This comprehensive review provides a deep exploration of the unique roles of single atom catalysts(SACs)in photocatalytic hydrogen peroxide(H_(2)O_(2))production.SACs offer multiple benefits over traditional catalysts...This comprehensive review provides a deep exploration of the unique roles of single atom catalysts(SACs)in photocatalytic hydrogen peroxide(H_(2)O_(2))production.SACs offer multiple benefits over traditional catalysts such as improved efficiency,selectivity,and flexibility due to their distinct electronic structure and unique properties.The review discusses the critical elements in the design of SACs,including the choice of metal atom,host material,and coordination environment,and how these elements impact the catalytic activity.The role of single atoms in photocatalytic H_(2)O_(2)production is also analysed,focusing on enhancing light absorption and charge generation,improving the migration and separation of charge carriers,and lowering the energy barrier of adsorption and activation of reactants.Despite these advantages,several challenges,including H_(2)O_(2)decomposition,stability of SACs,unclear mechanism,and low selectivity,need to be overcome.Looking towards the future,the review suggests promising research directions such as direct utilization of H_(2)O_(2),high-throughput synthesis and screening,the creation of dual active sites,and employing density functional theory for investigating the mechanisms of SACs in H_(2)O_(2)photosynthesis.This review provides valuable insights into the potential of single atom catalysts for advancing the field of photocatalytic H_(2)O_(2)production.展开更多
Hydrogenation/deuteration of carbon chloride(C–Cl)bonds is of high significance but remains a remarkable challenge in synthetic chemistry,especially using safe and inexpensive hydrogen donors.In this article,a visibl...Hydrogenation/deuteration of carbon chloride(C–Cl)bonds is of high significance but remains a remarkable challenge in synthetic chemistry,especially using safe and inexpensive hydrogen donors.In this article,a visible-light-photocatalytic watersplitting hydrogenation technology(WSHT)is proposed to in-situ generate active H-species(i.e.,Had)for controllable hydrogenation of aryl chlorides instead of using flammable H2.When applying heavy water-splitting systems,we could selectively install deuterium at the C–Cl position of aryl chlorides under mild conditions for the sustainable synthesis of high-valued added deuterated chemicals.Sub-micrometer Pd nanosheets(Pd NSs)decorated crystallined polymeric carbon nitrides(CPCN)is developed as the bifunctional photocatalyst,whereas Pd NSs not only serve as a cocatalyst of CPCN to generate and stabilize H(D)-species but also play a significant role in the sequential activation and hydrogenation/deuteration of C–Cl bonds.This article highlights a photocatalytic-WSHT for controllable hydrogenation/deuteration of low-cost aryl chlorides,providing a promising way for the photosynthesis of high-valued added chemicals instead of the hydrogen evolution.展开更多
Ultrabroad spectral absorption is required for semiconductor photocatalysts utilized for solar-to-chemical energy conversion.The light response range can be extended by element doping,but the photocatalytic performanc...Ultrabroad spectral absorption is required for semiconductor photocatalysts utilized for solar-to-chemical energy conversion.The light response range can be extended by element doping,but the photocatalytic performance is generally not enhanced correspondingly.Here we present a solid alkali activation strategy to synthesize near-infrared(NIR)light-activated