Solar cells hold a function of photovoltaic conversion,while rechargeable metal batteries have an advantage of high energy storage.The conventional charge mode of batteries is made based on complete utilization of ele...Solar cells hold a function of photovoltaic conversion,while rechargeable metal batteries have an advantage of high energy storage.The conventional charge mode of batteries is made based on complete utilization of electric energy.The combination of solar cells and rechargeable metal batteries brings a new opportunity for the development of photo-assisted rechargeable batteries,in which the solar energy can be utilized to partially achieve photo-charging with or without external electrical bias.This review highlights the working mechanism and structure design of photo-assisted rechargeable metal batteries according to the characteristics of rechargeable metal batteries and advantage of the photovoltaic technology.In particular,the recent advances are introduced for photo-assisted rechargeable batteries based on light-weight metal anodes,including metal lithium,metal sodium,and metal zinc.The working features of the integrated devices are also discussed for energy saving under photo-assisted charging mode.Finally,a future outlook is provided for further improving the performance of photoassisted rechargeable metal batteries.展开更多
Correction to:Nano-Micro Lett.(2024)16:57 https://doi.org/10.1007/s40820-023-01288-y.Following publication of the original article[1],the authors reported that the order of the images in Figs.5 and 6 were reversed,the...Correction to:Nano-Micro Lett.(2024)16:57 https://doi.org/10.1007/s40820-023-01288-y.Following publication of the original article[1],the authors reported that the order of the images in Figs.5 and 6 were reversed,the positions of the images needed to be exchanged.Another mistake is that the author inadvertently copied the same image in Fig.2(f)with Fig.2(e).The correct Figs.2,5 and 6 have been provided in this correction.The original article[1]has been updated。展开更多
Hydrogen energy has emerged as a pivotal solution to address the global energy crisis and pave the way for a cleaner,low-carbon,secure,and efficient modern energy system.A key imperative in the utilization of hydrogen...Hydrogen energy has emerged as a pivotal solution to address the global energy crisis and pave the way for a cleaner,low-carbon,secure,and efficient modern energy system.A key imperative in the utilization of hydrogen energy lies in the development of high-performance hydrogen storage materials.Magnesium-based hydrogen storage materials exhibit remarkable advantages,including high hydrogen storage density,cost-effectiveness,and abundant magnesium resources,making them highly promising for the hydrogen energy sector.Nonetheless,practical applications of magnesium hydride for hydrogen storage face significant challenges,primarily due to their slow kinetics and stable thermodynamic properties.Herein,we briefly summarize the thermodynamic and kinetic properties of MgH2,encompassing strategies such as alloying,nanoscaling,catalyst doping,and composite system construction to enhance its hydrogen storage performance.Notably,nanoscaling and catalyst doping have emerged as more effective modification strategies.The discussion focuses on the thermodynamic changes induced by nanoscaling and the kinetic enhancements resulting from catalyst doping.Particular emphasis lies in the synergistic improvement strategy of incorporating nanocatalysts with confinement materials,and we revisit typical works on the multi-strategy optimization of MgH2.In conclusion,we conduct an analysis of outstanding challenges and issues,followed by presenting future research and development prospects for MgH2 as hydrogen storage materials.展开更多
The severe dependence of traditional phase change materials(PCMs)on the temperature-response and lattice deficiencies in versatility cannot satisfy demand for using such materials in complex application scenarios.Here...The severe dependence of traditional phase change materials(PCMs)on the temperature-response and lattice deficiencies in versatility cannot satisfy demand for using such materials in complex application scenarios.Here,we introduced metal ions to induce the self-assembly of MXene nanosheets and achieve their ordered arrangement by combining suction filtration and rapid freezing.Subsequently,a series of MXene/K^(+)/paraffin wax(PW)phase change composites(PCCs)were obtained via vacuum impregnation in molten PW.The prepared MXene-based PCCs showed versatile applications from macroscale technologies,successfully transforming solar,electric,and magnetic energy into thermal energy stored as latent heat in the PCCs.Moreover,due to the absence of binder in the MXene-based aerogel,MK3@PW exhibits a prime solar-thermal conversion efficiency(98.4%).Notably,MK3@PW can further convert the collected heat energy into electric energy through thermoelectric equipment and realize favorable solar-thermal-electric conversion(producing 206 mV of voltage with light radiation intensity of 200 mw cm^(−2)).An excellent Joule heat performance(reaching 105℃with an input voltage of 2.5 V)and responsive magnetic-thermal conversion behavior(a charging time of 11.8 s can achieve a thermal insulation effect of 285 s)for contactless thermotherapy were also demonstrated by the MK3@PW.Specifically,as a result of the ordered arrangement of MXene nanosheet self-assembly induced by potassium ions,MK3@PW PCC exhibits a higher electromagnetic shielding efficiency value(57.7 dB)than pure MXene aerogel/PW PCC(29.8 dB)with the same MXene mass.This work presents an opportunity for the multi-scene response and practical application of PCMs that satisfy demand of next-generation multifunctional PCCs.展开更多
