TixCe1-xO2 nanocomposites: a monolithic catalyst for the direct conversion of carbon dioxide and methanol to dimethyl carbonate

doi:10.1039/c9gc00811j

	TixCe1-xO2 nanocomposites: a monolithic catalyst for the direct conversion of carbon dioxide and methanol to dimethyl carbonate
	Chen, Yongdong 2,3; Wang, Hong 2; Qin, Zhaoxian 3; Tian, Shanti 2,3; Ye, Zhongbin 2; Ye, Lin 2; Abroshan, Hadi 1,4; Li, Gao 3
刊名	GREEN CHEMISTRY
	2019-09-07
卷号	21 期号:17 页码:4642-4649
ISSN号	1463-9262
DOI	10.1039/c9gc00811j
通讯作者	Chen, Yongdong(yongdongchen@swpu.edu.cn) ; Abroshan, Hadi(hadi.abroshan@chemistry.gatech.edu) ; Li, Gao(gaoli@dicp.ac.cn)
英文摘要	Dimethyl carbonate (DMC) is widely employed as a versatile reagent and solvent for green organic synthesis and fuel additives. Owing to the environmental issues of the traditional methods for DMC production, the direct synthesis of DMC from carbon dioxide and methanol has received significant interest worldwide. Here, we demonstrate the catalytic effectiveness of monolithic titanium-doped cerium oxides, TixCe1-xO2 nanocomposites, for the direct synthesis of DMC. The TixCe1-xO2 nanocomposites are characterized by BET measurements, Raman spectroscopy, powder X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, and H-2-temperature-programmed reduction analysis. To increase the reaction efficiency, the TixCe1-xO2 composites are uniformly coated on honeycomb ceramics in a continuous tubular fixed-bed reactor. This leads to an extended surface area of the catalyst, and therefore the reaction conversion rate toward DMC production is significantly enhanced. Results indicate that the catalyst exhibits 24.3% methanol conversion with 79% selectivity for DMC synthesis at 140 degrees C in the absence of any dehydrating agents. The catalytic effectiveness of the TixCe1-xO2 nanocomposites is found to be considerably higher than those of conventional catalysts. Analysis shows that the concentration of active sites can be systemically enriched by incorporating an optimal amount of Ti dopants into CeO2 to improve the catalytic activity of the reaction. The results of this study demonstrate the promise of the TixCe1-xO2 nanocomposites for the green production of DMC, and may offer guidelines for designing efficient catalysts for the selective conversion of methanol to other building blocks of chemical synthesis.
资助项目	National Natural Science Foundation of China[21773189] ; National Undergraduate Training Program for Innovation and Entrepreneurship[201710615001] ; National Undergraduate Training Program for Innovation and Entrepreneurship[201810615032] ; Liaoning Revitalization Talents Program[XLYC1807121]
WOS关键词	CO2 ; OXIDATION ; CERIA ; TRANSESTERIFICATION ; NANOCLUSTERS ; MORPHOLOGY ; CE
WOS研究方向	Chemistry ; Science & Technology - Other Topics
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000483588100025
资助机构	National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Undergraduate Training Program for Innovation and Entrepreneurship ; National Undergraduate Training Program for Innovation and Entrepreneurship ; Liaoning Revitalization Talents Program ; Liaoning Revitalization Talents Program ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Undergraduate Training Program for Innovation and Entrepreneurship ; National Undergraduate Training Program for Innovation and Entrepreneurship ; Liaoning Revitalization Talents Program ; Liaoning Revitalization Talents Program ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Undergraduate Training Program for Innovation and Entrepreneurship ; National Undergraduate Training Program for Innovation and Entrepreneurship ; Liaoning Revitalization Talents Program ; Liaoning Revitalization Talents Program ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Undergraduate Training Program for Innovation and Entrepreneurship ; National Undergraduate Training Program for Innovation and Entrepreneurship ; Liaoning Revitalization Talents Program ; Liaoning Revitalization Talents Program
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/173060]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Chen, Yongdong; Abroshan, Hadi; Li, Gao
作者单位	1.Georgia Inst Technol, Sch Chem & Biochem, Atlanta, GA 30332 USA 2.Southwest Petr Univ, Coll Chem & Chem Engn, Chengdu 610500, Sichuan, Peoples R China 3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China 4.Stanford Univ, SUNCAT Ctr Interface Sci & Catalysis, Dept Chem Engn, Stanford, CA 94305 USA
推荐引用方式 GB/T 7714	Chen, Yongdong,Wang, Hong,Qin, Zhaoxian,et al. TixCe1-xO2 nanocomposites: a monolithic catalyst for the direct conversion of carbon dioxide and methanol to dimethyl carbonate[J]. GREEN CHEMISTRY,2019,21(17):4642-4649.
APA	Chen, Yongdong.,Wang, Hong.,Qin, Zhaoxian.,Tian, Shanti.,Ye, Zhongbin.,...&Li, Gao.(2019).TixCe1-xO2 nanocomposites: a monolithic catalyst for the direct conversion of carbon dioxide and methanol to dimethyl carbonate.GREEN CHEMISTRY,21(17),4642-4649.
MLA	Chen, Yongdong,et al."TixCe1-xO2 nanocomposites: a monolithic catalyst for the direct conversion of carbon dioxide and methanol to dimethyl carbonate".GREEN CHEMISTRY 21.17(2019):4642-4649.