Multiscale spatiotemporal heterogeneity of zeolite-catalyzed methanol-to-hydrocarbons reactionOA
The methanol-to-hydrocarbons(MTH)process provides a sustainable route to light olefins,aromatics,and gasoline-range products with methanol synthesized via syngas platform molecules obtained from nonpetroleum alternative feedstocks,such as coal,biomass,and natural gas.Zeolite-catalyzed MTH reactions inherently exhibit multiscale heterogeneity,which is intrinsically linked to the rational design of high-efficiency industrial catalysts and the regulation of product selectivity.Despite extensive research on zeolite-based MTH catalysis,most studies focused on a single scale and a multiscale understanding that connects molecular-scale,crystal-scale,particle-scale,and reactor-scale performance remains elusive.This review integrates recent advances in spectroscopic characterization,molecular imaging,and spatially resolved techniques to dissect the heterogeneity of the MTH reaction(i.e.from molecular diffusion to acidity,temperature distribution,and coke deposition)across four levels and to clarify how these nonuniform microenvironments emerge,interact,and propagate.By integrating insights across these four scales,we aim to bridge micro-(molecule)and macro-processes(reactor),summarize both the adverse and favorable effects of multiscale heterogeneity in zeolite‑catalyzed processes,reveal spatiotemporal heterogeneity as the intrinsic and crucial principle of MTH reaction over zeolites,and expect this knowledge to provide theoretical support for the rational design of new-generation high-efficiency catalysts,enabling a more effective and selective MTH process.
Jinxi Hou;Yiyao Chen;Yiming Liu;Yuchun Zhi;Yingxu Wei;Zhongmin Liu
Dalian National Laboratory for Clean Energy,National Engineering Research Center of Lower-Carbon Catalysis Technology,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China Energy College,University of Chinese Academy of Sciences,Beijing 100049,ChinaDalian National Laboratory for Clean Energy,National Engineering Research Center of Lower-Carbon Catalysis Technology,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China Energy College,University of Chinese Academy of Sciences,Beijing 100049,ChinaDalian National Laboratory for Clean Energy,National Engineering Research Center of Lower-Carbon Catalysis Technology,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China Energy College,University of Chinese Academy of Sciences,Beijing 100049,ChinaDalian National Laboratory for Clean Energy,National Engineering Research Center of Lower-Carbon Catalysis Technology,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China Energy College,University of Chinese Academy of Sciences,Beijing 100049,ChinaDalian National Laboratory for Clean Energy,National Engineering Research Center of Lower-Carbon Catalysis Technology,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China Energy College,University of Chinese Academy of Sciences,Beijing 100049,ChinaDalian National Laboratory for Clean Energy,National Engineering Research Center of Lower-Carbon Catalysis Technology,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China Energy College,University of Chinese Academy of Sciences,Beijing 100049,China
化学化工
MTHzeolitediffusionmultiscalespatiotemporal heterogeneity
《National Science Review》 2026 (12)
P.282-304,23
supported by the National Key R&D Program of China(2024YFB4105401)the National Natural Sci-ence Foundation of China(U25A20555,22372164,U25D9013,22288101 and 22072148).
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