Spatially confined microenvironments offer exceptional potential for regulating catalytic activity and selectivity.This study elucidates how the dynamic evolution of carbonaceous species during syngas conversion alter...Spatially confined microenvironments offer exceptional potential for regulating catalytic activity and selectivity.This study elucidates how the dynamic evolution of carbonaceous species during syngas conversion alters the confined environment within MCM-22 cages.We establish a confinement energy,quantified through ethylene adsorption measurements,as a key descriptor correlating with hydrogenation activity at Brönsted acid sites.As carbonaceous deposits expand in size during syngas reaction,they progressively occupy cage volume and reduce the available space,thereby enhancing confinement energy.Such energy gain universally weakens reactant adsorption,simultaneously suppressing hydrogenation activity and promoting olefin selectivity.Collectively,these findings advance fundamental understanding of dynamic confinement effects and provide valuable insights for further designing high-selectivity catalysts for syngas conversion.展开更多
摘要Spatially confined microenvironments offer exceptional potential for regulating catalytic activity and selectivity.This study elucidates how the dynamic evolution of carbonaceous species during syngas conversion alters the confined environment within MCM-22 cages.We establish a confinement energy,quantified through ethylene adsorption measurements,as a key descriptor correlating with hydrogenation activity at Brönsted acid sites.As carbonaceous deposits expand in size during syngas reaction,they progressively occupy cage volume and reduce the available space,thereby enhancing confinement energy.Such energy gain universally weakens reactant adsorption,simultaneously suppressing hydrogenation activity and promoting olefin selectivity.Collectively,these findings advance fundamental understanding of dynamic confinement effects and provide valuable insights for further designing high-selectivity catalysts for syngas conversion.