Dual-Role Membrane as NH3 Permselective Reactor and Azeotrope Separator in Urea Alcoholysis

doi:10.1021/acscentsci.9b00812

	Dual-Role Membrane as NH3 Permselective Reactor and Azeotrope Separator in Urea Alcoholysis
	Zeng, Gaofeng 1; Wang, Yue 1,2; Gong, Dian 1,2; Zhang, Yanfeng 1,4; Wu, Ping 1; Sun, Yuhan1,3
	2019-11-27
发表期刊	ACS CENTRAL SCIENCE
ISSN	2374-7943
EISSN	2374-7951
卷号	5 期号:11 页码:1834-1843
发表状态	已发表
DOI	10.1021/acscentsci.9b00812
摘要	Urea methanolysis is a green alternative to synthesize dimethyl carbonate (UMto-DMC). However, it is strongly challenged by the generated NH3 induced thermodynamic equilibrium limitation and the azeotropic products' separation. Herein, these predicaments are well-relieved by introducing membranes in both reaction and product separation. An NH3 permselective membrane reactor (MR) based on modified SAPO-34 membrane is successfully realized for UM-to-DMC. The permselectivity and acidity of the SAPO-34 membrane are significantly adjusted to cater the strict molecular sieving of NH3/methanol and chemical inertness upon the reaction. The MR exhibits excellent reactant conversion and DMC selectivity, resulting in >139% higher DMC yield than that of the nonmembrane reactor, due to in situ removal of NH3 by the membrane. The MR also demonstrates reliable chemical, thermal, and mechanical stability during >2000 h. Moreover, the regular SAPO-34 membrane with controlled thickness presents remarkable separation performance for the methanol-DMC azeotrope, in which the methanol-DMC separation factors and the methanol permeance are 1-2 orders of magnitude higher than those of the polymeric membranes. This study suggests the great potential that integration of such membranes offers for process intensification, energy savings, and efficiency improvement in a series of urea alcoholysis and even other NH3 releasing reactions.
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收录类别	SCI ; SCIE ; EI
语种	英语
资助项目	Science and Technology Commission Shanghai Municipality[19ZR1479200]
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:000499482200016
出版者	AMER CHEMICAL SOC
WOS关键词	DIMETHYL CARBONATE ; ZEOLITE MEMBRANE ; GRAPHENE OXIDE ; SAPO-34 MEMBRANES ; METHYL CARBAMATE ; HIGH-TEMPERATURE ; METHANOL ; DEHYDROGENATION ; CONVERSION ; HYDROGEN
原始文献类型	Article
引用统计
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/104522
专题	物质科学与技术学院_特聘教授组_孙予罕组
通讯作者	Zeng, Gaofeng; 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, Sch Chem Sci, 19A Yuquan Rd, Beijing 100049, Peoples R China 3.ShanghaiTech Univ, Sch Phys Sci & Technol, 393 Mid Huaxia Rd, Shanghai 201210, Peoples R China 4.Shanghai Univ Engn Sci, Sch Chem & Chem Engn, 333 Longteng Rd, Shanghai 201620, 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	Zeng, Gaofeng,Wang, Yue,Gong, Dian,et al. Dual-Role Membrane as NH3 Permselective Reactor and Azeotrope Separator in Urea Alcoholysis[J]. ACS CENTRAL SCIENCE,2019,5(11):1834-1843.
APA	Zeng, Gaofeng,Wang, Yue,Gong, Dian,Zhang, Yanfeng,Wu, Ping,&Sun, Yuhan.(2019).Dual-Role Membrane as NH3 Permselective Reactor and Azeotrope Separator in Urea Alcoholysis.ACS CENTRAL SCIENCE,5(11),1834-1843.
MLA	Zeng, Gaofeng,et al."Dual-Role Membrane as NH3 Permselective Reactor and Azeotrope Separator in Urea Alcoholysis".ACS CENTRAL SCIENCE 5.11(2019):1834-1843.