The rapid accumulation of spent LiFePO_(4)(LFP)cathodes from retired lithium-ion batteries necessitates the development of effective and environmental-friendly recycling strategies.In this context,direct regeneration ...The rapid accumulation of spent LiFePO_(4)(LFP)cathodes from retired lithium-ion batteries necessitates the development of effective and environmental-friendly recycling strategies.In this context,direct regeneration has emerged as a promising approach for reclaiming LFP cathode materials,offering a streamlined pathway to restore their electrochemical functionality.We report an integrated regeneration protocol that simultaneously repairs the degraded crystal structure and reconstructs the damaged carbon coating in spent LFP.The regenerated cathode material had superfast lithium-ion diffusion kinetics and a stable cathode-electrolyte interface,giving a remarkable rate capability with specific capacities of 122 m Ah g^(-1)at 5C and 106 m Ah g^(-1)at 10C(1C=170 m A g^(-1)).It also maintained capacities of 110.7 m Ah g^(-1)(5C)and 84.1 m Ah g^(-1)(10C)after 400 cycles.It could be used in harsh environments and could be stably cycled at subzero temperatures(-10 and-20°C)and in solid-state electrolyte batteries.Life cycle assessment combined with economic evaluation using the Ever Batt model reveals that this direct regeneration approach has high economic and environmental benefits.展开更多
Electrocatalytic CO_(2)reduction(ECR)to produce value-added fuels and chemicals using renewable electricity is an emerging strategy to mitigate global warming and decrease reliance on fossil fuels.Among various ECR pr...Electrocatalytic CO_(2)reduction(ECR)to produce value-added fuels and chemicals using renewable electricity is an emerging strategy to mitigate global warming and decrease reliance on fossil fuels.Among various ECR products,liquid oxygenates(Oxys)are especially attractive due to their high energy density,high safety and transportability that could be adapted to the existing infrastructure and transportation system.However,efficiently generating these highly reduced oxygen-containing products by ECR remains challenging due to the complexity of coupled proton and electron transfer processes.In recent years,in-depth studies of reaction mechanisms have advanced the design of catalysts and the regulation of reaction systems for ECR to produce Oxys,Here,by focusing on the production of typical Oxys,such as methanol,acetic acid,ethanol,acetone,n-propanol,and isopropanol,we outline various reaction paths and key intermediates for the electrochemical conversion of CO_(2)into these target products.We also summarize the current research status and recent advances in catalysts based on their elemental composition,and consider recent studies on the change of catalyst geometry and electronic structure,as well as the optimization of reaction systems to increase ECR performance.Finally,we analyze the challenges in the field of ECR to Oxys and provide an outlook on future directions for high-efficiency catalyst prediction and design,as well as the development of advanced reaction systems.展开更多
Nickel-rich LiNi_(1-x-y)Co_(x)Mn_(y)O_(2)(NCM,1-x-y≥0.6)is known as a promising cathode material for lithium-ion batteries since its superiority of high voltage and large capacity.However,polycrystalline Ni-rich NCMs...Nickel-rich LiNi_(1-x-y)Co_(x)Mn_(y)O_(2)(NCM,1-x-y≥0.6)is known as a promising cathode material for lithium-ion batteries since its superiority of high voltage and large capacity.However,polycrystalline Ni-rich NCMs suffer from poor cycle stability,limiting its further application.Herein,single crystal and polycrystalline LiNi_(0.84)Co_(0.07)Mn_(0.09)O_(2)cathode materials are compared to figure out the relation of the morphology and the electrochemical storage performance.According to the Li^(+)diffusion coefficient,the lower capacity of single crystal samples is mainly ascribed to the limited Li+diffusion in the large bulk.In situ XRD illustrates that the polycrystalline and single crystal NCMs show a virtually identical manner and magnitude in lattice contraction and expansion during cycling.Also,the electrochemically active surface area(ECSA)measurement is employed in lithium-ion battery study for the first time,and these two cathodes show huge discrepancy in the ECSA after the initial cycle.These results suggest that the single crystal sample exhibits reduced cracking,surface side reaction,and Ni/Li mixing but suffers the lower Li^(+)diffusion kinetics.This work offers a view of how the morphology of Ni-rich NCM effects the electrochemical performance,which is instructive for developing a promising strategy to achieve good rate performance and excellent cycling stability.展开更多
The continuous and excessive emission of CO_(2)into the atmosphere presents a pressing challenge for global sustainable development.In response,researchers have been devoting significant efforts to develop methods for...The continuous and excessive emission of CO_(2)into the atmosphere presents a pressing challenge for global sustainable development.In response,researchers have been devoting significant efforts to develop methods for converting CO_(2)into valuable chemicals and fuels.These conversions have the potential to establish a closed artificial carbon cycle and provide an alternative resource to depleting fossil fuels.Among the various conversion routes,thermochemical CO_(2)reduction stands out as a promising candidate for industrialization.Within the realm of heterogeneous catalysis,single atom catalysts(SACs)have garnered significant attention.The utilization of SACs offers tremendous potential for enhancing catalytic performance.To achieve optimal activity and selectivity of SACs in CO_(2)thermochemical reduction reactions,a comprehensive understanding of key factors such as single atom metal-support interactions,chemical coordination,and accessibility of active sites is crucial.Despite extensive research in this field,the atomic-scale reaction mechanisms in different chemical environments remain largely unexplored.While SACs have