The electrochemical reduction of CO_(2)(eCO_(2)R)under ambient conditions is crucial for reducing carbon emissions and achieving carbon neutrality.Despite progress with alkaline and neutral electrolytes,their efficien...The electrochemical reduction of CO_(2)(eCO_(2)R)under ambient conditions is crucial for reducing carbon emissions and achieving carbon neutrality.Despite progress with alkaline and neutral electrolytes,their efficiency is limited by(bi)carbonates formation.Acidic media have emerged as a solution,addressing the(bi)carbonates challenge but introducing the issue of the hydrogen evolu-tion reaction(HER),which reduces CO_(2) conversion efficiency in acidic environments.This review focuses on enhancing the selectivity of acidic CO_(2) electrolysis.It commences with an overview of the latest advancements in acidic CO_(2) electrolysis,focusing on product selectivity and electrocatalytic activity enhancements.It then delves into the critical factors shaping selectivity in acidic CO_(2) electrolysis,with a special emphasis on the influence of cations and catalyst design.Finally,the research challenges and personal perspectives of acidic CO_(2) electrolysis are suggested.展开更多
Infrared photodissociation spectroscopy of mass-selected[MO(CO2)n]^+(M=Sc,Y,La)complexes indicates that the conversion from the solvated structure into carbonate one can be achieved by the ScO^+ cation at n=5 and by t...Infrared photodissociation spectroscopy of mass-selected[MO(CO2)n]^+(M=Sc,Y,La)complexes indicates that the conversion from the solvated structure into carbonate one can be achieved by the ScO^+ cation at n=5 and by the YO^+ cation at n=4,while only the solvated structures are observed for the LaO^+ cation.These findings suggest that both the ScO^+ and YO^+cations are able to fix CO2 into carbonate.Quantum chemical calculations are performed on[MO(CO2)n]^+ to identify the structures of the low-lying isomers and to assign the observed spectral features.Theoretical analyses show that the[YO(CO2)n]^+ complex has the smallest barrier for the conversion from the solvated structure into carbonate one,while[LaO(CO2)n]^+ exhibits the largest conversion barrier among the three metal oxide cations.The present system affords a model in clarifying the effect of different metals in catalytic CO2 transformation at the molecular level.展开更多
Our experimental progresses on the reaction dynamics of dissociative electron attachment(DEA)to carbon dioxide(CO2)are summarized in this review.First,we introduce some fundamentals about the DEA dynamics and provide ...Our experimental progresses on the reaction dynamics of dissociative electron attachment(DEA)to carbon dioxide(CO2)are summarized in this review.First,we introduce some fundamentals about the DEA dynamics and provide an epitome about the DEAs to CO2.Second,the experimental technique developments are described,in particular,on the highresolution velocity map imaging apparatus in which we put a lot of efforts during the past two years.Third,our findings about the DEA dynamics of CO2 are surveyed and briefly compared with the others’work.At last,we give a perspective about the applications of the DEA studies and highlight the inspirations in the production of molecular oxygen on Mars and the catalytic transformations of CO2.展开更多
The mass-selected infrared photodissociation (IRPD) spectroscopy was utilized to investigate the interactions of cationic cobalt with carbon dioxide molecules. Quantum chemical calculations were performed on the [Co(C...The mass-selected infrared photodissociation (IRPD) spectroscopy was utilized to investigate the interactions of cationic cobalt with carbon dioxide molecules. Quantum chemical calculations were performed on the [Co(CO2)n]^+ clusters to identify the structures of the low-lying isomers and to assign the observed spectral features. All the [Co(CO2)n]^+(n=2-6) clusters studied here show resonances near the CO2 asymmetric stretch of free CO2 molecule. Experimental and calculated results indicate that the CO2 molecules are weakly bound to the Co+ cations in an end-on con guration via a charge-quadrupole electrostatic interaction. The present IRPD spectra of [Co(CO2)n]^+ clusters have been compared to those of Ar-tagged species ([Co(CO2)n]^+-Ar), which would provide insights into the tagging effect of rare gas on the weakly-bounded clusters.展开更多
基金Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China (51888103)National Natural Science Foundation of China (52006103)Fundamental Research Funds of the Central Universities (30919011403, 30920021137)。
文摘The electrochemical reduction of CO_(2)(eCO_(2)R)under ambient conditions is crucial for reducing carbon emissions and achieving carbon neutrality.Despite progress with alkaline and neutral electrolytes,their efficiency is limited by(bi)carbonates formation.Acidic media have emerged as a solution,addressing the(bi)carbonates challenge but introducing the issue of the hydrogen evolu-tion reaction(HER),which reduces CO_(2) conversion efficiency in acidic environments.This review focuses on enhancing the selectivity of acidic CO_(2) electrolysis.It commences with an overview of the latest advancements in acidic CO_(2) electrolysis,focusing on product selectivity and electrocatalytic activity enhancements.It then delves into the critical factors shaping selectivity in acidic CO_(2) electrolysis,with a special emphasis on the influence of cations and catalyst design.Finally,the research challenges and personal perspectives of acidic CO_(2) electrolysis are suggested.
