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| 1 | Cavity-controlled methanol conversion over zeolite catalysts显示文摘The successful development and application in industry of methanol-to-olefins(MTO)process brought about an innovative and efficient route for olefin production via non-petrochemical resources and also attracted attention of C1 chemistry and zeolite catalysis.Molecular sieve catalysts with diversified microenvironments embedding unique channel/cavity structure and acid properties,exhibit demonstrable features and advantages in the shape-selective catalysis of MTO.Especially,shape-selective catalysis over 8-MR and cavity-type zeolites with acidic supercage environment and narrow pore opening manifested special host–guest interaction between the zeolite catalyst and guest reactants,intermediates and products.This caused great differences in product distribution,catalyst deactivation and molecular diffusion,revealing the cavity-controlled methanol conversion over 8-MR and cavity-type zeolite catalyst.Furthermore,the dynamic and complicated cross-talk behaviors of catalyst material(coke)-reaction-diffusion over these types of zeolites determines the catalytic performance of the methanol conversion.In this review,we shed light on the cavity-controlled principle in the MTO reaction including cavity-controlled active intermediates formation,cavity-controlled reaction routes with the involvement of these intermediates in the complex reaction network,cavity-controlled catalyst deactivation and cavity-controlled diffusion.All these were exhibited by the MTO reaction performances and product selectivity over 8-MR and cavity-type zeolite catalysts.Advanced strategies inspired by the cavity-controlled principle were developed,providing great promise for the optimization and precise control of MTO process. | Wenna Zhang Shanfan Lin Yingxu Wei Peng Tian Mao Ye Zhongmin Liu | 2023 | National Science Review2023，10，9： | 0 |
| 2 | Multiscale dynamical cross-talk in zeolite-catalyzed methanol and dimethyl ether conversions显示文摘Establishing a comprehensive understanding of the dynamical multiscale diffusion and reaction process is crucial for zeolite shape-selective catalysis and is urgently demanded in academia and industry.So far,diffusion and reaction for methanol and dimethyl ether(DME)conversions have usually been studied separately and focused on a single scale.Herein,we decipher the dynamical molecular diffusion and reaction process for methanol and DME conversions within the zeolite material evolving with time,at multiple scales,from the scale of molecules to single catalyst crystal and catalyst ensemble.Microscopic intracrystalline diffusivity is successfully decoupled from the macroscopic experiments and verified by molecular dynamics simulation.Spatiotemporal analyses of the confined carbonaceous species allow us to track the migratory reaction fronts in a single catalyst crystal and the catalyst ensemble.The constrained diffusion of DME relative to methanol alleviates the high local chemical potential of the reactant by attenuating its local enrichment,enhancing the utilization efficiency of the inner active sites of the catalyst crystal.In this context,the dynamical cross-talk behaviors of material,diffusion and reaction occurring at multiple scales is uncovered.Zeolite catalysis not only reflects the reaction characteristics of heterogeneous catalysis,but also provides enhanced,moderate or suppressed local reaction kinetics through the special catalytic micro-environment,which leads to the heterogeneity of diffusion and reaction at multiple scales,thereby realizing efficient and shape-selective catalysis. | Shanfan Lin Yuchun Zhi Zhiqiang Liu Jiamin Yuan Wenjuan Liu Wenna Zhang Zhaochao Xu Anmin Zheng Yingxu Wei Zhongmin Liu | 2022 | National Science Review2022，9，9： | 0 |
| 3 | Coking and decoking chemistry for resource utilization of polycyclic aromatic hydrocarbons(PAHs)and low-carbon process显示文摘Low-carbon process for resource utilization of polycyclic aromatic hydrocarbons(PAHs)in zeolitecatalyzed processes,geared to carbon neutrality-a prominent trend throughout human activities,has been bottlenecked by the lack of a complete mechanistic understanding of coking and decoking chemistry,involving the speciation and molecular evolution of PAHs,the plethora of which causes catalyst deactivation and forces regeneration,rendering significant CO_(2) emission.Herein,by exploiting the high-resolution matrix-assisted laser desorption/ionization Fourier-transform ion cyclotron resonance mass spectrometry(MALDI FT-ICR MS),we unveil the missing fingerprints of the mechanistic pathways for both formation and decomposition of cross-linked cage-passing PAHs for SAPO-34-catalyzed,industrially relevant methanol-to-olefins(MTO)as a model reaction.Notable is the molecule-resolved symmetrical signature:their speciation originates exclusively from the direct coupling of in-cage hydrocarbon pool(HCP)species,whereas water-promoted decomposition of cage-passing PAHs initiates with selective cracking of inter-cage local structures at 8-rings followed by deep aromatic steam reforming.Molecular deciphering the reversibly dynamic evolution trajectory(fate)of full-spectrum aromatic hydrocarbons and fulfilling the real-time quantitative carbon resource footprints advance the fundamental knowledge of deactivation and regeneration phenomena(decay and recovery motifs of autocatalysis)and disclose the underlying mechanisms of especially the chemistry of coking and decoking in zeolite catalysis.The positive yet divergent roles of water in these two processes are disentangled.These unprecedented insights ultimately lead us to a steam regeneration strategy with valuable CO and H_(2) as main products,negligible CO_(2) emission in steam reforming and full catalyst activity recovery,which further proves feasible in other important chemical processes,promising to be a sustainable and potent approach that contributes to carbon-neutral chemical industry. | Nan Wang Li Wang Yuchun Zhi Jingfeng Han Chengwei Zhang Xinqiang Wu Jinling Zhang Linying Wang Benhan Fan Shutao Xu Yijun Zheng Shanfan Lin Renan Wu Yingxu Wei Zhongmin Liu | 2023 | Journal of Energy Chemistry2023，，1： | 0 |
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