been found successful applications in electrochemical and photochemical CO_(2)reduction reactions,their implementation in thermochemical CO_(2)reduction encounters challenges due to the sintering and/or agglomeration effects that occur at elevated temperatures.In this review,we present a unique approach that combines theoretical understanding with experimental strategies to guide researchers in the design of controlled and thermally stable SACs.By elucidating the underlying principles,we aim to enable the creation of SACs that exhibit stable and efficient catalytic activity for thermochemical CO_(2)reduction reactions.Subsequently,we provide a comprehensive overview of recent literature on noble metal-and transition metal-based SACs for thermochemical CO_(2)reduction.The current review is focused on certain CO_(2)-derived products involving one step reduction only for simplicity and for better understanding the SACs enhancement mechanism.We emphasize various synthesis methods employed and highlight the catalytic activity of these SACs.Finally,we delve into the perspectives and challenges associated with SACs in the context of thermochemical CO_(2)reduction reactions,providing valuable insights for future research endeavor.Through this review,we aim to contribute to the advancement of SACs in the field of thermochemical CO_(2)reduction,shedding light on their potential as effective catalysts and addressing the challenges that need to be overcome for their successful implementation as paradigm shift in catalysis.展开更多
Mixed polyanionic compounds are potential cathode materials for sodium-ion batteries(SIBs).Herein,considering the advantages of the strong inductive effect of sulfate and the diverse,flexible coordination modes of oxa...Mixed polyanionic compounds are potential cathode materials for sodium-ion batteries(SIBs).Herein,considering the advantages of the strong inductive effect of sulfate and the diverse,flexible coordination modes of oxalate,we systematically explored mixed sulfate-oxalate systems and obtained three sodium-contained polyanionic compounds.Interestingly,the novel three-dimensional Na_(2)Co(C(2)O_(4))(SO_(4))·xH_(2)O(x=1-1.5)was found to be a promising cathode material for SIBs with good electrochemical activity at high voltage.The present study sets an example of exploring sodium-storage materials in the mixed polyanionic family and provides new insights into designing novel high-voltage cathodes for sodium-based energy storage devices.展开更多
Hexagonal boron nitride nanosheets(BNNSs)exhibit remarkable thermal and dielectric properties.However,their self-assembly and alignment in macroscopic forms remain challenging due to the chemical inertness of boron ni...Hexagonal boron nitride nanosheets(BNNSs)exhibit remarkable thermal and dielectric properties.However,their self-assembly and alignment in macroscopic forms remain challenging due to the chemical inertness of boron nitride,thereby limiting their performance in applications such as thermal management.In this study,we present a coaxial wet spinning approach for the fabrication of BNNSs/polymer composite fibers with high nanosheet orientation.The composite fibers were prepared using a superacid-based solvent system and showed a layered structure comprising an aramid core and an aramid/BNNSs sheath.Notably,the coaxial fibers exhibited significantly higher BNNSs alignment compared to uniaxial aramid/BNNSs fibers,primarily due to the additional compressive forces exerted at the core-sheath interface during the hot drawing process.With a BNNSs loading of 60 wt%,the resulting coaxial fibers showed exceptional properties,including an ultrahigh Herman orientation parameter of 0.81,thermal conductivity of 17.2 W m^(-1)K^(-1),and tensile strength of 192.5 MPa.These results surpassed those of uniaxial fibers and previously reported BNNSs composite fibers,making them highly suitable for applications such as wearable thermal management textiles.Our findings present a promising strategy for fabricating high-performance composite fibers based on BNNSs.展开更多
Aqueous zinc ion batteries(AZIBs)are a promising energy storage technology due to their cost-effectiveness and safety.Organic materials with sustainable and designable structures are of great interest as AZIBs cath-od...Aqueous zinc ion batteries(AZIBs)are a promising energy storage technology due to their cost-effectiveness and safety.Organic materials with sustainable and designable structures are of great interest as AZIBs cath-odes.However,small molecules in organic cathode materials face dissolution problems and suboptimal cycle life,whereas large molecules suffer from a low theoretical capacity due to their inert carbon skeletons.Here,we designed two covalent organic framework(COF)materials(benzoquinoxaline benzoquinone-based COF(BB-COF)and triquinoxalinylene benzoquinone-based COF(TB-COF))with the same structure and number of energy storage groups to investigate the correlation between the densities of active sites and electrochemi-cal performance.We conclude that the electrochemical behavior of organic conjugate-based energy storage materials lacks a linear correlation with active site quantity.Adjusting active site densities is crucial for mate-rial advancement.BB-COF and TB-COF with dual active sites(C=O and C=N)exhibit distinct characteristics.TB-COF,which has dense active groups,shows a high initial capacity(222 mAh g^(-1)).Conversely,BB-COF,which features a large conjugated ring diameter,presents superior rate performance and enduring cycle stability.It even maintains stable cycling for 2000 cycles at-40℃.In-situ electrochemical quartz crystal mic-robalance tests reveal the energy storage mechanism of BB-COF,in which H+storage is followed by Zn2+storage.展开更多