W_(18)O_(49)nanowires(W_(18)O_(49)NWs)with unique one-dimension structures and excellent electron/ions transport properties have attracted increasing attention in academia and industry because of their potential appli...W_(18)O_(49)nanowires(W_(18)O_(49)NWs)with unique one-dimension structures and excellent electron/ions transport properties have attracted increasing attention in academia and industry because of their potential applications in many energy-related devices.In the past decades,many research articles related to W_(18)O_(49)have been published,but there are insufficient review articles focusing on W_(18)O_(49)NWs.In this review,we present the crystal structure of W_(18)O_(49)and briefly introduce the synthesis methods and growth mechanism of W_(18)O_(49)NWs.Moreover,their applications in energy conversion and storage devices are summarized.Finally,the current challenges and opportunities for applying W_(18)O_(49)NWs are provided.We hope this review can promote the development of W_(18)O_(49)NWs in energy conversion,storage,and other promising applications.展开更多
[4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid(Me-4PACz)self-assembled monolayer(SAM)as the hole transport materials have been demonstrated remarkable potential in perovskite solar cells(PSCs).However,the hyd...[4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid(Me-4PACz)self-assembled monolayer(SAM)as the hole transport materials have been demonstrated remarkable potential in perovskite solar cells(PSCs).However,the hydrophobicity of Me-4PACz presents a critical challenge for the fabrication of high-quality perovskite films due to its poor wettability.Here,a doped Al_(2)O_(3)with Me-4PACz to modify the Me-4PACz surface was proposed.On one hand,this approach improved the wettability of the Me-4PACz film,enhancing the coverage,uniformity,and buried interface properties of the perovskite film.On the other hand,compared to Al_(2)O_(3)modification alone,doping Al_(2)O_(3)with Me-4PACz allowed direct contact between the perovskite and Me-4PACz,resulting in better buried interface passivation.As a result,we achieved an efficiency of 22.71%for single-junction wide-bandgap perovskite solar cells(1.68 eV).Additionally,the efficiency of perovskite/silicon tandem solar cells was improved from 28.68%to 30.92%,with a significant reduction in hysteresis.Furthermore,the tandem cells demonstrated no degradation after 4200 s of operation at the maximum power point.展开更多
Heterogeneous solid frustrated-Lewis-pair(FLP)catalyst is of great promise in practical hydrogenation applications.It has been found that all-solid FLPs can be created on ceria via surface oxygen vacancy regulation.Co...Heterogeneous solid frustrated-Lewis-pair(FLP)catalyst is of great promise in practical hydrogenation applications.It has been found that all-solid FLPs can be created on ceria via surface oxygen vacancy regulation.Consequently,it is desired to investigate the mechanisms of the FLP-catalyzed hydrogenation of C=C and C=O and provide insight into the modification of CeO_(2)catalysts for the selective hydrogenation.In this work,the reaction mechanism of the hydrogenation of CH_(2)=CH_(2)and CH_(3)CH=O at the FLP sites constructed on CeO_(2)(110)surface was investigated by density functional theory(DFT),with the classical Lewis acid-base pairs(CLP)site as the reference.The results illustrate that at the CLP site,the dissociated hydride(H^(δ−))forms a stable H−O bond with the surface O atom,while at the FLP site,H^(δ−)is stabilized by Ce,displaying higher activity on the one hand.On the other hand,the electron cloud density of the Ce atom at the FLP site is higher,which can transfer more electrons to the adsorbed C_(C=C)and O_(C=O)atoms,leading to a higher degree of activation for C=C and C=O bonds,as indicated by the Bader charge analysis.Therefore,compared to the CLP site,the FLP site exhibits higher hydrogenation activity for CH_(2)=CH_(2)and CH_(3)CH=O.Furthermore,at the FLP sites,it demonstrates high efficiency in catalyzing the hydrogenation of CH_(2)=CH_(2)with the rate-determining barrier of 1.04 eV,but it shows limited activity for the hydrogenation of CH_(3)CH=O with the rate-determining barrier of 1.94 eV.It means that the selective hydrogenation of C=C can be effectively achieved at the FLP sites concerning selective hydrogenation catalysis.The insights shown in this work help to clarify the reaction mechanism of the hydrogenation of C=C and C=O at FLP site on CeO_(2)(110)and reveal the relationship between the catalytic performance and the nature of the active site,which is of great benefit to development of rational design of heterogeneous FLP catalysts.展开更多