基金supported by the National Natural Science Foundation of China (No.21327901,No.21673231,No.21673234,and No.21688102)the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB17000000)K. C. Wong Education Foundation.
文摘Infrared photodissociation spectroscopy of mass-selected[MO(CO2)n]^+(M=Sc,Y,La)complexes indicates that the conversion from the solvated structure into carbonate one can be achieved by the ScO^+ cation at n=5 and by the YO^+ cation at n=4,while only the solvated structures are observed for the LaO^+ cation.These findings suggest that both the ScO^+ and YO^+cations are able to fix CO2 into carbonate.Quantum chemical calculations are performed on[MO(CO2)n]^+ to identify the structures of the low-lying isomers and to assign the observed spectral features.Theoretical analyses show that the[YO(CO2)n]^+ complex has the smallest barrier for the conversion from the solvated structure into carbonate one,while[LaO(CO2)n]^+ exhibits the largest conversion barrier among the three metal oxide cations.The present system affords a model in clarifying the effect of different metals in catalytic CO2 transformation at the molecular level.
基金supported by the National Natural Science Foundation of China(No.21727804,No.21625301,No.21273213)。
文摘Our experimental progresses on the reaction dynamics of dissociative electron attachment(DEA)to carbon dioxide(CO2)are summarized in this review.First,we introduce some fundamentals about the DEA dynamics and provide an epitome about the DEAs to CO2.Second,the experimental technique developments are described,in particular,on the highresolution velocity map imaging apparatus in which we put a lot of efforts during the past two years.Third,our findings about the DEA dynamics of CO2 are surveyed and briefly compared with the others’work.At last,we give a perspective about the applications of the DEA studies and highlight the inspirations in the production of molecular oxygen on Mars and the catalytic transformations of CO2.
基金supported by the National Natural Science Foundation of China(No.21327901,No.21503222,No.21673231,and No.21688102)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB17000000)China Postdoctoral Science Foundation(No.2018M641718 and No.2018M641719)
文摘The mass-selected infrared photodissociation (IRPD) spectroscopy was utilized to investigate the interactions of cationic cobalt with carbon dioxide molecules. Quantum chemical calculations were performed on the [Co(CO2)n]^+ clusters to identify the structures of the low-lying isomers and to assign the observed spectral features. All the [Co(CO2)n]^+(n=2-6) clusters studied here show resonances near the CO2 asymmetric stretch of free CO2 molecule. Experimental and calculated results indicate that the CO2 molecules are weakly bound to the Co+ cations in an end-on con guration via a charge-quadrupole electrostatic interaction. The present IRPD spectra of [Co(CO2)n]^+ clusters have been compared to those of Ar-tagged species ([Co(CO2)n]^+-Ar), which would provide insights into the tagging effect of rare gas on the weakly-bounded clusters.