Layered materials with unique structures and symmetries have attracted tremendous interest for constructing 2-dimensional(2D)structures.The weak interlayer interaction renders them to be readily isolated into various ...Layered materials with unique structures and symmetries have attracted tremendous interest for constructing 2-dimensional(2D)structures.The weak interlayer interaction renders them to be readily isolated into various ultrathin nanosheets with exotic properties and diverse applications.In order to enrich the library of 2D materials,extensive progress has been made in the field of ternary layered materials.Consequently,many brand-new materials are derived,which greatly extend the members of 2D realm.In this review,we emphasize the recent progress made in synthesis and exploration of ternary layered materials.We first classify them in terms of stoichiometric ratio and summarize their difference in interlayer interaction,which is of great importance to produce corresponding 2D materials.The compositional and structural characteristics of resultant 2D ternary materials are then discussed so as to realize desired structures and properties.As a new family of 2D materials,we overview the layer-dependent properties and related applications in the fields of electronics,optoelectronics,and energy storage and conversion.The review finally provides a perspective for this rapidly developing field.展开更多
Converting CO_(2)into fuel or chemicals using renewable energy is a promising strategy for closing the anthropogenic carbon cycle.However,due to the highly stable C紏Obond,CO_(2)activation requires a significant energ...Converting CO_(2)into fuel or chemicals using renewable energy is a promising strategy for closing the anthropogenic carbon cycle.However,due to the highly stable C紏Obond,CO_(2)activation requires a significant energy input to elevate the reactant to a higher energy state,plus an efficient catalyst to surmount the activation energy barrier.Despite significant advancements in catalytic methods using a single energy input for CO_(2)reduction,the catalytic efficiency and economic viability have yet to be improved.However,integrating multiple energy sources in catalysis has shown significant potential for improving catalytic efficiency.These energy-coupled systems demonstrate a synergistic effect,stemming from themultiple excitationmodes of the reactants,the reaction intermediates,or even the catalysts.To our knowledge,there has not been a systematic review addressing synergetic energy-coupled catalysis for CO_(2)reduction.Herein,we aim to offer a comprehensive overview of recent advances in CO_(2)reduction driven by synergetic energycoupled catalysis.Furthermore,we explore the technological challenges and prospects associated with the synergistic effect in energy-coupled catalytic systems,presenting our insights on potential breakthrough directions.展开更多
A solar steam evaporator provides a sustainable and efficient alternative water purification solution to address the global freshwater shortage.Previous efforts have made significant advances in maximizing its water e...A solar steam evaporator provides a sustainable and efficient alternative water purification solution to address the global freshwater shortage.Previous efforts have made significant advances in maximizing its water evaporation rate,but no single evaporator has all the properties necessary for practical point-of-use application,including a high efficiency for generation of drinkable water,an excellent portability critical for on-site water purification,good washability for mitigating evaporator fouling,and good reusability.We report a strategy to produce a high-performance photothermal material for point-of-use water purification.By simultaneously incorporating graphene and gold particles grown from recycled electronic waste in a mechanically strong sponge,we achieved highly efficient water purification under realistic conditions.In addition to a high evaporation rate(3.55 kg/m^(2)/h under one-sun irradiation)attributed to a control of atomic structure of graphene and the size-dependent surface plasmon resonance of gold nanoparticles,it is portable which can be folded,vacuum compacted,dried and rehydrated without compromising performance.It also allows repeated washing to remove contaminant fouling so that it can be reused.The evaporator transforms various types of contaminated water into drinkable clean water,and can be mounted at any angle to optimize the incident solar irradiation.Furthermore,the assembled steam evaporator device could gain purified water meeting the World Health Organization drinking water standards with a high evaporation rate of 9.36 kg/m^(2)/h under outdoor sunlight.展开更多
Even in their bulk forms,complex alloys like high-entropy alloys(HEAs)exhibit favorable activity and stability as electrocatalysts for the oxygen evolution reaction(OER).However,the underlying reasons are not yet full...Even in their bulk forms,complex alloys like high-entropy alloys(HEAs)exhibit favorable activity and stability as electrocatalysts for the oxygen evolution reaction(OER).However,the underlying reasons are not yet fully understood.In a family of Mo-doped CrFeCoNi-based HEAs,we have identified three crucial factors that govern their performance:(i)homogeneous solid solution phase of HEAs helps to maintain high-valence states of metals;(ii)surface reconstruction results in a hybrid material comprising amorphous domains and percolated crystalline structures;(iii)diversity of active intermediate species(M–O,M–OOH,and,notably,the abundance of superoxideμ–OO),which display stronger adsorption capacity on the reconstructed surface.These results are revealing due to their resemblance to findings in other families of electrocatalysts for OER,as well as their unique features specific to HEAs.In line with these factors,a CrFeCoNiMo0.2 bulk integrated electrode displays a low overpotential of 215 mV,rapid kinetics,and long-term stability of over 90 d.Bulk HEAs hold great potential for industrial applications.展开更多