Integrating multi-scale sites in a composite catalyst is vital to realize efficient electrocatalysis.Herein,a synergistic composite catalyst consisting of Co atomic sites and in-situ generated PtCo intermetallic compo...Integrating multi-scale sites in a composite catalyst is vital to realize efficient electrocatalysis.Herein,a synergistic composite catalyst consisting of Co atomic sites and in-situ generated PtCo intermetallic compounds (IMCs)(o-PtCo@CoNC) is proposed through Co pre-anchoring and subsequent impregnation-reduction method.High loading of Co atoms provides a chance for in-situ generating PtCo ordered intermetallic compounds.The remaining Co single atoms and PtCo IMCs construct synergistic electrocatalytic micro-regions.Benefiting from the ordered structure,synergistic effect of Pt Co IMCs and Co single atoms,o-PtCo@CoNC exhibits excellent electrocatalytic performance for oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) with mass activity of 1.21 A mgPt-1(at 0.9 V) and5.70 A mgPt-1(at an overpotential of 100 mV),respectively.Besides,o-PtCo@CoNC delivers negligible loss of half-wave potential and overpotential during long-term stability test in acid solutions,with 13 mV decay after 50,000 potential cycles for ORR and a 2.7 mV decay after 20,000 potential cycles for HER.The integration strategy of single-atomic sites coupled IMCs paves the way for enhancing the activity and durability of Pt-based electrocatalysts.展开更多
Catalytic electron donor-acceptor(EDA) complex photochemistry has recently emerged as a popular and sustainable alternative to photoredox synthetic methods. Yet, the catalytic EDA strategy is still in its infancy for ...Catalytic electron donor-acceptor(EDA) complex photochemistry has recently emerged as a popular and sustainable alternative to photoredox synthetic methods. Yet, the catalytic EDA strategy is still in its infancy for organic synthesis due to the challenges of designing novel catalytic paradigm and expanding the substrate and reaction scope. Here, we disclose a catalytic EDA/Cu cooperative strategy by employing Na I as a catalytic donor for copper-catalyzed radical asymmetric carbocyanation. A diverse range of synthetically useful chiral benzyl nitriles are produced with high enantioselectivities. This synergetic EDA/copper catalysis enables the decarboxylative cyanation without request of any photoredox catalysts, further expanding the synthetic potential of catalytic EDA chemistry in organic synthesis.展开更多
Electrochemical CO_(2) reduction(ECR)driven by intermittent renewable energy sources is an emerging technology to achieve net-zero CO_(2) emissions.Tandem electrochemical CO_(2) reduction(T-ECR),employs tandem catalys...Electrochemical CO_(2) reduction(ECR)driven by intermittent renewable energy sources is an emerging technology to achieve net-zero CO_(2) emissions.Tandem electrochemical CO_(2) reduction(T-ECR),employs tandem catalysts with synergistic or complementary functions to efficiently convert CO_(2) into multi-carbon(C^(2+))products in a succession of reactions within single or sequentially coupled reactors.However,the lack of clear interpretation and systematic understanding of T-ECR mechanisms has resulted in suboptimal current outcomes.This review presents new perspectives and summarizes recent advancements in efficient T-ECR across various scales,including synergistic tandem catalysis at the microscopic scale,relay tandem catalysis at the mesoscopic scale,and tandem reactors at the macroscopic scale.We begin by outlining the principle of tandem catalysis,followed by discuss on tandem catalyst design,the electrode construction,and reactor configuration.Additionally,we address the challenges and prospects of tandem strategies,emphasizing the integration of machine learning,theoretical calculations,and advanced characterization techniques for developing industry-scale CO_(2) valorization.展开更多
To get large dissymmetric factor(g_(lum))of organic circularly polarized luminescence(CPL)materials is still a great challenge.Although helical chirality and planar chirality are usual efficient access to enhancement ...To get large dissymmetric factor(g_(lum))of organic circularly polarized luminescence(CPL)materials is still a great challenge.Although helical chirality and planar chirality are usual efficient access to enhancement of CPL,they are not combined together to boost CPL.Here,a new tetraphenylethylene(TPE)tetracycle acid helicate bearing both helical chirality and planar chirality was designed and synthesized.Uniquely,synergy of the helical chirality and planar chirality was used to boost CPL signals both in solution and in helical self-assemblies.In the presence of octadecylamine,the TPE helicate could form helical nanofibers that emitted strong CPL signals with an absolute g_(lum)value up to 0.237.Exceptionally,followed by addition of para-phenylenediamine,the g_(lum)value was successively increased to 0.387 due to formation of bigger helical nanofibers.Compared with that of TPE helicate itself,the CPL signal of the self-assemblies was not only magnified by 104-fold but also inversed,which was very rare result for CPL-active materials.Surprisingly,the interaction of TPE helicate with xylylenediamine even gave a gel,which was transformed into suspension by shaking.Unexpectedly,the suspension showed 40-fold stronger CPL signals than the gel with signal direction inversion each other.Using synergy of the helical chirality and planar chirality to significantly boost CPL intensity provides a new strategy in preparation of organic CPL materials having very large g_(lum)value.展开更多
