摘要
采用水热法制备了Mo/Sn物质的量比为1∶2的Mo1Sn2催化剂,通过改变焙烧温度(400−700℃),调控了钼锡催化剂的结构,并研究了催化剂结构变化对二甲醚(DME)选择氧化制甲酸甲酯(MF)性能的影响。发现400℃焙烧的Mo1Sn2催化剂具有良好的催化氧化二甲醚生成甲酸甲酯的性能,在110℃、常压条件下,DME转化率为9.2%,MF选择性可达86.9%,并且无CO_(x)生成。采用XRD、Raman、XPS、TPD、H_(2)-TPR和in-situ FT-IR等表征手段对催化剂的结构和表面性质进行了系统研究。结果表明,低温焙烧更利于钼锡催化剂表面形成更多的MoO_(x)结构和Mo^(5+)物种,由此引起的催化剂的酸性、氧化还原性的增强和中强碱性位的增多可明显促进催化剂活性的增强和甲酸甲酯的生成。
The Mo1Sn2 catalysts with a Mo/Sn molar ratio of 1∶2 were prepared by the hydrothermal method,and their structure was regulated by changing the calcination temperature(400–700℃).The effect of the structural transformation of catalysts on the performance of selective oxidation of dimethyl ether(DME)to methyl formate(MF)was studied.It was found that the Mo1Sn2 catalyst calcined at 400℃exhibited good performance in the oxidation of DME to methyl formate,showing a DME conversion of 9.2%and the MF selectivity of 86.9%at 110℃and under atmospheric pressure without the generation of CO_(x).The catalysts were systematically characterized by XRD,Raman,XPS,TPD,H_(2)-TPR and in-situ FT-IR.The results showed that the low-temperature calcination was favorable for the formation of MoO_(x)structure and more Mo^(5+) species on the catalyst surface,resulting in the enhanced acidity and redox ability of the catalyst,and the increase of medium to strong basic sites on the catalysts.In such case,the activity and methyl formate production of the catalyst were significantly promoted.
作者
熊盼
高秀娟
王文秀
张俊峰
宋法恩
张清德
韩怡卓
谭猗生
XIONG Pan;GAO Xiu-juan;WANG Wen-xiu;ZHANG Jun-feng;SONG Fa-en;ZHANG Qing-de;HAN Yi-zhuo;TAN Yi-sheng(State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China;University of Chinese Academy of Sciences,Beijing 10049,China;Dalian National Laboratory for Clean Energy,Dalian 116023,China)
出处
《燃料化学学报》
EI
CAS
CSCD
北大核心
2022年第1期63-71,共9页
Journal of Fuel Chemistry and Technology
基金
国家自然科学基金(21773283,21373253)
中国科学院创新交叉团队项目(BK2018001)
中国科学院洁净能源创新研究院合作基金(DNL 201903)
中国科学院青年创新促进会人才项目(2014155)
厦门大学固体表面物理化学国家重点实验室开放基金(201624)资助。
关键词
二甲醚氧化
Mo1Sn2催化剂
焙烧温度
结构
甲酸甲酯
dimethyl ether oxidation
Mo1Sn2 catalyst
calcination temperature
structure
methyl formate