Solid-state lithium-metal batteries(SLMBs)have been regarded as one of the most promising next-generation devices because of their potential high safety,high energy density,and simple packing procedure.However,the pra...Solid-state lithium-metal batteries(SLMBs)have been regarded as one of the most promising next-generation devices because of their potential high safety,high energy density,and simple packing procedure.However,the practical applications of SLMBs are restricted by a series of static and dynamic interfacial issues,including poor interfacial contact,(electro-)chemical incompatibility,dynamic Li dendrite penetration,etc.In recent years,considerable attempts have been made to obtain mechanistic insight into interfacial failures and to develop possible strategies towards excellent interfacial properties for SLMBs.The static and dynamic failure mechanisms at interfaces between solid electrolytes(SEs)and electrodes are comprehensively summarized,and design strategies involving interfacial modification,electrode/SE engineering,and the monolithic construction of SLMBs are discussed in detail.Finally,possible research methodologies such as theoretical calcu-lations,advanced characterization techniques,and versatile design strategies are provided to tackle these interfacial problems.展开更多
The development of durable electrocatalysts overcoming activity-stability compromises remains pivotal for advancing anion-exchange membrane fuel cells(AEMFCs).Herein,we engineer a rare earth-incorporated Pd-based meta...The development of durable electrocatalysts overcoming activity-stability compromises remains pivotal for advancing anion-exchange membrane fuel cells(AEMFCs).Herein,we engineer a rare earth-incorporated Pd-based metallene(PdLaCe)through lanthanide-based bimetallic coordination,resolving critical limitations in oxygen reduction reaction(ORR)catalysis.Combined experimental characterization and theoretical simulations reveal that La/Ce dualdoping induces charge polarization to generate Pd^(δ-)-La/Ce^(δ+)active sites,synergistically optimizing the electronic structure via d-band center downshifting.This configuration weakens oxygen intermediate adsorption while enhancing structural integrity across thermal cycles.The optimized PdLaCe metallene delivers exceptional ORR performance,achieving a record half-wave potential of 0.903 V(vs.RHE)with negligible degradation(<6%)after 20,000 cycles,far surpassing commercial Pt/C benchmarks.Integrated into AEMFCs,it demonstrates a peak power density of 82.8 mW cm^(-2)alongside unprecedented stability(0.8 V for 22 h).Fundamental insights into lanthanide-induced charge redistribution establish a universal paradigm for designing robust multimetallic electrocatalysts via rare earth coordination engineering,bridging critical gaps between functional optimization and industrialscale fuel cell applications.This work provides transformative strategies for next-generation energy conversion systems requiring high efficiency and ultra-stability.展开更多
Benefiting from the advantageous features of structural diversity and resource renewability,organic electroactive compounds are considered as attractive cathode materials for aqueous Zn-ion batteries(ZIBs).In this rev...Benefiting from the advantageous features of structural diversity and resource renewability,organic electroactive compounds are considered as attractive cathode materials for aqueous Zn-ion batteries(ZIBs).In this review,we discuss the recent developments of organic electrode materials for aqueous ZIBs.Although the proton(H^(+))storage chemistry in aqueous Zn-organic batteries has triggered an overwhelming literature surge in recent years,this topic remains controversial.Therefore,our review focuses on this significant issue and summarizes the reported electrochemical mechanisms,including pure Zn^(2+)intercalation,pure H^(+)storage,and H^(+)/Zn^(2+)co-storage.Moreover,the impact of H^(+)storage on the electrochemical performance of aqueous ZIBs is discussed systematically.Given the significance of H^(+)storage,we also highlight the relevant characterization methods employed.Finally,perspectives and directions on further understanding the charge storage mechanisms of organic materials are outlined.We hope that this review will stimulate more attention on the H^(+)storage chemistry of organic electrode materials to advance our understanding and further its application.展开更多
磁场触发的催化剂轨道电子自旋排列已成为促进析氧反应的一种有趣而可行的策略.然而,具有强d-d库仑相互作用的高熵合金(HEAs)催化剂中的磁场增强机制尚未得到充分挖掘.在此,我们设计了具有优异软磁性的高熵合金金属片,在微小磁场下表现...磁场触发的催化剂轨道电子自旋排列已成为促进析氧反应的一种有趣而可行的策略.然而,具有强d-d库仑相互作用的高熵合金(HEAs)催化剂中的磁场增强机制尚未得到充分挖掘.在此,我们设计了具有优异软磁性的高熵合金金属片,在微小磁场下表现出显著的磁场增强催化作用,其磁导率可作为评估磁场增强的描述因子.具体地,仅施加50 mT的磁场,(FeCoNi)_(82.5)Cr_(17.5)HEAs的过电位下降就超过了36mV@10 mA cm^(-2).此外,过电位的降低与HEA的磁导率呈线性关系.原位拉曼光谱与理论计算结果表明,施加磁场可显著提高自旋密度,改善催化剂的3d电子与*O自由基的2p轨道之间的自旋相互作用,从而有效降低速率决定步骤(*O→*OOH)的能量障碍,进而促进O-O的形成.展开更多
基金financial support from the National Key R&D Program of China(2022YFB2402600)the National Natural Science Foundation of China(52372250,52125105,52173242)+1 种基金Shenzhen Science and Technology Planning Project(RCYX20221008092850072,JSGG20220831104004008,KJZD20230923113859006,JCYJ20220531100405012,KJZD20241122161900001)Science and Technology Planning Project of Guangdong Province(2024A1515030076)。
文摘The rapid accumulation of spent LiFePO_(4)(LFP)cathodes from retired lithium-ion batteries necessitates the development of effective and environmental-friendly recycling strategies.In this context,direct regeneration has emerged as a promising approach for reclaiming LFP cathode materials,offering a streamlined pathway to restore their electrochemical functionality.We report an integrated regeneration protocol that simultaneously repairs the degraded crystal structure and reconstructs the damaged carbon coating in spent LFP.The regenerated cathode material had superfast lithium-ion diffusion kinetics and a stable cathode-electrolyte interface,giving a remarkable rate capability with specific capacities of 122 m Ah g^(-1)at 5C and 106 m Ah g^(-1)at 10C(1C=170 m A g^(-1)).It also maintained capacities of 110.7 m Ah g^(-1)(5C)and 84.1 m Ah g^(-1)(10C)after 400 cycles.It could be used in harsh environments and could be stably cycled at subzero temperatures(-10 and-20°C)and in solid-state electrolyte batteries.Life cycle assessment combined with economic evaluation using the Ever Batt model reveals that this direct regeneration approach has high economic and environmental benefits.
