Highly Efficient and Stable Vanadia-Titania-Sulfate Catalysts for Methanol Oxidation to Methyl Formate: Synthesis and Mechanistic Study

doi:10.1021/acs.jpcc.5b12621

	Highly Efficient and Stable Vanadia-Titania-Sulfate Catalysts for Methanol Oxidation to Methyl Formate: Synthesis and Mechanistic Study
	Liu, Ziyu 1; Zhang, Ruifang 1,2; Wang, Shibin1,3 ; Li, Na 1,4; Sima, Rui 1,5; Liu, Guojuan 1; Wu, Ping 1; Zeng, Gaofeng 1; Li, Shenggang1,3 ; Sun, Yuhan1,3
	2016-03-31
发表期刊	JOURNAL OF PHYSICAL CHEMISTRY C (IF:3.3[JCR-2023],3.5[5-Year])
ISSN	1932-7447
卷号	120 期号:12 页码:6591-6600
发表状态	已发表
DOI	10.1021/acs.jpcc.5b12621
摘要	Vanadia-titania-sulfate nanocatalysts for methanol oxidation to methyl formate (ME) were prepared by coprecipitation. When calcinated at 400 degrees C, both methanol conversion and MF selectivity reached similar to 98.5% at reaction temperatures of 140-145 degrees C. Characterizations with several experimental techniques revealed the catalysts as highly dispersed vanadia supported by anatase titania with acidic sites of significant strength and density. The catalysts also showed very high stability with lifetime exceeding 4500 h. Extensive density functional theory calculations using both cluster and surface models revealed MF to form via the hemiacetal mechanism, involving the condensation of methanol and formaldehyde at acidic sites and methanol and hemiacetal oxidations at redox sites. The alternative formyl mechanism was predicted kinetically much less favorable, showing these catalysts to work in a distinct mechanism from the rutile titania photocatalyst. Interestingly, methanol chemisorption at redox sites leads to the formation of acidic sites capable of catalyzing the condensation reaction.
收录类别	SCI ; EI
语种	英语
资助项目	"Hundred Talents" program of Chinese Academy of Sciences[Y224591401]
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science
WOS类目	Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号	WOS:000373416500034
出版者	AMER CHEMICAL SOC
EI入藏号	20161602271813
EI主题词	Catalysts ; Condensation ; Condensation reactions ; Density functional theory ; Oxidation ; Oxide minerals ; Titanium dioxide
EI分类号	Minerals:482.2 ; Chemical Reactions:802.2 ; Chemical Operations:802.3 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Probability Theory:922.1
WOS关键词	RUTHENIUM OXIDE CATALYSTS ; TOTAL-ENERGY CALCULATIONS ; ELASTIC BAND METHOD ; SELECTIVE OXIDATION ; BASIS-SETS ; NANOPARTICLES ; FORMALDEHYDE ; REACTIVITY ; SURFACE ; TIO2
原始文献类型	Article
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/1890
专题	物质科学与技术学院物质科学与技术学院_特聘教授组_孙予罕组物质科学与技术学院_特聘教授组_李圣刚组物质科学与技术学院_博士生
通讯作者	Li, Shenggang; Sun, Yuhan
作者单位	1.Chinese Acad Sci, Shanghai Adv Res Inst, CAS Key Lab Low Carbon Convers Sci & Engn, 100 Haike Rd, Shanghai 201210, Peoples R China 2.Univ Chinese Acad Sci, 19 Yuquan Rd, Beijing 100049, Peoples R China 3.ShanghaiTech Univ, Sch Phys Sci & Technol, 100 Haike Rd, Shanghai 201210, Peoples R China 4.Shanghai Univ, Dept Chem, 99 Shangda Rd, Shanghai 200444, Peoples R China 5.Shanghai Univ, Coll Environm & Chem Engn, 99 Shangda Rd, Shanghai 200444, Peoples R China
通讯作者单位	物质科学与技术学院
推荐引用方式 GB/T 7714	Liu, Ziyu,Zhang, Ruifang,Wang, Shibin,et al. Highly Efficient and Stable Vanadia-Titania-Sulfate Catalysts for Methanol Oxidation to Methyl Formate: Synthesis and Mechanistic Study[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2016,120(12):6591-6600.
APA	Liu, Ziyu.,Zhang, Ruifang.,Wang, Shibin.,Li, Na.,Sima, Rui.,...&Sun, Yuhan.(2016).Highly Efficient and Stable Vanadia-Titania-Sulfate Catalysts for Methanol Oxidation to Methyl Formate: Synthesis and Mechanistic Study.JOURNAL OF PHYSICAL CHEMISTRY C,120(12),6591-6600.
MLA	Liu, Ziyu,et al."Highly Efficient and Stable Vanadia-Titania-Sulfate Catalysts for Methanol Oxidation to Methyl Formate: Synthesis and Mechanistic Study".JOURNAL OF PHYSICAL CHEMISTRY C 120.12(2016):6591-6600.