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Modeling and analysis of air combustion and steam regeneration in methanol to olefins processes

Chinese Journal of Chemical Engineering 2024年第2期66卷 94-103页

作者： Jinqiang Liang Danzhu Liu Shuliang Xu Mao Ye Department of Chemical Physics University of Science and Technology of ChinaHefei 230026China National Engineering Research Center of Lower-Carbon Catalysis Technology Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116021China University of Chinese Academy of Sciences Beijing 100049China

Light olefins is the incredibly important materials in chemical *** to olefins(MTO),which provides a non-oil route for light olefins production,received considerable attention in the past ***,the catalyst deactivation is an inevitable feature in MTO processes,and regeneration,therefore,is one of the key steps in industrial MTO *** the MTO catalyst is regenerated by removing the deposited coke via air combustion,which unavoidably transforms coke into carbon dioxide and reduces the carbon utilization *** study shows that the coke species over MTO catalyst can be regenerated via steam,which can promote the light olefins yield as the deactivated coke species can be essentially transferred to industrially useful synthesis gas,is a promising pathway for further MTO processes *** this work,we modelled and analyzed these two MTO regeneration methods in terms of carbon utilization efficiency and technology *** shown,the steam regeneration could achieve a carbon utilization efficiency of 84.31%,compared to 74.74%for air combustion *** MTO processes using steam regeneration can essentially achieve the near-zero carbon *** addition,light olefins production of the MTO processes using steam regeneration is 12.81%higher than that using air combustion *** this regard,steam regeneration could be considered as a potential yet promising regeneration method for further MTO processes,showing not only great environmental benefits but also competitive economic performance.

关键词： Model methanol to olefins Regeneration Greenhouse gas Processes simulation

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Recent progress in the deactivation mechanism of zeolite catalysts in methanol to olefins

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Science China Chemistry 2024年第12期67卷 3934-3943页

作者： Sheng Fan Han Wang Sen Wang Mei Dong Weibin Fan State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China University of Chinese Academy of Sciences Beijing 100049China

methanol to olefins(MTO)as an important reaction in C1 chemistry can effectively transform non-petroleum carbon resources into value-added *** have been widely used as MTO ***,they usually suffer from a rapid deactivation due to bulky coke species production,and thus require continuous regenerations in industrial *** key to design and develop highly stable zeolite catalysts for MTO process is to unravel the deactivation mechanism and clarify the structure–performance relationship of ***,in this mini-review,we investigate the critical intermediate species inducing zeolite deactivation and analyze the formation and evolution pathways of polycyclic aromatic hydrocarbons(PAHs)that are the precursors of carbonaceous *** addition,some methods to alleviate the coking mainly including acid regulation,morphology modification and process optimization,are also summarized.

关键词： methanol to olefins zeolites deactivation mechanism polycyclic aromatic hydrocarbons

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Significant Breakthrough in Industrial Test of the "methanol to olefins" Process Developed by Dalian Institute of Chemical Physics,Chinese Academy of Sciences

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Journal of Natural Gas Chemistry 2006年第4期15卷 I0001-I0002页

A process of ＂methanol or Dimethylether to olefins＂ developed by Dalian Institute of Chemical Physics （DICP）, designated as the DMTO process, has attained great success in industrial scaling up testing. DICP, by collaborating with the Xinxing Coal Chemical Co., Ltd. of Shaanxi Province and the Luoyang Petrochemical Engineering Co. of the SINOPEC Group, operated successfully a 50t（methanol）/d unit for the conversion of methanol to lower olefins, with a methanol conversion of close to 100%, and a selectivity to lower olefins（ethylene, propylene and butylenes） of higher than 90%. On 23rd August, the industrial test project has passed a state appraisal. The experts of the Appraisal Group, headed by Prof. YUAN Qingtang, academician of Chinese Academy of Engineering, drew the conclusions that the DMTO process, by utilizing a proprietary SAPO-34 catalyst system and a recycling fluidized bed reaction system for the production of lower olefins from methanol, is the first unit in the world having a capacity of producing nearly ten thousand tons lower olefins per year. The technological level of the industrial test is at a leading position internationally. This accomplishment will provide a sound base for the subsequent commercialization of the DMTO process.