基金financial supports from the National Natural Science Foundation of China(52201237)the Talent Introduction Project of Chinese Academy of Sciences(E344011)+4 种基金the Shenzhen High Level Talent Team Project(KQTD2022110109364705)the Joint Research Project of China Merchants Group and SIAT(E2Z1521)the Cross Institute Joint Research Youth Team Project of SIAT(E25427)National Natural Science Foundation of China(52402136)the China Postdoctoral Science Foundation(E325281005)。
文摘Electrocatalytic CO_(2)reduction(ECR)to produce value-added fuels and chemicals using renewable electricity is an emerging strategy to mitigate global warming and decrease reliance on fossil fuels.Among various ECR products,liquid oxygenates(Oxys)are especially attractive due to their high energy density,high safety and transportability that could be adapted to the existing infrastructure and transportation system.However,efficiently generating these highly reduced oxygen-containing products by ECR remains challenging due to the complexity of coupled proton and electron transfer processes.In recent years,in-depth studies of reaction mechanisms have advanced the design of catalysts and the regulation of reaction systems for ECR to produce Oxys,Here,by focusing on the production of typical Oxys,such as methanol,acetic acid,ethanol,acetone,n-propanol,and isopropanol,we outline various reaction paths and key intermediates for the electrochemical conversion of CO_(2)into these target products.We also summarize the current research status and recent advances in catalysts based on their elemental composition,and consider recent studies on the change of catalyst geometry and electronic structure,as well as the optimization of reaction systems to increase ECR performance.Finally,we analyze the challenges in the field of ECR to Oxys and provide an outlook on future directions for high-efficiency catalyst prediction and design,as well as the development of advanced reaction systems.
基金supported by the National Natural Science Foundation of China(Nos.51872157,52072208)Shenzhen Technical Plan Project(JCYJ20170817161753629)+1 种基金Fundamental Research Project of Shenzhen(No.JCYJ20190808153609561)Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(2017BT01N111).
文摘Nickel-rich LiNi_(1-x-y)Co_(x)Mn_(y)O_(2)(NCM,1-x-y≥0.6)is known as a promising cathode material for lithium-ion batteries since its superiority of high voltage and large capacity.However,polycrystalline Ni-rich NCMs suffer from poor cycle stability,limiting its further application.Herein,single crystal and polycrystalline LiNi_(0.84)Co_(0.07)Mn_(0.09)O_(2)cathode materials are compared to figure out the relation of the morphology and the electrochemical storage performance.According to the Li^(+)diffusion coefficient,the lower capacity of single crystal samples is mainly ascribed to the limited Li+diffusion in the large bulk.In situ XRD illustrates that the polycrystalline and single crystal NCMs show a virtually identical manner and magnitude in lattice contraction and expansion during cycling.Also,the electrochemically active surface area(ECSA)measurement is employed in lithium-ion battery study for the first time,and these two cathodes show huge discrepancy in the ECSA after the initial cycle.These results suggest that the single crystal sample exhibits reduced cracking,surface side reaction,and Ni/Li mixing but suffers the lower Li^(+)diffusion kinetics.This work offers a view of how the morphology of Ni-rich NCM effects the electrochemical performance,which is instructive for developing a promising strategy to achieve good rate performance and excellent cycling stability.
基金support by Khalifa University through CIRA-2020-077 and RC2-2018-024 grants。
文摘The continuous and excessive emission of CO_(2)into the atmosphere presents a pressing challenge for global sustainable development.In response,researchers have been devoting significant efforts to develop methods for converting CO_(2)into valuable chemicals and fuels.These conversions have the potential to establish a closed artificial carbon cycle and provide an alternative resource to depleting fossil fuels.Among the various conversion routes,thermochemical CO_(2)reduction stands out as a promising candidate for industrialization.Within the realm of heterogeneous catalysis,single atom catalysts(SACs)have garnered significant attention.The utilization of SACs offers tremendous potential for enhancing catalytic performance.To achieve optimal activity and selectivity of SACs in CO_(2)thermochemical reduction reactions,a comprehensive understanding of key factors such as single atom metal-support interactions,chemical coordination,and accessibility of active sites is crucial.Despite extensive research in this field,the atomic-scale reaction mechanisms in different chemical environments remain largely unexplored.While SACs have been found successful applications in electrochemical and photochemical CO_(2)reduction reactions,their implementation in thermochemical CO_(2)reduction encounters challenges due to the sintering and/or agglomeration effects that occur at elevated temperatures.In this review,we present a unique approach that combines theoretical understanding with experimental strategies to guide researchers in the design of controlled and thermally stable SACs.By elucidating the underlying principles,we aim to enable the creation of SACs that exhibit stable and efficient catalytic activity for thermochemical CO_(2)reduction reactions.Subsequently,we provide a comprehensive overview of recent literature on noble metal-and transition metal-based SACs for thermochemical CO_(2)reduction.The current review is focused on certain CO_(2)-derived products involving one step reduction only for simplicity and for better understanding the SACs enhancement mechanism.We emphasize various synthesis methods employed and highlight the catalytic activity of these SACs.Finally,we delve into the perspectives and challenges associated with SACs in the context of thermochemical CO_(2)reduction reactions,providing valuable insights for future research endeavor.Through this review,we aim to contribute to the advancement of SACs in the field of thermochemical CO_(2)reduction,shedding light on their potential as effective catalysts and addressing the challenges that need to be overcome for their successful implementation as paradigm shift in catalysis.
