Rational electrode structure design is of great significance for realizing superior Na^(+)storage performance.Herein,a metal salt-induced polymer blowing-bubble approach followed by selenization procedure is developed...Rational electrode structure design is of great significance for realizing superior Na^(+)storage performance.Herein,a metal salt-induced polymer blowing-bubble approach followed by selenization procedure is developed to in-situ generate abundant sub-10 nm CoSe_(2) nanocrystals on 3D Se/N co-doped carbon networks(CoSe_(2)@3DSNC).The phase transition from Co to CoSe_(2) and the incorporation of Se into the carbon layer are realized simultaneously to establish above configuration,in which the CoSe_(2) nanocrystals are anchored on interlayer expanded carbon networks.Such unique configuration endows electrode with lower Na+diffusion energy barrier,higher Na+storage capability and better structural durability.Reflected in SIBs,the optimized CoSe_(2)@3 DSNC delivers superior rate capability(310 m Ah g^(-1) at 10 A g^(-1))and excellent longterm cycling stability(409 m Ah g^(-1) after 1200 cycles at 5 A g^(-1)).Moreover,this configuration can also be obtained in other metal selenides-carbon composite through a similar approach.展开更多
Over the past few decades,photocatalysis technology has received extensive attention because of its potential to mitigate or solve energy and environmental pollution problems.Designing novel materials with outstanding...Over the past few decades,photocatalysis technology has received extensive attention because of its potential to mitigate or solve energy and environmental pollution problems.Designing novel materials with outstanding photocatalytic activities has become a research hotspot in this field.In this study,we prepared a series of photocatalysts in which BiOCl nanosheets were modified with carbon quantum dots(CQDs)to form CQDs/BiOCl composites by using a simple solvothermal method.The photocatalytic performance of the resulting CQDs/BiOCl composite photocatalysts was assessed by rhodamine B and tetracycline degradation under visible-light irradiation.Compared with bare BiOCl,the photocatalytic activity of the CQDs/BiOCl composites was significantly enhanced,and the 5 wt%CQDs/BiOCl composite exhibited the highest photocatalytic activity with a degradation efficiency of 94.5%after 30 min of irradiation.Moreover,photocatalytic N_(2)reduction performance was significantly improved after introducing CQDs.The 5 wt%CQDs/BiOCl composite displayed the highest photocatalytic N_(2)reduction performance to yield NH_3(346.25μmol/(g h)),which is significantly higher than those of 3 wt%CQDs/BiOCl(256.04μmol/(g h)),7 wt%CQDs/BiOCl(254.07μmol/(g h)),and bare BiOCl(240.19μmol/(g h)).Our systematic characterizations revealed that the key role of CQDs in improving photocatalytic performance is due to their increased light harvesting capacity,remarkable electron transfer ability,and higher photocatalytic activity sites.展开更多
Aqueous zinc ion batteries(ZIBs) are attracting considerable attentions for practical energy storage because of their low cost and high safety.Nevertheless,the traditional manganese oxide cathode materials suffer from...Aqueous zinc ion batteries(ZIBs) are attracting considerable attentions for practical energy storage because of their low cost and high safety.Nevertheless,the traditional manganese oxide cathode materials suffer from the low intrinsic electronic conductivity,sluggish ions diffusion kinetics,and structural collapse,hindering their large-scale application.Herein,we successfully developed a latent amorphous Mn_(1.8)Fe_(1.2)O_(4) hollow nanocube(a-H-MnFeO) cathode material derived from Prussian blue analogue precursor.The amorphous nature endows the cathode with lower diffusion barrier and narrower band gap compared with crystalline counterpart,resulting in the superior Zn^(2+) ions and electrons transport kinetics.Hollow structure can furnish abundant surface sites and suppress the structural collapse during the repeated charge/discharge processes.By virtue of the multiple advantageous features,the a-H-MnFeO cathode exhibits exceptional electrochemical performance,in terms of high capacity,excellent rate capability,and prolonged cycle life.This strategy will pave the way for the structural design of emerging cathode materials.展开更多
Surface co-catalyst modification is a feasible strategy to boost photocatalytic activity.However,it usually meets the issue of limited contact area and poor interfacial interaction,which greatly affects the interfacia...Surface co-catalyst modification is a feasible strategy to boost photocatalytic activity.However,it usually meets the issue of limited contact area and poor interfacial interaction,which greatly affects the interfacial charge transfer efficiency.Herein,a self-adaptive partially oxidised W-based quantum dot(WQDs)is designed to boost the photocatalytic performance of Bi_(12)O_(17)Br_(2).Because of the formation of the strong coupled interface,the BiS1O4 site can be created with a local interfacial asymmetric configuration.This BiS_(1)O_(4)site can serve as an axial polarisation centre to drive rapid interfacial charge transport from Bi12O17Br2 to WQDs via the formed Bi-S bond.At the same time,the partially oxidised WQDs supply a higher charge aggregate state,favouring the small molecule coordination and activation.Benefiting from these features,the greatly improved photocatalytic performance can be achieved for WQDs/Bi_(12)O_(17)Br_(2).This work offers a feasible approach for designing a self-adaptive partially oxidised quantum dot cocatalyst to build a strong coupled interfacial asymmetric configuration to optimise photocatalytic activity.展开更多
