The reliance on fossil fuels intensifies CO_(2) emissions,worsening political and environmental challenges.CO_(2) capture and conversion present a promising solution,influenced by industrialization and urbanization.In...The reliance on fossil fuels intensifies CO_(2) emissions,worsening political and environmental challenges.CO_(2) capture and conversion present a promising solution,influenced by industrialization and urbanization.In recent times,catalytic conversion of CO_(2) into fuels and chemical precursors,particularly methane,are gaining traction for establishing a sustainable,carbon-neutral economy due to methane’s advantages in renewable energy applications.Though homogeneous and heterogeneous catalysts are available for the conversion of CO_(2) to methane,the efficiency is found to be higher in heterogeneous catalysts.Therefore,this review focuses only on the heterogeneous catalysts.In this context,the efficient heterogeneous catalysts with optimum utility are yet to be obtained.Therefore,the quest for suitable catalyst for the catalytic conversion of CO_(2) to CH4 is still continuing and designing efficient catalysts requires assessing their synthetic feasibility,often achieved through computational methods like density functional theory simulations,providing insights into reaction mechanisms,rate-limiting steps,catalytic cycle,activation of C=O bonds and enhancing understanding while lowering costs.In this context,this review examines the conversion of CO_(2) to CH4 using seven distinct types of catalysts,including single and double atom catalysts,metal organic frameworks,metalloporphyrins,graphdiyne and graphitic carbon nitrite and alloys with some case studies.The main focus of this review is to offer a detailed and extensive examination of diverse catalyst design approaches and their utilization in CH4 production,with a specific emphasis on computational aspects.It explores the array of design methodologies used to identify reaction pathways and investigates the critical role of computational tools in their refinement and enhancement.We believe this review will help budding researchers to explore the possibilities of designing catalysts for the CO_(2) to CH4 conversion from computational framework.展开更多
Zeolites catalyzed methanol-to-olefins （MTO） conversion provides an alternative process to produce light olefins such as ethene and propene from nonpetroleum resources. Despite of successful industrialization of the...Zeolites catalyzed methanol-to-olefins （MTO） conversion provides an alternative process to produce light olefins such as ethene and propene from nonpetroleum resources. Despite of successful industrialization of the MTO process, its detailed reaction mechanism is not yet well understood. Here we summarize our work on the hydrocarbon pool reaction mechanism based on theoretical calculations. We proposed that the olefins themselves are likely to be the dominating hydrocarbon pool species, and the distribution of cracking precursors and diffusion constraints affect the selectivity. The similarities between aromatic-based and olefin-based cycles are highlighted.展开更多
基金National Key Research and Development Program of China(Grant No.2022YFE0208400).
文摘The reliance on fossil fuels intensifies CO_(2) emissions,worsening political and environmental challenges.CO_(2) capture and conversion present a promising solution,influenced by industrialization and urbanization.In recent times,catalytic conversion of CO_(2) into fuels and chemical precursors,particularly methane,are gaining traction for establishing a sustainable,carbon-neutral economy due to methane’s advantages in renewable energy applications.Though homogeneous and heterogeneous catalysts are available for the conversion of CO_(2) to methane,the efficiency is found to be higher in heterogeneous catalysts.Therefore,this review focuses only on the heterogeneous catalysts.In this context,the efficient heterogeneous catalysts with optimum utility are yet to be obtained.Therefore,the quest for suitable catalyst for the catalytic conversion of CO_(2) to CH4 is still continuing and designing efficient catalysts requires assessing their synthetic feasibility,often achieved through computational methods like density functional theory simulations,providing insights into reaction mechanisms,rate-limiting steps,catalytic cycle,activation of C=O bonds and enhancing understanding while lowering costs.In this context,this review examines the conversion of CO_(2) to CH4 using seven distinct types of catalysts,including single and double atom catalysts,metal organic frameworks,metalloporphyrins,graphdiyne and graphitic carbon nitrite and alloys with some case studies.The main focus of this review is to offer a detailed and extensive examination of diverse catalyst design approaches and their utilization in CH4 production,with a specific emphasis on computational aspects.It explores the array of design methodologies used to identify reaction pathways and investigates the critical role of computational tools in their refinement and enhancement.We believe this review will help budding researchers to explore the possibilities of designing catalysts for the CO_(2) to CH4 conversion from computational framework.
文摘Zeolites catalyzed methanol-to-olefins （MTO） conversion provides an alternative process to produce light olefins such as ethene and propene from nonpetroleum resources. Despite of successful industrialization of the MTO process, its detailed reaction mechanism is not yet well understood. Here we summarize our work on the hydrocarbon pool reaction mechanism based on theoretical calculations. We proposed that the olefins themselves are likely to be the dominating hydrocarbon pool species, and the distribution of cracking precursors and diffusion constraints affect the selectivity. The similarities between aromatic-based and olefin-based cycles are highlighted.
