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
A novel technology of preparing zeolites based on solid-solid mass transformation mechanism is developed for the first time. By employing this technology, three different types of highly crystallized pentasil zeolites...A novel technology of preparing zeolites based on solid-solid mass transformation mechanism is developed for the first time. By employing this technology, three different types of highly crystallized pentasil zeolites, ZSM-35 (FER-type), Silicalite-1(MFI-type) and Mordenite(MOR-type), are successfully synthesized in the solid system. In terms of commercial production, the technology-could simplify synthesis procedure and make the continuous production of zeolites possible, so as to improve the productivity. Additionally, it is environmentally friendly because the crystallization occurs in solid phase where there exists no pollution caused by waste liquid. Therefore, this technique provides us with a new industrial process for the clean and continuous production of zeolites. The characteristics in synthesis chemistry and the crystallization mechanism involved in the technology are also discussed.展开更多
Identification of the catalyst characteristics correlating with the key performance parameters including selectivity and stability is key to the rational catalyst design. Herein we focused on the identification of pro...Identification of the catalyst characteristics correlating with the key performance parameters including selectivity and stability is key to the rational catalyst design. Herein we focused on the identification of property-performance relationships in the methanol-to-olefin(MTO) process by studying in detail the catalytic behaviour of MFI, MEL and their respective intergrowth zeolites. The detailed material characterization reveals that both the high production of propylene and butylenes and the large Me OH conversion capacity correlate with the enrichment of lattice Al sites in the channels of the pentasil structure as identified by 27 Al MAS NMR and 3-methylpentane cracking results. The lack of correlation between MTO performance and other catalyst characteristics, such as crystal size, presence of external Brønsted acid sites and Al pairing suggests their less pronounced role in defining the propylene selectivity. Our analysis reveals that catalyst deactivation is rather complex and is strongly affected by the enrichment of lattice Al in the intersections, the overall Al-content, and crystal size. The intergrowth of MFI and MEL phases accelerates the catalyst deactivation rate.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.
基金Supported by the National Natural Science Foundation of China (No.20173039) and by China National Petroleum Corporation (No.2002B50501)
文摘A novel technology of preparing zeolites based on solid-solid mass transformation mechanism is developed for the first time. By employing this technology, three different types of highly crystallized pentasil zeolites, ZSM-35 (FER-type), Silicalite-1(MFI-type) and Mordenite(MOR-type), are successfully synthesized in the solid system. In terms of commercial production, the technology-could simplify synthesis procedure and make the continuous production of zeolites possible, so as to improve the productivity. Additionally, it is environmentally friendly because the crystallization occurs in solid phase where there exists no pollution caused by waste liquid. Therefore, this technique provides us with a new industrial process for the clean and continuous production of zeolites. The characteristics in synthesis chemistry and the crystallization mechanism involved in the technology are also discussed.
基金supported by the BASF and the Advanced Research Center Chemical Building Blocks Consortium (ARC CBBC) for Funding under Project (2016.007.TUD)
文摘Identification of the catalyst characteristics correlating with the key performance parameters including selectivity and stability is key to the rational catalyst design. Herein we focused on the identification of property-performance relationships in the methanol-to-olefin(MTO) process by studying in detail the catalytic behaviour of MFI, MEL and their respective intergrowth zeolites. The detailed material characterization reveals that both the high production of propylene and butylenes and the large Me OH conversion capacity correlate with the enrichment of lattice Al sites in the channels of the pentasil structure as identified by 27 Al MAS NMR and 3-methylpentane cracking results. The lack of correlation between MTO performance and other catalyst characteristics, such as crystal size, presence of external Brønsted acid sites and Al pairing suggests their less pronounced role in defining the propylene selectivity. Our analysis reveals that catalyst deactivation is rather complex and is strongly affected by the enrichment of lattice Al in the intersections, the overall Al-content, and crystal size. The intergrowth of MFI and MEL phases accelerates the catalyst deactivation rate.
