Carbon dioxide hydrogenation to gasoline can effectively alleviate the energy crisis and benefit the global environment.Owing to its orthogonally connected nanosheet configuration,large pore volume,and appropriate thi...Carbon dioxide hydrogenation to gasoline can effectively alleviate the energy crisis and benefit the global environment.Owing to its orthogonally connected nanosheet configuration,large pore volume,and appropriate thickness of single nanosheet,self-pillared pentasil(SPP)nanosheet zeolite is integrated with In_(2)O_(3)-ZrO_(2)as a tandem catalyst for CO_(2)hydrogenation to C_(5+)hydrocarbons.By substituting Al in the SPP framework with Ga,the acid strength of SPP is reduced,and acid density is increased,which favors the generation of C_(5+)hydrocarbons and enhances the cracking resistance of long-chain hydrocarbons.A maximum C_(5+)hydrocarbon selectivity of 82%was obtained on In_(2)O_(3)-ZrO_(2)/Ga-SPP(Si/Ga=100),which shows no deactivation after 200 h reaction time.Furthermore,introducing Pd into the In_(2)O_(3)-ZrO_(2)not only boosts CO_(2)conversion to 11%but also suppresses methane selectivity to below 1%.This study offers valuable insights into the design of highly active CO_(2)-to-gasoline catalysts by leveraging the distinctive structure and acidity of zeolites within the tandem catalyst systems.展开更多
基金financially supported by the National Key Research and Development Program of China(2024YFB4105401)the National Natural Science Foundation of China(22472017)+1 种基金the Liaoning Binhai Laboratory(LBLG-2024-06)the Fundamental Research Funds for the Central Universities(DUT22LAB602and DUT24RC(3)071)。
文摘Carbon dioxide hydrogenation to gasoline can effectively alleviate the energy crisis and benefit the global environment.Owing to its orthogonally connected nanosheet configuration,large pore volume,and appropriate thickness of single nanosheet,self-pillared pentasil(SPP)nanosheet zeolite is integrated with In_(2)O_(3)-ZrO_(2)as a tandem catalyst for CO_(2)hydrogenation to C_(5+)hydrocarbons.By substituting Al in the SPP framework with Ga,the acid strength of SPP is reduced,and acid density is increased,which favors the generation of C_(5+)hydrocarbons and enhances the cracking resistance of long-chain hydrocarbons.A maximum C_(5+)hydrocarbon selectivity of 82%was obtained on In_(2)O_(3)-ZrO_(2)/Ga-SPP(Si/Ga=100),which shows no deactivation after 200 h reaction time.Furthermore,introducing Pd into the In_(2)O_(3)-ZrO_(2)not only boosts CO_(2)conversion to 11%but also suppresses methane selectivity to below 1%.This study offers valuable insights into the design of highly active CO_(2)-to-gasoline catalysts by leveraging the distinctive structure and acidity of zeolites within the tandem catalyst systems.