基金support from the National Key R&D Program of China(grant no.2022YFB2402600)the National Natural Science Foundation of China(grant nos.52125105,52061160484,52372250)+1 种基金the Shenzhen Science and Technology Planning Project(grant nos.RCYX20221008092850072,GJHZ20210705141407023,ZDSYS20210706144000003)the Guangdong Basic and Applied Basic Research Foundation(grant nos.2021A1515010184 and 2022A1515110031).
文摘Mixed polyanionic compounds are potential cathode materials for sodium-ion batteries(SIBs).Herein,considering the advantages of the strong inductive effect of sulfate and the diverse,flexible coordination modes of oxalate,we systematically explored mixed sulfate-oxalate systems and obtained three sodium-contained polyanionic compounds.Interestingly,the novel three-dimensional Na_(2)Co(C(2)O_(4))(SO_(4))·xH_(2)O(x=1-1.5)was found to be a promising cathode material for SIBs with good electrochemical activity at high voltage.The present study sets an example of exploring sodium-storage materials in the mixed polyanionic family and provides new insights into designing novel high-voltage cathodes for sodium-based energy storage devices.
基金This work was supported by the National Key Research and Development Project(Nos.2019YFA0705403,2022YFA1205300)the National Natural Science Foundation of China(No.T2293693)+3 种基金the Guangdong Innovative and Entrepreneurial Research Team Program(No.2017ZT07C341)the Guangdong Basic and Applied Basic Research Foundation(No.2020B0301030002)the Shenzhen Basic Research Project(Nos.WDZC20200824091903001,JSGG20220831105402004)Zhiyuan Xiong thanks the financial support from South China University of Technology.
文摘Hexagonal boron nitride nanosheets(BNNSs)exhibit remarkable thermal and dielectric properties.However,their self-assembly and alignment in macroscopic forms remain challenging due to the chemical inertness of boron nitride,thereby limiting their performance in applications such as thermal management.In this study,we present a coaxial wet spinning approach for the fabrication of BNNSs/polymer composite fibers with high nanosheet orientation.The composite fibers were prepared using a superacid-based solvent system and showed a layered structure comprising an aramid core and an aramid/BNNSs sheath.Notably,the coaxial fibers exhibited significantly higher BNNSs alignment compared to uniaxial aramid/BNNSs fibers,primarily due to the additional compressive forces exerted at the core-sheath interface during the hot drawing process.With a BNNSs loading of 60 wt%,the resulting coaxial fibers showed exceptional properties,including an ultrahigh Herman orientation parameter of 0.81,thermal conductivity of 17.2 W m^(-1)K^(-1),and tensile strength of 192.5 MPa.These results surpassed those of uniaxial fibers and previously reported BNNSs composite fibers,making them highly suitable for applications such as wearable thermal management textiles.Our findings present a promising strategy for fabricating high-performance composite fibers based on BNNSs.
基金supported by the National Natural Science Foundation of China(Nos.22279160 and 22109134)Guangdong Basic and Applied Basic Research Foundation(2022A1515010920)+3 种基金the Outstanding Youth Basic Research Project of Shenzhen(RCYX20221008092934093)the China Postdoctoral Science Foundation(2023M733670)Special Research Assistant Funding Project of the Chinese Academy of Sciencessupported by the public computing service platform provided by SIAT.
文摘Aqueous zinc ion batteries(AZIBs)are a promising energy storage technology due to their cost-effectiveness and safety.Organic materials with sustainable and designable structures are of great interest as AZIBs cath-odes.However,small molecules in organic cathode materials face dissolution problems and suboptimal cycle life,whereas large molecules suffer from a low theoretical capacity due to their inert carbon skeletons.Here,we designed two covalent organic framework(COF)materials(benzoquinoxaline benzoquinone-based COF(BB-COF)and triquinoxalinylene benzoquinone-based COF(TB-COF))with the same structure and number of energy storage groups to investigate the correlation between the densities of active sites and electrochemi-cal performance.We conclude that the electrochemical behavior of organic conjugate-based energy storage materials lacks a linear correlation with active site quantity.Adjusting active site densities is crucial for mate-rial advancement.BB-COF and TB-COF with dual active sites(C=O and C=N)exhibit distinct characteristics.TB-COF,which has dense active groups,shows a high initial capacity(222 mAh g^(-1)).Conversely,BB-COF,which features a large conjugated ring diameter,presents superior rate performance and enduring cycle stability.It even maintains stable cycling for 2000 cycles at-40℃.In-situ electrochemical quartz crystal mic-robalance tests reveal the energy storage mechanism of BB-COF,in which H+storage is followed by Zn2+storage.
基金the National Natural Science Foundation of China(Nos.52188101,22275205,22005284,and 52273311)Shenzhen Basic Research Project(No.JCYJ20200109144616617)+1 种基金the Science and Technology Foundation of Shenzhen(JCYJ20220530154404010)China Postdoctoral Fund(No.2022M713270)。
文摘Layered materials with unique structures and symmetries have attracted tremendous interest for constructing 2-dimensional(2D)structures.The weak interlayer interaction renders them to be readily isolated into various ultrathin nanosheets with exotic properties and diverse applications.In order to enrich the library of 2D materials,extensive progress has been made in the field of ternary layered materials.Consequently,many brand-new materials are derived,which greatly extend the members of 2D realm.In this review,we emphasize the recent progress made in synthesis and exploration of ternary layered materials.We first classify them in terms of stoichiometric ratio and summarize their difference in interlayer interaction,which is of great importance to produce corresponding 2D materials.The compositional and structural characteristics of resultant 2D ternary materials are then discussed so as to realize desired structures and properties.As a new family of 2D materials,we overview the layer-dependent properties and related applications in the fields of electronics,optoelectronics,and energy storage and conversion.The review finally provides a perspective for this rapidly developing field.