Pyridine(Py) and 3-methylpyridine(3-MP) are crucial intermediates in chemical industrial processes.Here,we provide a simple and energy-efficient approach for the isolation of Py and 3-MP by employing crystalline cucur...Pyridine(Py) and 3-methylpyridine(3-MP) are crucial intermediates in chemical industrial processes.Here,we provide a simple and energy-efficient approach for the isolation of Py and 3-MP by employing crystalline cucurbit[6]uril(Q[6]).The crystal exhibit high selectivity for Py from the mixture of Py and 3-MP in both vapor and liquid phases,with separation purities close to 100%.The selectivity is attributed to the varying stability of the host-vip complexes after the absorption of Py or 3-MP,as revealed by the single-crystal structure analysis.ITC experimental results and DFT calculations indicate that,compared to3-MP,Q[6] has a higher binding strength and lower binding energy with Py.In addition,pyridine can be removed from the Q[6] cavity through vacuum heating or organic solvent immersion,enabling Q[6]reuse via reversible vip loading.This method offers a promising approach for high-purity Py and 3-MP separation with significant economic and environmental benefits.展开更多
The integrated technology of interfacial solar steam generation and photo-Fenton oxidation has emerged as a promising way to simultaneously mitigate freshwater scarcity and degrade organic pollutants.However,fabricati...The integrated technology of interfacial solar steam generation and photo-Fenton oxidation has emerged as a promising way to simultaneously mitigate freshwater scarcity and degrade organic pollutants.However,fabricating low-cost,multi-functional evaporators with high water evaporation and catalytic ability still presents a significant challenge.Herein,we report the functional upcycling of waste polyimide into semiconducting Fe-BTEC and subsequently construct Fe-BTEC-based composite evaporators for simultaneous freshwater production and photo-Fenton degradation of pollutants.Firstly,through a two-step solvothermal-solution stirring method,Fe-BTEC nanoparticles with the size of 20-100 nm are massively produced from waste polyimide,with a band gap energy of 2.2 eV.The composite evaporator based on Fe-BTEC and graphene possesses wide solar-spectrum absorption capacity,high photothermal conversion capacity,rapid delivery of water,and low enthalpy of evaporation.Benefiting from the merits above,the composite evaporator achieves a high evaporation rate of 2.72kgm^(-2) h^(-1) from tetracycline solution,as well as the photothermal conversion efficiency of 97%when exposed to irradiation of 1 Sun,superior to many evaporators.What is more,the evaporator exhibits the tetracycline degradation rate of 99.6%with good recycling stability,ranking as one of the most powerful heterogeneous Fenton catalysts.COMSOL Multiphysics and density functional theory calculation results prove the synergistic effect of the concentrated heat produced by interfacial solar steam generation and catalytic active sites of Fe-BTEC on promoting H_(2)O_(2) activation to form reactive oxidation radicals.This work not only provides a green strategy for upcycling waste polyimide,but also proposes a new approach to fabricate multi-functional evaporators.展开更多
High entropy alloy(HEA)based materials have been extensively investigated as viable catalysts in hydrogen storage for their unique properties.Herein,we demonstrate a relatively mild synthesis strategy for constructing...High entropy alloy(HEA)based materials have been extensively investigated as viable catalysts in hydrogen storage for their unique properties.Herein,we demonstrate a relatively mild synthesis strategy for constructing carbon-supported by NiCoFeCuMg HEA(NiCoFe-CuMg@C)nanocatalysts by utilizing polymetallic metal-organic frameworks(MOFs)as precursors.The incorporation of prepared catalysts into MgH_(2) greatly improved the hydrogen storage performance:the MgH_(2)+NiCoFeCuMg@C composite can rapidly desorb 6.01 wt%H2 at 325℃,and the initial dehydrogenation temperature decreased to 167.2℃,nearly 163.8℃ lower than that of the pure MgH_(2).Besides,the composite exhibits a fairly stable reversible capacity with 97%capacity retention after 20 cycles.Most importantly,ex-situ structural characterization reveals that the synergistic effects of the“hydrogen pump”role of Mg_(2)Ni(Cu)/Mg_(2)Ni(Cu)H_(4) and“hydrogen gateway”role of Co3Fe7,as well as the excellent dispersion function of carbon material,contribute to the outstanding hydrogen storage properties of the MgH_(2)+NiCoFeCuMg@C composite.This study provides valuable insights into the performance improvement of carbon-supported HEA catalysts in modification of MgH_(2).展开更多
