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Achieving a Superlong Lifetime in the Zeolite-Catalyzed MTO Reaction under High Pressure: Synergistic Effect of Hydrogen and Water

文献类型：期刊论文

作者Guo, Xinwen3; Zhao, Xuebin1,2,3; Li, Jinzhe2; Tian, Peng2; Wang, Linying2; Li, Xiaofang1,2; Lin, Shanfan1,2; Liu, Zhongmin2
刊名ACS CATALYSIS
出版日期2019-04-01
卷号9期号:4页码:3017-3025
关键词methanol to olefins SAPO-34 long lifetime high-pressure H-2 hydrogenation
ISSN号2155-5435
DOI10.1021/acscatal.8b04402
通讯作者Tian, Peng(tianpeng@dicp.ac.cn) ; Liu, Zhongmin(liuzm@dicp.ac.cn)
英文摘要Zeolites are usually considered to be acid catalysts, which are prone to deactivation due to the coke deposition in the hydrocarbon conversions such as methanol-to-olefins (MTO) reaction. Herein, a high-pressure MTO process with cofeeding H-2 and H2O is reported, which can effectively prolong the catalytic lifetime of SAPO-34. The corresponding methanol handling capacity is about 200 times larger than that under the normal-pressure condition. Investigation reveals that the ultralong lifetime originates from the hydrogenation ability of the acid sites on SAPO-34 for aromatic species, which can hydrogenate the heavy aromatic deposits (especially the phenanthrene composed of three benene rings) to active aromatic intermediates (methylbenzenes and methylnaphthalenes) and thus slow down the evolution of coke species. A positive synergistic effect between H-2 and H2O on prolonging the catalyst lifetime is observed at higher H2O partial pressure, likely resulting from the reduced barriers of hydrogenation reactions in the presence of H2O. Furthermore, the evolution pathways of coke species are markedly affected by reaction temperature, and fast deactivation may occur below 400 degrees C due to the formation of large molecule diadamantanes.
WOS关键词TO-OLEFINS CONVERSION ; COKE FORMATION ; HYDROCARBON FORMATION ; SELECTIVE CONVERSION ; REACTION-MECHANISM ; METHANOL ; SAPO-34 ; SYNGAS ; CONFINEMENT ; METHYLATION
资助项目National Natural Science Foundation of China[21676262] ; National Natural Science Foundation of China[21576256] ; CAS[QYZDB-SSW-JSC040]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000464075700032
出版者AMER CHEMICAL SOC
资助机构National Natural Science Foundation of China ; National Natural Science Foundation of China ; CAS ; CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; CAS ; CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; CAS ; CAS ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; CAS ; CAS
源URL[http://cas-ir.dicp.ac.cn/handle/321008/165654]  
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Tian, Peng; Liu, Zhongmin
作者单位1.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
2.Chinese Acad Sci, Dalian Natl Lab Clean Energy, IChEM Collaborat Innovat Ctr Chem Energy Mat, Natl Engn Lab Methanol Olefins,Dalian Inst Chem P, Dalian 116023, Peoples R China
3.Dalian Univ Technol, Sch Chem Engn, PSU DUT Joint Ctr Energy Res, State Key Lab Fine Chem, Dalian 116024, Peoples R China
推荐引用方式
GB/T 7714		 Guo, Xinwen,Zhao, Xuebin,Li, Jinzhe,et al. Achieving a Superlong Lifetime in the Zeolite-Catalyzed MTO Reaction under High Pressure: Synergistic Effect of Hydrogen and Water[J]. ACS CATALYSIS,2019,9(4):3017-3025.
APA Guo, Xinwen.,Zhao, Xuebin.,Li, Jinzhe.,Tian, Peng.,Wang, Linying.,...&Liu, Zhongmin.(2019).Achieving a Superlong Lifetime in the Zeolite-Catalyzed MTO Reaction under High Pressure: Synergistic Effect of Hydrogen and Water.ACS CATALYSIS,9(4),3017-3025.
MLA Guo, Xinwen,et al."Achieving a Superlong Lifetime in the Zeolite-Catalyzed MTO Reaction under High Pressure: Synergistic Effect of Hydrogen and Water".ACS CATALYSIS 9.4(2019):3017-3025.

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来源：大连化学物理研究所

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