关键词： methanol to olefins Process Developed by Dalian Institute of Chemical Physics,Chinese Academy of Sciences Significant Breakthrough in Industrial Test of the DMTO Test

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In situ Synthesis of SAPO-34 Zeolites in Kaolin Microspheres for a Fluidized methanol or Dimethyl Ether to olefins Process

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Chinese Journal of Chemical Engineering 2010年第6期18卷 979-987页

作者： ZHU Jie CUI Yu NAWAZ Zeeshan WANG Yao WEI Fei Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical Engineering Tsinghua University Beijing 100084 China

SAPO-34 zeolite is considered to be an effective catalyst for methanol or dimethyl ether conversion to olefins. In this study,we developed the in situ synthesis technology to prepare SAPO-34 zeolite in kaolin micro-spheres as a catalyst for fluidized methanol or dimethyl ether to olefins process. The silicoaluminophosphate zeolite was first time reported to be synthesized in kaolin microspheres. The SAPO-34 content of synthesized catalyst was about 22% as measured by three different quantitative methods(micropore area,X-ray fluorescence and energy dispersive spectroscopy element analysis) . Most of the SAPO-34 zeolites were in nanoscale size and distributed uniformly inside the spheres. The catalytic performance was evaluated in fixed bed and fluidized bed reactors. Compared with the conventional spray-dry catalyst,SAPO/kaolin catalyst showed superior catalytic activities,bet-ter olefin selectivities(up to 94%,exclusive coke) ,and very good hydrothermal stability. The in situ synthesis of SAPO-34 in kaolin microspheres is a facile and economically feasible way to prepare more effective catalyst for fluidized MTO/DTO(methanol to olefins/dimethyl ether to olefins) process.

关键词： SAPO-34 in situ synthesis kaolin fluidized bed methanol to olefins

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Data-driven optimal operation of the industrial methanol to olefin process based on relevance vector machine

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Chinese Journal of Chemical Engineering 2021年第6期34卷 106-115页

作者： Zhiquan Wang Liang Wang Zhihong Yuan Bingzhen Chen Department of Chemical Engineering Tsinghua UniversityBeijing 100084China State Key Laboratory of Chemical Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

methanol to olefin(MTO)technology provides the opportunity to produce olefins from nonpetroleum sources such as coal,biomass and natural *** than 20 commercial MTO plants have been put into *** now,contributions on optimal operation of industrial MTO plants from a process systems engineering perspective are *** on relevance vector machine(RVM),a data-driven framework for optimal operation of the industrial MTO process is established to fully utilize the plentiful industrial data *** correlates the yield distribution prediction of main products and the operation *** correlations then serve as the constraints for the multi-objective optimization model to pursue the optimal operation of the *** sorting genetic algorithmⅡis used to solve the optimization *** tests demonstrate that the ethylene yield is effectively improved based on the proposed *** RVM does provide the distribution prediction instead of point estimation,the established model is expected to provide guidance for actual production operations under uncertainty.

关键词： methanol to olefins Relevance vector machine Genetic algorithm Operation optimization Systems engineering Process systems

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Changing the balance of the MTO reaction dual-cycle mechanism: Reactions over ZSM-5 with varying contact times

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Chinese Journal of Catalysis 2016年第8期37卷 1413-1422页

作者：张默之徐舒涛魏迎旭李金哲王金棒张雯娜高树树刘中民中国科学院大连化学物理研究所洁净能源国家实验室(筹)甲醇制烯烃国家工程实验室能源材料化学协同创新中心辽宁大连116023 中国科学院大学北京100049 中国科学院大连化学物理研究所催化基础国家重点实验室辽宁大连116023

The methanol to olefins （MTO） reaction was performed over ZSM‐5 zeolite at 300℃ under various methanol weight hourly space velocity （WHSV） values. During these trials, the catalytic perfor‐mance was assessed, in addition to the formation and function of organic compounds retained in the zeolite. Analysis of reaction effluents and confined organics demonstrated a dual‐cycle reaction mechanism when employing ZSM‐5. The extent of the hydrogen transfer reaction, a secondary reac‐tion in the MTO process, varied as the catalyst‐methanol contact time was changed. In addition, 12C/13C‐methanol switch experiments indicated a relationship between the dual‐cycle mechanism and the extent of the hydrogen transfer reaction. Reactions employing a low methanol WHSV in conjunction with a long contact time favored the hydrogen transfer reaction to give alkene products and promoted the generation and accumulation of retained organic species, such as aromatics and methylcyclopentadienes, which enhance the aromatic cycle. When using higher WHSV values, the reduced contact times lessened the extent of the hydrogen transfer reaction and limited the genera‐tion of methylcyclopentadienes and aromatic species. This suppressed the aromatic cycle, such that the alkene cycle became the dominant route during the MTO reaction.