Polyphosphazene with phenoxy or 4-ester phenoxy as pendent groups are demonstrated as both ligands and host matrices for CsPbBr_(3) perovskite nanocrystals(NCs). These polymers produced fiexible nanocomposite films wi...Polyphosphazene with phenoxy or 4-ester phenoxy as pendent groups are demonstrated as both ligands and host matrices for CsPbBr_(3) perovskite nanocrystals(NCs). These polymers produced fiexible nanocomposite films with excellent NCs dispersion, optical transparency and stability in various extreme conditions. Both films remained stable even after 30 days of air storage. CsPbBr_(3) /poly[bis(phenoxy phosphazene)](PBPP) delivered better air and light stability, and CsPbBr_(3) /poly[bis(4-esterphenoxy)phosphazene](PBEPP) exhibited superior water and heat resistance. CsPbBr_(3) /PBEPP showed a greater increase in fiuorescence intensity under 365 nm UV light and demonstrated a 10% luminescence increase after 96 h of water immersion and even at high temperature(150℃). These findings thus provide new insight into fiexible luminescent CsPbBr_(3) films with high stability in optoelectronic applications.展开更多
Fiber fabrics have been wildly utilized for solar interracial evaporators to address freshwater scarcity.However,the complex and expensive manufacturing processes remain limited to their scalable development.Herein,a ...Fiber fabrics have been wildly utilized for solar interracial evaporators to address freshwater scarcity.However,the complex and expensive manufacturing processes remain limited to their scalable development.Herein,a fabric-based Janus interracial evaporator is efficiently fabricated on a large scale by integrating an extremely innovative self-designed melt-centrifugal spinning technology with spray coating technology.The prepared fabric-based Janus interfacial evaporator has differential hydrophilicity,uneven surfaces,and channels that allow moisture escape.Benefiting from the excellent photothermai conversion of graphene oxide and the charge transfer actions of titanium dioxide,such a multifunction evaporator can reach a high evaporation rate of 1.72 kg m^(-2)h^(-1)under 1 sun irradiation,a superior antibacterial rate of 99%,excellent photocatalytic degradation,and effective thermoelectric ability simultaneously.Moreover,it also shows fantastic performance in salt resistance,recyclable evaporation,and real desalination,This work demonstrates a high-efficiency,cost-effective,multifunctional,and scalable strategy for high-performance fiber fabrics solar interfacial evaporation.展开更多
Ships experience rolling motion under the action of sea waves and may even face the risk of capsizing.Anti-rolling devices are designed to reduce this motion and enhance vessel safety.This is especially critical for e...Ships experience rolling motion under the action of sea waves and may even face the risk of capsizing.Anti-rolling devices are designed to reduce this motion and enhance vessel safety.This is especially critical for engineering ships operating at sea under zero-speed conditions,where a stable posture is essential for efficient performance.Gyro stabilizers can suppress roll motion at zero speed;however,their high cost typically makes them unsuitable for large civilian vessels.Additionally,most existing anti-rolling devices rely on a certain water speed to function,which results in increased drag.In this study,an anti-rolling system incorporating swing control is proposed.Inspired by the human body's ability to maintain balance by swinging arms during walking or running,the system generates an antirolling moment by oscillating a water tank.This approach operates independently of water speed and does not generate additional drag.The mechanical design of the anti-rolling system is introduced,and a corresponding control system model is derived.The swing-tank mechanism provides phase lead compensation and reduces the system's sensitivity to wave disturbances.To enhance performance,robust control techniques are applied.Simulation results demonstrate that the proposed anti-rolling system delivers effective roll reduction for ships.展开更多
The heterogeneity ofα-Al(Fe,Mn)Si dispersoids andβ″precipitates was tuned to enhance the strength−ductility synergy of air-cooled Al−Mg−Si alloys.Scanning electron microscopy(SEM)and transmission electron microscop...The heterogeneity ofα-Al(Fe,Mn)Si dispersoids andβ″precipitates was tuned to enhance the strength−ductility synergy of air-cooled Al−Mg−Si alloys.Scanning electron microscopy(SEM)and transmission electron microscopy(TEM)were employed to elucidate the microstructural parameters of these two strengthening phases.The results show that the microstructural heterogeneity can be triggered by the absence of homogenization,resulting in the presence of dispersoid-free zones(DFZs)and dispersoid zones(DZs),in conjunction with bimodalβ″precipitates.Further analytical calculations,from the strengthening model,clarify that the strategically dispersedα-Al(Fe,Mn)Si andβ″particles create“soft”and“hard”domains within the alloy,resultantly improving the mechanical properties.展开更多
