Syngas to aromatics(STA)over bifunctional catalysts has attracted much attention in recent years,but the mechanism underlying the formation of aromatics remains controversial.The critical reaction intermediates,carbox...Syngas to aromatics(STA)over bifunctional catalysts has attracted much attention in recent years,but the mechanism underlying the formation of aromatics remains controversial.The critical reaction intermediates,carboxylates,were first identified and then confirmed to essentially promote aromatization in the syngas conversion over a ZnCrAlO_(x)&H-ZSM-5 composite catalyst.This study provides evidence that the carboxylates can be formed during the reactions of formate species and olefins.In addition,it is shown that the carboxylates favor the formation of aromatics over H-ZSM-5 even in the presence of H2.A novel mechanism for the formation of aromatics via the generation and transformation of carboxylate intermediates is proposed,and the transformation of carboxylates to aromatics via methyl-2-cyclopenten-1-one(MCPO)intermediates is indeed likely.A better understanding of the formation mechanism of aromatics would help optimize the composite catalyst.展开更多
Over the past decade,electrocatalytic reduction of CO_(2)has gained substantial attention.However,hardly any of the previous reviews have focused on the systematic discussion of polymer-molecular catalyst composites a...Over the past decade,electrocatalytic reduction of CO_(2)has gained substantial attention.However,hardly any of the previous reviews have focused on the systematic discussion of polymer-molecular catalyst composites as an emerging system for the electrochemical transformation of CO_(2)to value-added products.In this review,we first give a brief overview of the general features of solid-state and molecular catalysts,and then advance the discussion to polymer-catalyst composite systems,with particular emphasis on polymer-encapsulated molecular catalysts,where the coordination environment surrounding molecular catalysts can be modified via polymer encapsulation to promote the overall performance of CO_(2)electrocatalysis.The elucidation of the possible reaction mechanisms of this emerging electrocat-alytic system along with proposed optimization strategies is also summarized and discussed based on recently published reports,followed by the challenges and prospects of their industrial applications at the end of this review.From this review,we hope the audience can gain a comprehensive understanding of the electrocatalytic mechanism of the coordinating polymers and valuable insights into engineering the microenvironment surrounding the metal complexes for potential future research directions.展开更多
文摘Syngas to aromatics(STA)over bifunctional catalysts has attracted much attention in recent years,but the mechanism underlying the formation of aromatics remains controversial.The critical reaction intermediates,carboxylates,were first identified and then confirmed to essentially promote aromatization in the syngas conversion over a ZnCrAlO_(x)&H-ZSM-5 composite catalyst.This study provides evidence that the carboxylates can be formed during the reactions of formate species and olefins.In addition,it is shown that the carboxylates favor the formation of aromatics over H-ZSM-5 even in the presence of H2.A novel mechanism for the formation of aromatics via the generation and transformation of carboxylate intermediates is proposed,and the transformation of carboxylates to aromatics via methyl-2-cyclopenten-1-one(MCPO)intermediates is indeed likely.A better understanding of the formation mechanism of aromatics would help optimize the composite catalyst.
基金supported by the National Energy R&D Center of Petroleum Refining Technology(RIPP,SINOPEC)the National Key R&D Program of China(Nos.2021YFE0191200 and 2022YFA1504200).
文摘Over the past decade,electrocatalytic reduction of CO_(2)has gained substantial attention.However,hardly any of the previous reviews have focused on the systematic discussion of polymer-molecular catalyst composites as an emerging system for the electrochemical transformation of CO_(2)to value-added products.In this review,we first give a brief overview of the general features of solid-state and molecular catalysts,and then advance the discussion to polymer-catalyst composite systems,with particular emphasis on polymer-encapsulated molecular catalysts,where the coordination environment surrounding molecular catalysts can be modified via polymer encapsulation to promote the overall performance of CO_(2)electrocatalysis.The elucidation of the possible reaction mechanisms of this emerging electrocat-alytic system along with proposed optimization strategies is also summarized and discussed based on recently published reports,followed by the challenges and prospects of their industrial applications at the end of this review.From this review,we hope the audience can gain a comprehensive understanding of the electrocatalytic mechanism of the coordinating polymers and valuable insights into engineering the microenvironment surrounding the metal complexes for potential future research directions.