关键词： methanol to olefins Dual-cycle mechanism ZSM-5 Contact time Hydrogen transfer reaction

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Enhanced MTO performance over acid treated hierarchical SAPO-34

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Chinese Journal of Catalysis 2017年第1期38卷 123-130页

作者： Shu Ren Guojuan Liu Xian Wu Xinqing Chen Minghong Wu Gaofeng Zeng Ziyu Liu Yuhan Sun College of Science Shanghai University Shanghai 201900 China CAS Key Laboratory of Low‐Carbon Conversion Science and Engineering Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201210 China School of Environmental and Chemical Engineering Shanghai University Shanghai 201900 China

Hierarchical SAPO‐34 crystals were synthesized by a facile acid etching post‐treatment. Butterfly‐shaped porous patterns on four side faces and hierarchical pores composed of micropores,mesopores and macropores were formed after a nitric acid or oxalic acid treatment. The catalyticperformance of the hierarchical SAPO‐34 for the methanol to olefins (MTO) process showed that thesynergistic effect of the hierarchical pores and acid sites resulted in a longer catalyst lifetime (from210 to 390 min for the acid treated SAPO‐34) and higher selectivity to light olefins of 92%–94%.The ethylene selectivity can be adjusted between 37.4% and 51.5% by the pore size. No hierarchical SAPO‐34 was obtained after a treatment with butanedioic acid, and with this sample, fast deactivation was detected after 100 min.

关键词： Acid treatment Hierarchical pore SAPO‐34 methanol to olefins Single‐run lifetime

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Charge compensation dominates the distribution of silica in SAPO-34

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Chinese Journal of Catalysis 2016年第2期37卷 227-233页

作者：赵慧茹史淑美吴金雄丁月李牛南开大学材料科学与工程学院新催化材料研究所天津300071 国家新材料科学研究院天津300071

The distribution of Si atoms in the SAPO-34 framework determines its acidity and catalytic *** was investigated using the charge balance between the inorganic framework and trapped template *** types of templates,which yielded R~＋,2R~＋ and 2R^（2＋） positive charges in the cages of SAPO-34,were obtained from single crystal data and they were used to direct the synthesis of SAPO-34 with different Si contents and formation of isolated Si atoms and Si islands in the *** concentration limits of SiO2 in the gel for constituting isolated Si atoms were calculated and verified *** islands,including 5-Si,8-Si,11-Si,14-Si island were described on the basis of host-guest charge *** overall view of the distribution of Si atoms in SAPO-34 was given and a criterion for the strength and density of acid sites in SAPO-34 for it to be an efficient catalyst for MTO was made available.

关键词： SAPO-34 Si distribution Synthesis Silicon island methanol to olefins

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Synthesis and characterization of an unusual snowflake-shaped ZSM-5 zeolite with high catalytic performance in the methanol to olefin reaction

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Chinese Journal of Catalysis 2016年第2期37卷 308-315页

作者：李静刘粟侥张怀科吕恩静任鹏举任杰中国科学院山西煤炭化学研究所煤间接液化国家工程实验室山西太原030001 中国科学院大学北京100049 中科合成油技术有限公司北京101407

The ZSM-5 zeolite with an unusual snowflake-shaped morphology was hydrothermally synthesized for the first time,and compared with common ellipsoidal and boat-like shaped *** samples were characterized by N2 adsorption-desorption,X-ray fluorescence spectroscopy,scanning electron microscopy,X-ray diffraction,magic angle spinning nuclear magnetic resonance,temperature-programmed desorption of ammonia,and infrared spectroscopy of pyridine *** results suggest that the BET surface area and SiO2/Al2O3 ratio of these samples are similar,while the snowflake-shaped ZSM-5 zeolite possesses more of the（101） face,and distortion,dislocation,and asymmetry in the framework,resulting in a larger number of acid sites than the conventional *** for the methanol to olefin（MTO） reaction were prepared by loading Ca on the *** snowflake-shaped Ca/ZSM-5 zeolite exhibited excellent selectivity for total light olefin（72%） and propene（39%） in *** catalytic performance influenced by the morphology can be mainly attributed to the snowflake-shaped ZSM-5 zeolite possessing distortion,dislocation,and asymmetry in the framework,and lower diffusion limitation than the conventional samples.

关键词： ZSM-5 zeolite Modification methanol to olefins

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