Mo-Sn催化剂上甲醇低温氧化制甲缩醛  

Low-temperature oxidation of methanol to dimethoxymethane over Mo-Sn catalyst

作　　者：王文秀 高秀娟[1,2] 熊盼 张俊峰 宋法恩[1] 张清德[1,3] 韩怡卓[1] 谭猗生 WANG Wen-xiu;GAO Xiu-juan;XIONG Pan;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)

机构地区：[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]中国科学院大学,北京100049 [3]中国科学院洁净能源创新研究院,辽宁大连116023

出　　处：《燃料化学学报》2021年第10期1487-1494,共8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(DNL201903);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。

摘　　要：采用水热合成法制备了甲醇合成甲缩醛的新型Mo-Sn催化剂。该催化剂可以在低Mo含量时实现甲醇低温氧化高选择性制取甲缩醛。通过考察Mo含量对催化剂结构及甲醇低温氧化制甲缩醛性能的影响,发现Mo1Sn10催化剂在甲醇氧化中表现出了较好的催化性能,在140℃、常压反应条件下,甲醇转化率为14.2%,甲缩醛选择性达到了88.9%,并且反应过程中无CO_(x)生成。采用XRD、Raman、FT-IR、XPS、NH_(3)-TPD及H_(2)-TPR等表征手段对催化剂进行深入研究。结果表明,不同Mo含量的催化剂结构性能存在着明显的差别,较低含量Mo的存在更有利于Mo5+及MoOx的生成,而由此引起的酸性及氧化还原性的变化是催化剂具有良好性能的重要原因。A new Mo-Sn catalyst prepared by hydrothermal method was used for the synthesis of dimethoxymethane(DMM)from methanol oxidation.The catalyst with low Mo content can achieve low-temperature oxidation of methanol to DMM with high selectivity.The influence of Mo content on the structure and the catalytic performance of the catalyst was investigated.It was found that Mo1Sn10 catalyst showed the best catalytic performance under the conditions of 140℃ and atmospheric pressure,the methanol conversion was 14.2%,and the selectivity of DMM reached 88.9%without the formation of CO_(x) during the reaction process.The catalysts were characterized by XRD,Raman,FT-IR,XPS,NH_(3)-TPD and H_(2)-TPR.The results showed that the catalysts with different Mo content had obvious differences in structure and performance.Lower Mo content was more conducive to the formation of Mo5+and MoOx,and the resulting changes in acidity and redox properties were the important reasons for the excellent performance of the catalysts.

关 键 词：甲醇 低温氧化 甲缩醛 Mo-Sn催化剂 Mo^(5+)物种 

分 类 号：O643[理学—物理化学]