Light-driven CO_(2) reduction reaction(CO_(2)RR)to value-added ethylene(C2H4)holds significant promise for addressing energy and environmental challenges.While the high energy barriers for*CO intermediates hydrogenati...Light-driven CO_(2) reduction reaction(CO_(2)RR)to value-added ethylene(C2H4)holds significant promise for addressing energy and environmental challenges.While the high energy barriers for*CO intermediates hydrogenation and C–C coupling limit the C_(2)H_(4)generation.Herein,CuxP/g-C_(3)N_(4) heterojunction prepared by an in-situ phosphating technique,achieved collaborative photocatalytic CO_(2) and H2O,producing CO and C_(2)H_(4)as the main products.Notably,the selectivity of C_(2)H_(4)produced by CuxP/g-C_(3)N_(4) attained to 64.25%,which was 9.85 times that of CuxP(6.52%).Detailed time-resolution photoluminescence spectra,femtosecond transient absorption spectroscopy tests and density functional theory(DFT)calculation validate the ultra-fast interfacial electron transfer mechanism in CuxP/g-C_(3)N_(4) heterojunction.Successive*H on P sites caused by adsorbed H2O splitting with moderate hydrogenation ability enables the multi-step hydrogenation during CO_(2)RR process over CuxP/g-C_(3)N_(4).With the aid of mediated asymmetric Cu and P dual sites by g-C_(3)N_(4) nanosheet,the produced*CHO shows an energetically favorable for C–C coupling.The coupling formed*CHOCHO further accepts photoexcited efficient e–and*H to deeply produce C_(2)H_(4)according to the C^(2+)intermediates,which has been detected by in-situ diffuse reflectance infrared Fourier transform spectroscopy and interpreted by DFT calculation.The novel insight mechanism offers an essential understanding for the development of CuxP-based heterojunctions for photocatalytic CO_(2) to C^(2+)value-added fuels.展开更多
Rechargeable metal-air batteries have gained significant interest due to their high energy density and environmental benignity.However,these batteries face significant challenges,particularly related to the air-breath...Rechargeable metal-air batteries have gained significant interest due to their high energy density and environmental benignity.However,these batteries face significant challenges,particularly related to the air-breathing electrode,resulting in poor cycle life,low efficiency,and catalyst degradation.Developing a robust bifunctional electrocatalyst remains difficult,as oxygen electrocatalysis involves sluggish kinetics and follows different reaction pathways,often requiring distinct active sites.Consequently,the poorly understood mechanisms and irreversible surface reconstruction in the catalyst’s microenvironment,such as atomic modulation,nano-/microscale,and surface interfaces,lead to accelerated degradation during charge and discharge cycles.Overcoming these barriers requires advancements in the development and understanding of bifunctional electrocatalysts.In this review,the critical components of metal-air batteries,the associated challenges,and the current engineering approaches to address these issues are discussed.Additionally,the mechanisms of oxygen electrocatalysis on the air electrodes are examined,along with insights into how chemical characteristics of materials influence these mechanisms.Furthermore,recent advances in bifunctional electrocatalysts are highlighted,with an emphasis on the synthesis strategies,microenvironmental modulations,and stabilized systems demonstrating efficient performance,particularly zinc-and lithium-air batteries.Finally,perspectives and future research directions are provided for designing efficient and durable bifunctional electrocatalysts for metal-air batteries.展开更多
基金Financial supports from National Natural Science Foundation(21875123)of Chinathe project of Jiangxi Academy of Sciences(2020-YZD-3)are gratefully acknowledged.
文摘Solar cells hold a function of photovoltaic conversion,while rechargeable metal batteries have an advantage of high energy storage.The conventional charge mode of batteries is made based on complete utilization of electric energy.The combination of solar cells and rechargeable metal batteries brings a new opportunity for the development of photo-assisted rechargeable batteries,in which the solar energy can be utilized to partially achieve photo-charging with or without external electrical bias.This review highlights the working mechanism and structure design of photo-assisted rechargeable metal batteries according to the characteristics of rechargeable metal batteries and advantage of the photovoltaic technology.In particular,the recent advances are introduced for photo-assisted rechargeable batteries based on light-weight metal anodes,including metal lithium,metal sodium,and metal zinc.The working features of the integrated devices are also discussed for energy saving under photo-assisted charging mode.Finally,a future outlook is provided for further improving the performance of photoassisted rechargeable metal batteries.
文摘Correction to:Nano-Micro Lett.(2024)16:57 https://doi.org/10.1007/s40820-023-01288-y.Following publication of the original article[1],the authors reported that the order of the images in Figs.5 and 6 were reversed,the positions of the images needed to be exchanged.Another mistake is that the author inadvertently copied the same image in Fig.2(f)with Fig.2(e).The correct Figs.2,5 and 6 have been provided in this correction.The original article[1]has been updated。
基金supported by National Key Research and Development Program of China(2021YFB4000604)National Natural Science Foundation of China(52271220)111 Project(B12015)and the Fundamental Research Funds for the Central Universities.