基金financial supports from the National Natural Science Foundation of China(52201237)Shenzhen Science and Technology Innovation Bureau(KQTD2022110109364705,ZDSYS20210706144000003)+2 种基金the China Postdoctoral Science Foundation(E325281005 and E325281003)the Joint Research Project of China Merchants Group and SIAT(E2Z1521)the Cross Institute Joint Research Youth Team Project of SIAT(E25427).
文摘Converting CO_(2)into fuel or chemicals using renewable energy is a promising strategy for closing the anthropogenic carbon cycle.However,due to the highly stable C紏Obond,CO_(2)activation requires a significant energy input to elevate the reactant to a higher energy state,plus an efficient catalyst to surmount the activation energy barrier.Despite significant advancements in catalytic methods using a single energy input for CO_(2)reduction,the catalytic efficiency and economic viability have yet to be improved.However,integrating multiple energy sources in catalysis has shown significant potential for improving catalytic efficiency.These energy-coupled systems demonstrate a synergistic effect,stemming from themultiple excitationmodes of the reactants,the reaction intermediates,or even the catalysts.To our knowledge,there has not been a systematic review addressing synergetic energy-coupled catalysis for CO_(2)reduction.Herein,we aim to offer a comprehensive overview of recent advances in CO_(2)reduction driven by synergetic energycoupled catalysis.Furthermore,we explore the technological challenges and prospects associated with the synergistic effect in energy-coupled catalytic systems,presenting our insights on potential breakthrough directions.
基金supported primarily by the Peacock Team Project(KQTD20210811090112002)the National Natural Science Foundation of China(52188101)+2 种基金the Scientific Research Start-up Funds of Tsinghua SIGS(QD2021026C)the Research Fund from Shenzhen International Graduate School,Tsinghua University(JC2021011)Shenzhen Geim Graphene Center。
文摘A solar steam evaporator provides a sustainable and efficient alternative water purification solution to address the global freshwater shortage.Previous efforts have made significant advances in maximizing its water evaporation rate,but no single evaporator has all the properties necessary for practical point-of-use application,including a high efficiency for generation of drinkable water,an excellent portability critical for on-site water purification,good washability for mitigating evaporator fouling,and good reusability.We report a strategy to produce a high-performance photothermal material for point-of-use water purification.By simultaneously incorporating graphene and gold particles grown from recycled electronic waste in a mechanically strong sponge,we achieved highly efficient water purification under realistic conditions.In addition to a high evaporation rate(3.55 kg/m^(2)/h under one-sun irradiation)attributed to a control of atomic structure of graphene and the size-dependent surface plasmon resonance of gold nanoparticles,it is portable which can be folded,vacuum compacted,dried and rehydrated without compromising performance.It also allows repeated washing to remove contaminant fouling so that it can be reused.The evaporator transforms various types of contaminated water into drinkable clean water,and can be mounted at any angle to optimize the incident solar irradiation.Furthermore,the assembled steam evaporator device could gain purified water meeting the World Health Organization drinking water standards with a high evaporation rate of 9.36 kg/m^(2)/h under outdoor sunlight.
基金work was supported by the National Thousand a Young Talents Program of China,the Fundamental Research Funds for the Central Universities(2018KFYXKJC009)the National Natural Science Foundation of China(51871076)the NSFC of Hubei(Grant 2021CFB420).
文摘Even in their bulk forms,complex alloys like high-entropy alloys(HEAs)exhibit favorable activity and stability as electrocatalysts for the oxygen evolution reaction(OER).However,the underlying reasons are not yet fully understood.In a family of Mo-doped CrFeCoNi-based HEAs,we have identified three crucial factors that govern their performance:(i)homogeneous solid solution phase of HEAs helps to maintain high-valence states of metals;(ii)surface reconstruction results in a hybrid material comprising amorphous domains and percolated crystalline structures;(iii)diversity of active intermediate species(M–O,M–OOH,and,notably,the abundance of superoxideμ–OO),which display stronger adsorption capacity on the reconstructed surface.These results are revealing due to their resemblance to findings in other families of electrocatalysts for OER,as well as their unique features specific to HEAs.In line with these factors,a CrFeCoNiMo0.2 bulk integrated electrode displays a low overpotential of 215 mV,rapid kinetics,and long-term stability of over 90 d.Bulk HEAs hold great potential for industrial applications.
基金supported by the National Key R&D Program of China(2022YFB2402600)the National Natural Science Foundation of China(11904379,51972329,52061160484,52125105,52188101)+1 种基金the Shenzhen Science and Technology Planning Project(JCYJ20210324101203009,JCYJ2020010911562492,JCYJ20190807171803813)the Guangdong Basic and Applied Basic Research Foundation(2022A1515011493,2019A1515011902,2019TX05L389,2020B0301030002).
