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Dynamic confinement of SAPO-17 cages on the selectivity control of syngas conversion

National Science Review 2022年第9期9卷 40-46页

作者： Haodi Wang Feng Jiao Yi Ding Wenjuan Liu Zhaochao Xu Xiulian Pan Xinhe Bao State Key Laboratory of Catalysis 2011-Collaborative Innovation Center of Chemistry for Energy Materials Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences Department of Chemical Physics University of Science and Technology of China Key Laboratory of Separation Science for Analytical Chemistry Dalian Institute of Chemical Physics Chinese Academy of Sciences

The OXZEO(oxide-zeolite) bifunctional catalyst concept has enabled selective syngas conversion to a series of value-added chemicals and fuels such as light olefins,aromatics and gasoline.Herein we report for the first time a dynamic confinement of SAPO-17 cages on the selectivity control of syngas conversion observed during an induction period.Structured illumination microscopy,intelligent gravimetric analysis,UV-Raman,X-ray diffraction,thermogravimetry and gas chromatography-mass spectrometer analysis indicate that this is attributed to the evolution of carbonaceous species as the reaction proceeds,which gradually reduces the effective space inside the cage.Consequently,the difusion of molecules is hindered and the hindering is much more prominent for larger molecules such as C4+.As a result,the selectivity of ethylene is enhanced whereas that of C4+is suppressed.Beyond the induction period,the product selectivity levels off.For instance, ethylene selectivity levels off at 44% and propylene selectivity at 31 %,as well as CO conversion at 27%.The findings here bring a new fundamental understanding that will guide further development of selective catalysts for olefin synthesis based on the OXZEO concept.

关键词： syngas conversion OXZEO dynamic confinement zeolite diffusion

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SAPO-34 facilitates the formation of benzene,toluene and xylenes in direct syngas conversion over MnCrO_(x)-SAPO-34-ZSM-5

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Science China Chemistry 2024年第2期67卷 732-740页

作者： Shuchi Zhang Dengyun Miao Yi Ding Mengyuan Li Shujing Guo Yujuan Zhang Xiulian Pan Xinhe Bao State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China University of Chinese Academy of Sciences Beijing100049China Shaanxi Yanchang Petroleum(Group)Co. Ltd.&Dalian Institute of Chemical Physics Xi’an Clean Energy(Chemical Industry)Research InstituteXi’an710000China

Direct conversion of syngas to aromatics over metal oxide and zeolite(OXZEO) composite catalysts is promising.However,the selectivity of more valuable products such as benzene,toluene and xylenes(BTX) is limited due to undesired secondary methylation of BTX.Herein,we report that the introduction of SAPO-34 into MnCrO_(x)-ZSM-5 catalyst enhances significantly the formation of BTX without sacrificing the aromatics selectivity.Under optimized conditions,the fraction of BTX in aromatics reaches 64.7% versus 28.9% over the catalyst without SAPO-34.A number of model reaction tests and characterizations reveal that SAPO-34 consumes partially the intermediates such as ketene,by converting them to light olefins.Thus,the methylation of BTX by ketene to heavy aromatics is inhibited over the external acid sites of ZSM-5,leading to an enhanced BTX selectivity in the products.This hybrid catalyst provides an efficient method for highly selective synthesis of BTX from syngas.

关键词： selective syngas conversion OXZEO aromatics BTX multi-functional catalysts

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Modulated hydrocarbon distribution of gasoline deriving from butene conversion in the presence of syngas

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Journal of Energy Chemistry 2022年第10期31卷 416-421,I0010页

作者： Yi Ding Feng Jiao Xiulian Pan Xinhe Bao Department of Chemical Physics University of Science and Technology of ChinaHefei 230026AnhuiChina State Key Laboratory of Catalysis Dalian National Laboratory for Clean Energy2011-Collaborative Innovation Center of Chemistry for Energy MaterialsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

With the expansion of butene production capacity,clean and efficient conversion of mixed butene attracts increasing attention.Herein we report direct co-conversion of butene and syngas to highquality gasoline enabled by a bifunctional OXZEO catalyst comprising ZnCrO_(x) oxide and ZSM-5 zeolite.A gasoline selectivity of 71.6% at 98.1% butene conversion and 26.2% CO conversion have been obtained under the reaction conditions of 360℃,3 MPa and 3000 mL g^(-1) h^(-1).The space time yield of gasoline of0.25 g·g^(-1) h^(-1) is achieved.Interestingly,the presence of syngas can effectively facilitate iso-paraffin production while hindering the formation of aromatics.This is attributed to the prohibited hydrogen transfer aromatization process of butene on ZSM-5 in the presence of H2.Fu rthermore,the formation of isomers of gasoline range hydrocarbons is favored because the active intermediates generated from CO/H_(2) activation over ZnCrO_(x) oxide could react with butene over ZSM-5 zeolite.Thus,the product distribution among gasoline range hydrocarbons is modulated with reduced heavy aromatics and improved iso-paraffins,which is desirable for application as fuels.This provides an alternative environmentally friendly technology to utilize still increasing mixed butene.

关键词： Butene utilization Bifunctional catalysts OXZEO Syngas conversion Gasoline

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