文摘Hydrogen energy has emerged as a pivotal solution to address the global energy crisis and pave the way for a cleaner,low-carbon,secure,and efficient modern energy system.A key imperative in the utilization of hydrogen energy lies in the development of high-performance hydrogen storage materials.Magnesium-based hydrogen storage materials exhibit remarkable advantages,including high hydrogen storage density,cost-effectiveness,and abundant magnesium resources,making them highly promising for the hydrogen energy sector.Nonetheless,practical applications of magnesium hydride for hydrogen storage face significant challenges,primarily due to their slow kinetics and stable thermodynamic properties.Herein,we briefly summarize the thermodynamic and kinetic properties of MgH2,encompassing strategies such as alloying,nanoscaling,catalyst doping,and composite system construction to enhance its hydrogen storage performance.Notably,nanoscaling and catalyst doping have emerged as more effective modification strategies.The discussion focuses on the thermodynamic changes induced by nanoscaling and the kinetic enhancements resulting from catalyst doping.Particular emphasis lies in the synergistic improvement strategy of incorporating nanocatalysts with confinement materials,and we revisit typical works on the multi-strategy optimization of MgH2.In conclusion,we conduct an analysis of outstanding challenges and issues,followed by presenting future research and development prospects for MgH2 as hydrogen storage materials.
基金the National Natural Science Foundation of China[grant numbers 52203038,52173036 and 52073107]the National Key Technology R&D Program of China[grant number 2022YFC3901904,2022YFC3901903,and 2020YFB1709301]the Central University Basic Research Fund of China[grant number 2021XXJS035].
文摘The severe dependence of traditional phase change materials(PCMs)on the temperature-response and lattice deficiencies in versatility cannot satisfy demand for using such materials in complex application scenarios.Here,we introduced metal ions to induce the self-assembly of MXene nanosheets and achieve their ordered arrangement by combining suction filtration and rapid freezing.Subsequently,a series of MXene/K^(+)/paraffin wax(PW)phase change composites(PCCs)were obtained via vacuum impregnation in molten PW.The prepared MXene-based PCCs showed versatile applications from macroscale technologies,successfully transforming solar,electric,and magnetic energy into thermal energy stored as latent heat in the PCCs.Moreover,due to the absence of binder in the MXene-based aerogel,MK3@PW exhibits a prime solar-thermal conversion efficiency(98.4%).Notably,MK3@PW can further convert the collected heat energy into electric energy through thermoelectric equipment and realize favorable solar-thermal-electric conversion(producing 206 mV of voltage with light radiation intensity of 200 mw cm^(−2)).An excellent Joule heat performance(reaching 105℃with an input voltage of 2.5 V)and responsive magnetic-thermal conversion behavior(a charging time of 11.8 s can achieve a thermal insulation effect of 285 s)for contactless thermotherapy were also demonstrated by the MK3@PW.Specifically,as a result of the ordered arrangement of MXene nanosheet self-assembly induced by potassium ions,MK3@PW PCC exhibits a higher electromagnetic shielding efficiency value(57.7 dB)than pure MXene aerogel/PW PCC(29.8 dB)with the same MXene mass.This work presents an opportunity for the multi-scene response and practical application of PCMs that satisfy demand of next-generation multifunctional PCCs.
基金Financial support from the National Natural Science Foundation(No.22075151)of Chinathe Natural Science Foundation of Jiangxi(No.20161BBE50095)the project of Jiangxi Academy of Sciences(No.2022YSBG21019 and No.2023YJC2018)is gratefully acknowledged。
文摘W_(18)O_(49)nanowires(W_(18)O_(49)NWs)with unique one-dimension structures and excellent electron/ions transport properties have attracted increasing attention in academia and industry because of their potential applications in many energy-related devices.In the past decades,many research articles related to W_(18)O_(49)have been published,but there are insufficient review articles focusing on W_(18)O_(49)NWs.In this review,we present the crystal structure of W_(18)O_(49)and briefly introduce the synthesis methods and growth mechanism of W_(18)O_(49)NWs.Moreover,their applications in energy conversion and storage devices are summarized.Finally,the current challenges and opportunities for applying W_(18)O_(49)NWs are provided.We hope this review can promote the development of W_(18)O_(49)NWs in energy conversion,storage,and other promising applications.
