The effects of the mo-sn contact interface on the oxidation reaction of dimethyl ether to methyl formate at a low reaction temperature
文献类型：期刊论文
| 作者 | Zhang, Zhenzhou1,2; Zhang, Qingde1; Jia, Lingyu1,2; Wang, Wenfeng1,2; Tian, Shao Peng1,2; Wang, Peng1,2; Xiao, He1,2; Han, Yizhuo1; Tsubaki, Noritatsu1,3; Tan, Yisheng1 |
| 刊名 | Catalysis science & technology
 |
| 出版日期 | 2016 |
| 卷号 | 6期号:15页码:6109-6117 |
| ISSN号 | 2044-4753 |
| DOI | 10.1039/c6cy00460a |
| 通讯作者 | Zhang, qingde(qdzhang@sxicc.ac.cn) ; Tan, yisheng(tan@sxicc.ac.cn) |
| 英文摘要 | With increasing degrees of mo-sn interface contact, the molar ratio of methyl formate (mf) to methanol (meoh) and formaldehyde (fa) was found to linearly increase at the same time, which indicates that a high degree of moo3 and sno2 interface contact has a strong positive effect on the conversion of the methoxyl intermediate to mf in the dimethyl ether (dme) oxidation reaction. xrd and fourier transform exafs indicate that the structure of molybdenum oxide starts to change from moo3 clusters to oligomer moox domains with an increase in the degree of mo-sn interface contact, and the mo-o-sn structure begins to dominate at the contact interfaces when the degree of interface contact increases to 0.0256 and 0.0384 nm(2) sno2/mo atom. hrtem also confirms the presence of the moox domains on the surface of the catalyst possessing the smallest molybdenum oxide content, the signals of which were even undetected by xrd and raman. moreover, esr, xps and xafs suggest that mo5+ species exist in the mo-sn contact interfaces rather than on the surface of the catalysts. the evaluation results of moo3-sba-15 further verify the key role of mo5+ in the formation of mf. therefore, mo5+ is reasonably proposed to be the active center for the formation of mf in the dme oxidation reaction. based on the catalytic characterization results, the reaction pathway of dme oxidation to mf via methoxyl intermediates was proposed on the mo(v) sites. first, dme was absorbed and consequently dissociated to become an absorbed methoxy-mo(v) species with the assistance of acidic sites and lattice oxygen. then, the beta-h was eliminated, and an absorbed fa-mo(iv) species was formed. consequently, the absorbed methoxy-mo(v) species reacted with the neighboring absorbed fa-mo(iv) species, producing mf, and then, the mo(iv) species was regenerated to become an mo(v) species by the oxidation of o-2 so it could catalyze another reaction cycle. the deeper understanding of this investigation has substantial meaning for the preparation of a catalyst with a specific molybdenum oxide structure that can be applied for transforming the methoxyl intermediate to produce other high-value products through the dme oxidation reaction. |
| WOS关键词 | SELECTIVE OXIDATION ; MOLYBDENUM OXIDE ; MILD CONDITIONS ; GAMMA-ALUMINA ; CATALYSTS ; METHANOL ; FORMALDEHYDE ; SURFACE ; ACID ; NANOPARTICLES |
| WOS研究方向 | Chemistry |
| WOS类目 | Chemistry, Physical |
| 语种 | 英语 |
| WOS记录号 | WOS:000381431200035 |
| 出版者 | ROYAL SOC CHEMISTRY |
| URI标识 | http://www.irgrid.ac.cn/handle/1471x/2376223 |
| 专题 | 中国科学院大学 |
| 通讯作者 | Zhang, Qingde; Tan, Yisheng |
| 作者单位 | 1.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Toyama Univ, Sch Engn, Dept Appl Chem, Gofuku 3190, Toyama 9308555, Japan |
| 推荐引用方式 GB/T 7714 | Zhang, Zhenzhou,Zhang, Qingde,Jia, Lingyu,et al. The effects of the mo-sn contact interface on the oxidation reaction of dimethyl ether to methyl formate at a low reaction temperature[J]. Catalysis science & technology,2016,6(15):6109-6117. |
| APA | Zhang, Zhenzhou.,Zhang, Qingde.,Jia, Lingyu.,Wang, Wenfeng.,Tian, Shao Peng.,...&Tan, Yisheng.(2016).The effects of the mo-sn contact interface on the oxidation reaction of dimethyl ether to methyl formate at a low reaction temperature.Catalysis science & technology,6(15),6109-6117. |
| MLA | Zhang, Zhenzhou,et al."The effects of the mo-sn contact interface on the oxidation reaction of dimethyl ether to methyl formate at a low reaction temperature".Catalysis science & technology 6.15(2016):6109-6117. |
入库方式： iSwitch采集
来源：中国科学院大学
浏览0
下载0
收藏0
其他版本
除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。