Carrier dynamics and surface reaction are two critical processes for determining the performance of photocatalytic reaction.Highly designable polymer-based photocatalysts have shown promising protectives in energetic ...Carrier dynamics and surface reaction are two critical processes for determining the performance of photocatalytic reaction.Highly designable polymer-based photocatalysts have shown promising protectives in energetic and environmental applications.In this prospective,we first distinguished the differences of physiochemical properties between polymer-based semiconductors and traditional inorganic semiconductors.Then,the effects of single-atom sites on the charge dynamics and reaction kinetics of polymer-based photocatalysts are further elaborated.Time(excitation)-space(wavefunction)population analysis,which can provide relevant information to clarify the structure-excitation relationships after introducing the single atom sites was also reviewed.In the future,with the further development of artificial intelligence,the establishment of an energy function with a regression accuracy close to or reaching the level of density functional theory is highly desired to infer the energetic diagram of the photocatalytic systems at the excited states.Furthermore,coordination structures,interaction with inorganic semiconductors,photocatalytic stability and solvent effects should also be carefully considered in the future studies of polymer-based photocatalyst.展开更多
In recent years,single-atom catalysts(SACs)have attracted increasing attention in catalysis.However,their stability is considerably challenging.As a result,fine-tuning the interaction of metal single atoms(SA)with dif...In recent years,single-atom catalysts(SACs)have attracted increasing attention in catalysis.However,their stability is considerably challenging.As a result,fine-tuning the interaction of metal single atoms(SA)with different types of supports has emerged as an effective strategy for improving their thermal and chemical stabilities.Owing to its non-toxicity,cost-effectiveness,high abundance,and excellent stability,as well as presence of rich,tunable,and reliable anchor sites for metal SA,TiO_(2)has been extensively explored as a superior support for SACs.In this review,recent advances of TiO_(2)-supported SACs(M1/TiO_(2))are discussed,and synthetic strategies,structure elucidation,and catalytic applications are summarized.First,the recently developed synthetic strategies for M1/TiO_(2)arehighlighted and summarized,identifying the major challenges for the precise fabrication of M1/TiO_(2).Subsequently,key characterization techniques for the structure identification of M1/TiO_(2)are discussed.Next,catalytic applications of M1/TiO_(2)are highlighted,viz.photocatalysis,electrocatalysis,and thermocatalysis.In addition,the mechanism via geometric structures and electronic states of metal centers facilitate catalytic reactions is outlined.Finally,opportunities and challenges of M1/TiO_(2)in catalysis are discussed,which may inspire the future development of M1/TiO_(2)for multifunctional catalytic applications.展开更多
基金Mitsubishi Chemical Corporation,JSPS Grant-in-Aid for Scientific Research(B,No.20H02847)Grant-in-Aid for JSPS Fellows(DC2,No.20J13064)+2 种基金National Natural Science Foundation of China(No.21805191)Guangdong Basic and Applied Basic Research Foundation,China(No.2020A1515010982)Shenzhen Stable Support Project,China(No.20200812122947002).
文摘Carrier dynamics and surface reaction are two critical processes for determining the performance of photocatalytic reaction.Highly designable polymer-based photocatalysts have shown promising protectives in energetic and environmental applications.In this prospective,we first distinguished the differences of physiochemical properties between polymer-based semiconductors and traditional inorganic semiconductors.Then,the effects of single-atom sites on the charge dynamics and reaction kinetics of polymer-based photocatalysts are further elaborated.Time(excitation)-space(wavefunction)population analysis,which can provide relevant information to clarify the structure-excitation relationships after introducing the single atom sites was also reviewed.In the future,with the further development of artificial intelligence,the establishment of an energy function with a regression accuracy close to or reaching the level of density functional theory is highly desired to infer the energetic diagram of the photocatalytic systems at the excited states.Furthermore,coordination structures,interaction with inorganic semiconductors,photocatalytic stability and solvent effects should also be carefully considered in the future studies of polymer-based photocatalyst.
基金National Natural Science Foundation of China(Nos.21805191,21972094,22102102)China Postdoctoral Science Foundation(No.2021T140472)+1 种基金Guangdong Basic and Applied Basic Research Foundation,China(No.2020A1515010982)Shenzhen Science and Technology Program,China(Nos.20200812122947002,20200812160737002,RCJC20200714114434086,827-000421).
文摘In recent years,single-atom catalysts(SACs)have attracted increasing attention in catalysis.However,their stability is considerably challenging.As a result,fine-tuning the interaction of metal single atoms(SA)with different types of supports has emerged as an effective strategy for improving their thermal and chemical stabilities.Owing to its non-toxicity,cost-effectiveness,high abundance,and excellent stability,as well as presence of rich,tunable,and reliable anchor sites for metal SA,TiO_(2)has been extensively explored as a superior support for SACs.In this review,recent advances of TiO_(2)-supported SACs(M1/TiO_(2))are discussed,and synthetic strategies,structure elucidation,and catalytic applications are summarized.First,the recently developed synthetic strategies for M1/TiO_(2)arehighlighted and summarized,identifying the major challenges for the precise fabrication of M1/TiO_(2).Subsequently,key characterization techniques for the structure identification of M1/TiO_(2)are discussed.Next,catalytic applications of M1/TiO_(2)are highlighted,viz.photocatalysis,electrocatalysis,and thermocatalysis.In addition,the mechanism via geometric structures and electronic states of metal centers facilitate catalytic reactions is outlined.Finally,opportunities and challenges of M1/TiO_(2)in catalysis are discussed,which may inspire the future development of M1/TiO_(2)for multifunctional catalytic applications.
