DICP OpenIR
Achieving a Superlong Lifetime in the Zeolite-Catalyzed MTO Reaction under High Pressure: Synergistic Effect of Hydrogen and Water
Zhao, Xuebin1,2,3; Li, Jinzhe1; Tian, Peng1; Wang, Linying1; Li, Xiaofang1,2; Lin, Shanfan1,2; Guo, Xinwen3; Liu, Zhongmin1
Corresponding AuthorTian, Peng(tianpeng@dicp.ac.cn) ; Liu, Zhongmin(liuzm@dicp.ac.cn)
Keywordmethanol to olefins SAPO-34 long lifetime high-pressure H-2 hydrogenation
Source PublicationACS CATALYSIS
2019-04-01
ISSN2155-5435
DOI10.1021/acscatal.8b04402
Volume9Issue:4Pages:3017-3025
Funding ProjectNational Natural Science Foundation of China[21676262] ; National Natural Science Foundation of China[21576256] ; CAS[QYZDB-SSW-JSC040]
Funding OrganizationNational 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
WOS SubjectChemistry, Physical
WOS Research AreaChemistry
WOS KeywordTO-OLEFINS CONVERSION ; COKE FORMATION ; HYDROCARBON FORMATION ; SELECTIVE CONVERSION ; REACTION-MECHANISM ; METHANOL ; SAPO-34 ; SYNGAS ; CONFINEMENT ; METHYLATION
AbstractZeolites 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.
Language英语
Funding OrganizationNational 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
WOS IDWOS:000464075700032
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:2[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/165655
Collection中国科学院大连化学物理研究所
Corresponding AuthorTian, Peng; Liu, Zhongmin
Affiliation1.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
2.Univ Chinese Acad Sci, Beijing 100049, 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
Recommended Citation
GB/T 7714
Zhao, Xuebin,Li, Jinzhe,Tian, Peng,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 Zhao, Xuebin.,Li, Jinzhe.,Tian, Peng.,Wang, Linying.,Li, Xiaofang.,...&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 Zhao, Xuebin,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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