carbon-doped polymeric carbon nitride(A-cPCN)by combining the copolymerization of melamine and 1,3,5-trimesic acid.The prepared A-cPCN is highly crystalline with a narrowed bandgap and enhanced efficiency in the separation of photogenerated electrons and holes.Under irradiation with NIR light(780 nm≥λ≥700 nm),A-cPCN shows an excellent photocatalytic activity for H_(2)generation from water with rate of 165µmol g^(−1)h^(−1),and the photo-redox activity for H_(2)O_(2)production(109µmol g^(−1)h^(−1))from H_(2)O and O_(2),whereas no observed photocatalytic activity over pure PCN.The NIR photocatalytic activity is due to carbon doping,which leads to the formation of an interband level,and the alkali activation that achieved shrinking the transfer distance of photocarriers.The current synergistic strategy may open insights to fabricate other carbon-nitrogen-based photocatalysts for enhanced solar energy capture and conversion.展开更多
随着大规模储能需求的不断增加,水性锌离子电池在世界范围内引起了越来越多的关注.然而,基于锌离子存储的宿主材料有限,严重地阻碍了锌离子电池的商业化应用.基于此,本论文精确地构建了一系列相结构(正交、三方和四方晶系)的钼钒氧化物...随着大规模储能需求的不断增加,水性锌离子电池在世界范围内引起了越来越多的关注.然而,基于锌离子存储的宿主材料有限,严重地阻碍了锌离子电池的商业化应用.基于此,本论文精确地构建了一系列相结构(正交、三方和四方晶系)的钼钒氧化物,研究了该钼钒氧化物电极材料在锌离子电池中的储锌性能.一系列开放的框架和隧道结构有利于锌离子的扩散动力学.通过相工程优化,正交晶系的钼钒氧化物电极材料的比容量能够达到约400 m A h g^(−1),循环稳定性达到了1000次.正交晶系的钼钒氧化物相中具有大量的六元和七元环结构,在锌离子的可逆嵌入/脱出反应方面发挥了至关重要的作用.本文提出的相工程策略为锌离子电池中正极材料的设计提供了一种新方法.展开更多
基金This work was financially supported by the Guangdong Basic and Applied Basic Research Foundation(2020A1515010982)the National Natural Science Foundation of China(21805191)+2 种基金Shenzhen Science and Technology Program(JCYJ20210324094000001,20190808142001745,20200812122947002)Shenzhen Peacock Plan(20210802524B and 20180921273B)the Australian Research Council(FT200100015)。
文摘This comprehensive review provides a deep exploration of the unique roles of single atom catalysts(SACs)in photocatalytic hydrogen peroxide(H_(2)O_(2))production.SACs offer multiple benefits over traditional catalysts such as improved efficiency,selectivity,and flexibility due to their distinct electronic structure and unique properties.The review discusses the critical elements in the design of SACs,including the choice of metal atom,host material,and coordination environment,and how these elements impact the catalytic activity.The role of single atoms in photocatalytic H_(2)O_(2)production is also analysed,focusing on enhancing light absorption and charge generation,improving the migration and separation of charge carriers,and lowering the energy barrier of adsorption and activation of reactants.Despite these advantages,several challenges,including H_(2)O_(2)decomposition,stability of SACs,unclear mechanism,and low selectivity,need to be overcome.Looking towards the future,the review suggests promising research directions such as direct utilization of H_(2)O_(2),high-throughput synthesis and screening,the creation of dual active sites,and employing density functional theory for investigating the mechanisms of SACs in H_(2)O_(2)photosynthesis.This review provides valuable insights into the potential of single atom catalysts for advancing the field of photocatalytic H_(2)O_(2)production.
基金supported by the National Natural Science Foundation of China(21972094,51701127,21401190)China Postdoctoral Science Foundation(2017M612709)+5 种基金Guangdong Special Support ProgramPengcheng Scholar ProgramShenzhen Peacock Plan(KQJSCX20170727100802505,KQTD2016053112042971)Educational Commission of Guangdong Province(2016KTSCX126)Foundation for Distinguished Young Talents in Higher Education of Guangdong(2018KQNCX221)Shenzhen Innovation Program(JCYJ20170818142642395).