Solid-state lithium-metal batteries based on poly(vinylidene fluoride-co-hexafluoropropylene)(PVH)are frequently proposed to address the detrimental safety issue of conventional lithium-ion batteries by eliminating th...Solid-state lithium-metal batteries based on poly(vinylidene fluoride-co-hexafluoropropylene)(PVH)are frequently proposed to address the detrimental safety issue of conventional lithium-ion batteries by eliminating the use of flammable solvents,but still face a key challenge:low capacity and sluggish charge/discharge rate due to the intrinsic large-gradient Li^(+)distribution across the ionically-inert PVH matrix.Herein,Te vacancies in form of Bi_(2)Te_(3-x) are proposed to polarize the PVH unit to realize efficient decoupling of lithium salts at the atomic level in PVH-based solid polymeric electrolyte.Te vacancies in the PVH electrolyte doped with Bi_(2)Te_(3-x)(PVBT)induce a high-throughput and homogenous Li^(+)flow within the PVH matrices and near the Li metal.Theoretical calculations show that Te vacancies own high adsorption energy with bis(trifluoromethanesulfonyl)imide anions(TFSI^(-)),repulsive effect on Li^(+),and localized electron distribution,giving rise to a lithium-ion concentration gradient of 30 mol m^(-3),the smallest among the PVH-based inorganic/organic composite electrolytes.Consequently,the polarized electrolyte owns an unprecedented high-rate battery capacity of 114 mAh g^(-1)at~700 mA g^(-1)and also superior capacity performances with a cathode loading of 12 mg cm^(-2),outperforming the state-of-art PVH-based inorganic/organic composite electrolytes in Li||LiFePO_(4)battery.The work demonstrates an efficient strategy for achieving fast Liþdiffusion dynamics across polymeric matrices of classic solid-state electrolytes.展开更多
Urea plays a vital role in human society,which has various applications in organic synthesis,medicine,materials chemistry,and other fields.Conventional industrial urea production process is energy−intensive and enviro...Urea plays a vital role in human society,which has various applications in organic synthesis,medicine,materials chemistry,and other fields.Conventional industrial urea production process is energy−intensive and environmentally damaging.Recently,electrosynthesis offers a greener alternative to efficient urea synthesis involving coupling CO_(2)and nitrogen sources at ambient conditions,which affords an achievable way for diminishing the energy consumption and CO_(2)emissions.Additionally,urea electrolysis,namely the electrocatalytic urea oxidation reaction(UOR),is another emerging approach very recently.When coupling with hydrogen evolution reaction,the UOR route potentially utilizes 93%less energy than water electrolysis.Although there have been many individual reviews discussing urea electrosynthesis and urea electrooxidation,there is a critical need for a comprehensive review on urea electrocatalysis.The review will serve as a valuable reference for the design of advanced electrocatalysts to enhance the electrochemical urea electrocatalysis performance.In the review,we present a thorough review on two aspects:the electrocatalytic urea synthesis and urea oxidation reaction.We summarize in turn the recently reported catalyst materials,multiple catalysis mechanisms and catalyst design principles for electrocatalytic urea synthesis and urea electrolysis.Finally,major challenges and opportunities are also proposed to inspire further development of urea electrocatalysis technology.展开更多
基金financially supported by the National Natural Science Foundation of China(21471040)。
文摘Rational electrode structure design is of great significance for realizing superior Na^(+)storage performance.Herein,a metal salt-induced polymer blowing-bubble approach followed by selenization procedure is developed to in-situ generate abundant sub-10 nm CoSe_(2) nanocrystals on 3D Se/N co-doped carbon networks(CoSe_(2)@3DSNC).The phase transition from Co to CoSe_(2) and the incorporation of Se into the carbon layer are realized simultaneously to establish above configuration,in which the CoSe_(2) nanocrystals are anchored on interlayer expanded carbon networks.Such unique configuration endows electrode with lower Na+diffusion energy barrier,higher Na+storage capability and better structural durability.Reflected in SIBs,the optimized CoSe_(2)@3 DSNC delivers superior rate capability(310 m Ah g^(-1) at 10 A g^(-1))and excellent longterm cycling stability(409 m Ah g^(-1) after 1200 cycles at 5 A g^(-1)).Moreover,this configuration can also be obtained in other metal selenides-carbon composite through a similar approach.
