 catalyst prepared by hydrothermal synthesis method for dimethyl ether catalytic oxidation[J]. Journal of Fuel Chemistry and Technology, 2019, 47(8): 934-941
Authors:YANG Qi  GAO Xiu-juan  FENG Ru  LI Ming-jie  ZHANG Jun-feng  ZHANG Qing-de  HAN Yi-zhuo  TAN Yi-sheng
Abstract:MoO3-SnO2 composite metal oxide catalyst was synthesized by one-step hydrothermal synthesis method without precipitant. The effect of MoOx dispersion state on the catalytic performance of MoO3-SnO2 catalysts with different Mo/Sn molar ratios was investigated for dimethyl ether (DME) low-temperature oxidation to methyl formate (MF). MF selectivity reaches 77.6% with DME conversation of 22.0% over Mo1Sn2 at 150 ℃. The physiochemical properties of these catalysts were characterized by TEM, XRD, Raman, FT-IR, NH3-TPD and H2-TPR. The results showed that the addition of SnO2 into MoO3 affected the crystal structure of catalysts, forming MoOx species with different degree of dispersion on the surface of SnO2. The special architecture of MoOx-SnO2 plays a major role in modifying the acidity and the oxidizability of MoO3-SnO2 catalysts, leading to the obvious differences on catalytic activity.
Keywords:hydrothermal synthesis  dimethyl ether  selective oxidation  methyl formate  MoOx  
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