文摘Hydrogenation/deuteration of carbon chloride(C–Cl)bonds is of high significance but remains a remarkable challenge in synthetic chemistry,especially using safe and inexpensive hydrogen donors.In this article,a visible-light-photocatalytic watersplitting hydrogenation technology(WSHT)is proposed to in-situ generate active H-species(i.e.,Had)for controllable hydrogenation of aryl chlorides instead of using flammable H2.When applying heavy water-splitting systems,we could selectively install deuterium at the C–Cl position of aryl chlorides under mild conditions for the sustainable synthesis of high-valued added deuterated chemicals.Sub-micrometer Pd nanosheets(Pd NSs)decorated crystallined polymeric carbon nitrides(CPCN)is developed as the bifunctional photocatalyst,whereas Pd NSs not only serve as a cocatalyst of CPCN to generate and stabilize H(D)-species but also play a significant role in the sequential activation and hydrogenation/deuteration of C–Cl bonds.This article highlights a photocatalytic-WSHT for controllable hydrogenation/deuteration of low-cost aryl chlorides,providing a promising way for the photosynthesis of high-valued added chemicals instead of the hydrogen evolution.
基金supported by the National Natural Science Foundation of China(21972094,21902105)the National Postdoctoral Program for Innovative Talents(BX20180203)+4 种基金China Postdoctoral Science Foundation(2018M643176)Guangdong Special Support ProgramPengcheng Scholar programShenzhen Peacock Plan(KQJSCX20170727100802505 and KQTD2016053112042971)Foundation for Distinguished Young Talents in Higher Education of Guangdong(2018KQNCX221)。
基金supported by the National Natural Science Foundation of China(Nos.21972094,21902105,21805191,51701127,21401190)Guangdong Special Support Program,Pengcheng Scholar Program,Shenzhen Innovation Program(Nos.JCYJ20170818142642395,JCYJ20190808142001745)the Natural Science Foundation of Guangdong Province(No.2020A1515010982).
文摘Ultrabroad spectral absorption is required for semiconductor photocatalysts utilized for solar-to-chemical energy conversion.The light response range can be extended by element doping,but the photocatalytic performance is generally not enhanced correspondingly.Here we present a solid alkali activation strategy to synthesize near-infrared(NIR)light-activated carbon-doped polymeric carbon nitride(A-cPCN)by combining the copolymerization of melamine and 1,3,5-trimesic acid.The prepared A-cPCN is highly crystalline with a narrowed bandgap and enhanced efficiency in the separation of photogenerated electrons and holes.Under irradiation with NIR light(780 nm≥λ≥700 nm),A-cPCN shows an excellent photocatalytic activity for H_(2)generation from water with rate of 165µmol g^(−1)h^(−1),and the photo-redox activity for H_(2)O_(2)production(109µmol g^(−1)h^(−1))from H_(2)O and O_(2),whereas no observed photocatalytic activity over pure PCN.The NIR photocatalytic activity is due to carbon doping,which leads to the formation of an interband level,and the alkali activation that achieved shrinking the transfer distance of photocarriers.The current synergistic strategy may open insights to fabricate other carbon-nitrogen-based photocatalysts for enhanced solar energy capture and conversion.
基金supported by Guangdong Natural Science Foundation(2019A1515010675)the Science and Technology Project of Shenzhen(JCYJ20180305125106329,KQJSCX20180328094001794)。
文摘随着大规模储能需求的不断增加,水性锌离子电池在世界范围内引起了越来越多的关注.然而,基于锌离子存储的宿主材料有限,严重地阻碍了锌离子电池的商业化应用.基于此,本论文精确地构建了一系列相结构(正交、三方和四方晶系)的钼钒氧化物,研究了该钼钒氧化物电极材料在锌离子电池中的储锌性能.一系列开放的框架和隧道结构有利于锌离子的扩散动力学.通过相工程优化,正交晶系的钼钒氧化物电极材料的比容量能够达到约400 m A h g^(−1),循环稳定性达到了1000次.正交晶系的钼钒氧化物相中具有大量的六元和七元环结构,在锌离子的可逆嵌入/脱出反应方面发挥了至关重要的作用.本文提出的相工程策略为锌离子电池中正极材料的设计提供了一种新方法.