基金financially suppor ted by Key Research and Development Project of Anhui Province(No.2023h11020002)Natural Science Research Project for Universities in Anhui Province(No.KJ2021ZD0006)+3 种基金Natural Science Foundation of Anhui Province(No.2208085MB21)Fundamental Research Funds for the Central Universities of China(No.PA2022GDSK0056)Anhui Laboratory of Molecule-Based Materials(No.fzj22009)National Natural Science Foundation of China(Nos.21725102,22205108)。
文摘Over the past few decades,photocatalysis technology has received extensive attention because of its potential to mitigate or solve energy and environmental pollution problems.Designing novel materials with outstanding photocatalytic activities has become a research hotspot in this field.In this study,we prepared a series of photocatalysts in which BiOCl nanosheets were modified with carbon quantum dots(CQDs)to form CQDs/BiOCl composites by using a simple solvothermal method.The photocatalytic performance of the resulting CQDs/BiOCl composite photocatalysts was assessed by rhodamine B and tetracycline degradation under visible-light irradiation.Compared with bare BiOCl,the photocatalytic activity of the CQDs/BiOCl composites was significantly enhanced,and the 5 wt%CQDs/BiOCl composite exhibited the highest photocatalytic activity with a degradation efficiency of 94.5%after 30 min of irradiation.Moreover,photocatalytic N_(2)reduction performance was significantly improved after introducing CQDs.The 5 wt%CQDs/BiOCl composite displayed the highest photocatalytic N_(2)reduction performance to yield NH_3(346.25μmol/(g h)),which is significantly higher than those of 3 wt%CQDs/BiOCl(256.04μmol/(g h)),7 wt%CQDs/BiOCl(254.07μmol/(g h)),and bare BiOCl(240.19μmol/(g h)).Our systematic characterizations revealed that the key role of CQDs in improving photocatalytic performance is due to their increased light harvesting capacity,remarkable electron transfer ability,and higher photocatalytic activity sites.
基金funding supported by the National Natural Science Foundation of China (52101246)the Fundamental Research Funds for the Central Universities+1 种基金the Natural Science Foundation of Heilongjiang Province, China (YQ2022B006)the funding supported by the Natural Science Foundation of Anhui Province (2208085MB21)。
文摘Aqueous zinc ion batteries(ZIBs) are attracting considerable attentions for practical energy storage because of their low cost and high safety.Nevertheless,the traditional manganese oxide cathode materials suffer from the low intrinsic electronic conductivity,sluggish ions diffusion kinetics,and structural collapse,hindering their large-scale application.Herein,we successfully developed a latent amorphous Mn_(1.8)Fe_(1.2)O_(4) hollow nanocube(a-H-MnFeO) cathode material derived from Prussian blue analogue precursor.The amorphous nature endows the cathode with lower diffusion barrier and narrower band gap compared with crystalline counterpart,resulting in the superior Zn^(2+) ions and electrons transport kinetics.Hollow structure can furnish abundant surface sites and suppress the structural collapse during the repeated charge/discharge processes.By virtue of the multiple advantageous features,the a-H-MnFeO cathode exhibits exceptional electrochemical performance,in terms of high capacity,excellent rate capability,and prolonged cycle life.This strategy will pave the way for the structural design of emerging cathode materials.
基金supported by the National Natural Science Foundation of China(Nos.U23A20121,22475004,22205108,22473002,and 22073001)Key Research and Development Project of Anhui Province(No.2023h11020002)+2 种基金the Natural Science Research Project for Universities in Anhui Province(No.KJ2021ZD0006)the Natural Science Foundation of Anhui Province(No.2208085MB21)Anhui Laboratory of Molecule-Based Materials(No.fzj22009).