文摘Solid-state lithium-metal batteries(SLMBs)have been regarded as one of the most promising next-generation devices because of their potential high safety,high energy density,and simple packing procedure.However,the practical applications of SLMBs are restricted by a series of static and dynamic interfacial issues,including poor interfacial contact,(electro-)chemical incompatibility,dynamic Li dendrite penetration,etc.In recent years,considerable attempts have been made to obtain mechanistic insight into interfacial failures and to develop possible strategies towards excellent interfacial properties for SLMBs.The static and dynamic failure mechanisms at interfaces between solid electrolytes(SEs)and electrodes are comprehensively summarized,and design strategies involving interfacial modification,electrode/SE engineering,and the monolithic construction of SLMBs are discussed in detail.Finally,possible research methodologies such as theoretical calcu-lations,advanced characterization techniques,and versatile design strategies are provided to tackle these interfacial problems.
基金supported by the National Natural Science Foundation of China(12204253,52502102,22502229)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(22KJB430039,24KJB150026)+3 种基金the Distinguished Young Scholars Fund of Jiangsu Province(BK20220061)the Training Programs of Innovation for Undergraduates(202510304023)the Collaborative Innovation Center of Suzhou Nano Science and Technologythe Large Instruments Open Foundation of Nantong University(KFJN2526)。
文摘The development of durable electrocatalysts overcoming activity-stability compromises remains pivotal for advancing anion-exchange membrane fuel cells(AEMFCs).Herein,we engineer a rare earth-incorporated Pd-based metallene(PdLaCe)through lanthanide-based bimetallic coordination,resolving critical limitations in oxygen reduction reaction(ORR)catalysis.Combined experimental characterization and theoretical simulations reveal that La/Ce dualdoping induces charge polarization to generate Pd^(δ-)-La/Ce^(δ+)active sites,synergistically optimizing the electronic structure via d-band center downshifting.This configuration weakens oxygen intermediate adsorption while enhancing structural integrity across thermal cycles.The optimized PdLaCe metallene delivers exceptional ORR performance,achieving a record half-wave potential of 0.903 V(vs.RHE)with negligible degradation(<6%)after 20,000 cycles,far surpassing commercial Pt/C benchmarks.Integrated into AEMFCs,it demonstrates a peak power density of 82.8 mW cm^(-2)alongside unprecedented stability(0.8 V for 22 h).Fundamental insights into lanthanide-induced charge redistribution establish a universal paradigm for designing robust multimetallic electrocatalysts via rare earth coordination engineering,bridging critical gaps between functional optimization and industrialscale fuel cell applications.This work provides transformative strategies for next-generation energy conversion systems requiring high efficiency and ultra-stability.
基金We acknowledge the financial support from National Natural Science Foundation of China(22109134)Guangdong Basic and Applied Basic Research Foundation(2022A1515010920)+1 种基金the Science and Technology Foundation of Shenzhen(JCYJ20190808153609561)the Open Research Found of Songshan Lake Materials Laboratory(2021SLABFN04)。
文摘Benefiting from the advantageous features of structural diversity and resource renewability,organic electroactive compounds are considered as attractive cathode materials for aqueous Zn-ion batteries(ZIBs).In this review,we discuss the recent developments of organic electrode materials for aqueous ZIBs.Although the proton(H^(+))storage chemistry in aqueous Zn-organic batteries has triggered an overwhelming literature surge in recent years,this topic remains controversial.Therefore,our review focuses on this significant issue and summarizes the reported electrochemical mechanisms,including pure Zn^(2+)intercalation,pure H^(+)storage,and H^(+)/Zn^(2+)co-storage.Moreover,the impact of H^(+)storage on the electrochemical performance of aqueous ZIBs is discussed systematically.Given the significance of H^(+)storage,we also highlight the relevant characterization methods employed.Finally,perspectives and directions on further understanding the charge storage mechanisms of organic materials are outlined.We hope that this review will stimulate more attention on the H^(+)storage chemistry of organic electrode materials to advance our understanding and further its application.
基金financially supported by the National Natural Science Foundation of China(52188101,Cheng HM,22275205,Peng J)Shenzhen Basic Research Project(JCYJ20200109144616617,Cheng HM)+5 种基金the Science and Technology Foundation of Shenzhen(JCYJ20220530154404010,Peng J)Guangdong Basic and Applied Basic Research Foundation(2023B1515020102,Peng J2022A1515110408,Chen ZJ)China Postdoctoral Science Foundation(2022M713270,Chen ZJ)the Cross Institute Joint Research Youth Team Project of SIAT(E25427,Peng J)supported by the public computing service platform provided by the Network and Computing Center of Huazhong University of Science and Technology。
文摘磁场触发的催化剂轨道电子自旋排列已成为促进析氧反应的一种有趣而可行的策略.然而,具有强d-d库仑相互作用的高熵合金(HEAs)催化剂中的磁场增强机制尚未得到充分挖掘.在此,我们设计了具有优异软磁性的高熵合金金属片,在微小磁场下表现出显著的磁场增强催化作用,其磁导率可作为评估磁场增强的描述因子.具体地,仅施加50 mT的磁场,(FeCoNi)_(82.5)Cr_(17.5)HEAs的过电位下降就超过了36mV@10 mA cm^(-2).此外,过电位的降低与HEA的磁导率呈线性关系.原位拉曼光谱与理论计算结果表明,施加磁场可显著提高自旋密度,改善催化剂的3d电子与*O自由基的2p轨道之间的自旋相互作用,从而有效降低速率决定步骤(*O→*OOH)的能量障碍,进而促进O-O的形成.