文摘Surface co-catalyst modification is a feasible strategy to boost photocatalytic activity.However,it usually meets the issue of limited contact area and poor interfacial interaction,which greatly affects the interfacial charge transfer efficiency.Herein,a self-adaptive partially oxidised W-based quantum dot(WQDs)is designed to boost the photocatalytic performance of Bi_(12)O_(17)Br_(2).Because of the formation of the strong coupled interface,the BiS1O4 site can be created with a local interfacial asymmetric configuration.This BiS_(1)O_(4)site can serve as an axial polarisation centre to drive rapid interfacial charge transport from Bi12O17Br2 to WQDs via the formed Bi-S bond.At the same time,the partially oxidised WQDs supply a higher charge aggregate state,favouring the small molecule coordination and activation.Benefiting from these features,the greatly improved photocatalytic performance can be achieved for WQDs/Bi_(12)O_(17)Br_(2).This work offers a feasible approach for designing a self-adaptive partially oxidised quantum dot cocatalyst to build a strong coupled interfacial asymmetric configuration to optimise photocatalytic activity.
基金supported by Chongqing Technology Innovation and Application Development Special Key Project,CSTB2023TIAD-KPX0010Chongqing Technology Innovation and Application Development Special Major Project,CSTB2023TIAD-STX0033+1 种基金Natural Science Foundation of Chongqing,China(CSTB2022NSCQ-MSX0246,CSTB2022NSCQ-MSX1572,CSTB2022NSCQ-MSX0310)the Science Foundation of National Key Laboratory of Science and Technology on Advanced Composites in Special Environments.
文摘Solid-state lithium-metal batteries based on poly(vinylidene fluoride-co-hexafluoropropylene)(PVH)are frequently proposed to address the detrimental safety issue of conventional lithium-ion batteries by eliminating the use of flammable solvents,but still face a key challenge:low capacity and sluggish charge/discharge rate due to the intrinsic large-gradient Li^(+)distribution across the ionically-inert PVH matrix.Herein,Te vacancies in form of Bi_(2)Te_(3-x) are proposed to polarize the PVH unit to realize efficient decoupling of lithium salts at the atomic level in PVH-based solid polymeric electrolyte.Te vacancies in the PVH electrolyte doped with Bi_(2)Te_(3-x)(PVBT)induce a high-throughput and homogenous Li^(+)flow within the PVH matrices and near the Li metal.Theoretical calculations show that Te vacancies own high adsorption energy with bis(trifluoromethanesulfonyl)imide anions(TFSI^(-)),repulsive effect on Li^(+),and localized electron distribution,giving rise to a lithium-ion concentration gradient of 30 mol m^(-3),the smallest among the PVH-based inorganic/organic composite electrolytes.Consequently,the polarized electrolyte owns an unprecedented high-rate battery capacity of 114 mAh g^(-1)at~700 mA g^(-1)and also superior capacity performances with a cathode loading of 12 mg cm^(-2),outperforming the state-of-art PVH-based inorganic/organic composite electrolytes in Li||LiFePO_(4)battery.The work demonstrates an efficient strategy for achieving fast Liþdiffusion dynamics across polymeric matrices of classic solid-state electrolytes.
基金C.L.acknowledges the Fundamental Research Funds for the Central Universities and the National Natural Science Foundation of China(52302231 and 22479034).
文摘Urea plays a vital role in human society,which has various applications in organic synthesis,medicine,materials chemistry,and other fields.Conventional industrial urea production process is energy−intensive and environmentally damaging.Recently,electrosynthesis offers a greener alternative to efficient urea synthesis involving coupling CO_(2)and nitrogen sources at ambient conditions,which affords an achievable way for diminishing the energy consumption and CO_(2)emissions.Additionally,urea electrolysis,namely the electrocatalytic urea oxidation reaction(UOR),is another emerging approach very recently.When coupling with hydrogen evolution reaction,the UOR route potentially utilizes 93%less energy than water electrolysis.Although there have been many individual reviews discussing urea electrosynthesis and urea electrooxidation,there is a critical need for a comprehensive review on urea electrocatalysis.The review will serve as a valuable reference for the design of advanced electrocatalysts to enhance the electrochemical urea electrocatalysis performance.In the review,we present a thorough review on two aspects:the electrocatalytic urea synthesis and urea oxidation reaction.We summarize in turn the recently reported catalyst materials,multiple catalysis mechanisms and catalyst design principles for electrocatalytic urea synthesis and urea electrolysis.Finally,major challenges and opportunities are also proposed to inspire further development of urea electrocatalysis technology.