基金supported by the National Key Research and Development Program of China(2023YFB4202503)the cooperation project between Three Gorges Corporation and Nankai University(202103571)+6 种基金the National Natural Science Foundation Joint Fund(U21A2072)the National Science Foundation(62274099,62104115)Tianjin Science and Technology Project(24ZXZSSS00160)Yunnan Provincial Science and Technology Project at Southwest United Graduate School(202302A0370009)the China Higher Education Discipline Innovation Overseas Expert Introduction Project(B16027)the Haihe Laboratory of Sustainable Chemical Transformationsthe Fundamental Research Funds for the Central Universities,Nankai University。
文摘[4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid(Me-4PACz)self-assembled monolayer(SAM)as the hole transport materials have been demonstrated remarkable potential in perovskite solar cells(PSCs).However,the hydrophobicity of Me-4PACz presents a critical challenge for the fabrication of high-quality perovskite films due to its poor wettability.Here,a doped Al_(2)O_(3)with Me-4PACz to modify the Me-4PACz surface was proposed.On one hand,this approach improved the wettability of the Me-4PACz film,enhancing the coverage,uniformity,and buried interface properties of the perovskite film.On the other hand,compared to Al_(2)O_(3)modification alone,doping Al_(2)O_(3)with Me-4PACz allowed direct contact between the perovskite and Me-4PACz,resulting in better buried interface passivation.As a result,we achieved an efficiency of 22.71%for single-junction wide-bandgap perovskite solar cells(1.68 eV).Additionally,the efficiency of perovskite/silicon tandem solar cells was improved from 28.68%to 30.92%,with a significant reduction in hysteresis.Furthermore,the tandem cells demonstrated no degradation after 4200 s of operation at the maximum power point.
基金supported by the National Natural Science Foundation of China(22302115,22072079)the Fundamental Research Program of Shanxi Province(202303021221056).
文摘Heterogeneous solid frustrated-Lewis-pair(FLP)catalyst is of great promise in practical hydrogenation applications.It has been found that all-solid FLPs can be created on ceria via surface oxygen vacancy regulation.Consequently,it is desired to investigate the mechanisms of the FLP-catalyzed hydrogenation of C=C and C=O and provide insight into the modification of CeO_(2)catalysts for the selective hydrogenation.In this work,the reaction mechanism of the hydrogenation of CH_(2)=CH_(2)and CH_(3)CH=O at the FLP sites constructed on CeO_(2)(110)surface was investigated by density functional theory(DFT),with the classical Lewis acid-base pairs(CLP)site as the reference.The results illustrate that at the CLP site,the dissociated hydride(H^(δ−))forms a stable H−O bond with the surface O atom,while at the FLP site,H^(δ−)is stabilized by Ce,displaying higher activity on the one hand.On the other hand,the electron cloud density of the Ce atom at the FLP site is higher,which can transfer more electrons to the adsorbed C_(C=C)and O_(C=O)atoms,leading to a higher degree of activation for C=C and C=O bonds,as indicated by the Bader charge analysis.Therefore,compared to the CLP site,the FLP site exhibits higher hydrogenation activity for CH_(2)=CH_(2)and CH_(3)CH=O.Furthermore,at the FLP sites,it demonstrates high efficiency in catalyzing the hydrogenation of CH_(2)=CH_(2)with the rate-determining barrier of 1.04 eV,but it shows limited activity for the hydrogenation of CH_(3)CH=O with the rate-determining barrier of 1.94 eV.It means that the selective hydrogenation of C=C can be effectively achieved at the FLP sites concerning selective hydrogenation catalysis.The insights shown in this work help to clarify the reaction mechanism of the hydrogenation of C=C and C=O at FLP site on CeO_(2)(110)and reveal the relationship between the catalytic performance and the nature of the active site,which is of great benefit to development of rational design of heterogeneous FLP catalysts.
基金National Natural Science Foundation of China (22279036)Innovation and Talent Recruitment Base of New Energy Chemistry and Device (B21003)。
文摘Integrating multi-scale sites in a composite catalyst is vital to realize efficient electrocatalysis.Herein,a synergistic composite catalyst consisting of Co atomic sites and in-situ generated PtCo intermetallic compounds (IMCs)(o-PtCo@CoNC) is proposed through Co pre-anchoring and subsequent impregnation-reduction method.High loading of Co atoms provides a chance for in-situ generating PtCo ordered intermetallic compounds.The remaining Co single atoms and PtCo IMCs construct synergistic electrocatalytic micro-regions.Benefiting from the ordered structure,synergistic effect of Pt Co IMCs and Co single atoms,o-PtCo@CoNC exhibits excellent electrocatalytic performance for oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) with mass activity of 1.21 A mgPt-1(at 0.9 V) and5.70 A mgPt-1(at an overpotential of 100 mV),respectively.Besides,o-PtCo@CoNC delivers negligible loss of half-wave potential and overpotential during long-term stability test in acid solutions,with 13 mV decay after 50,000 potential cycles for ORR and a 2.7 mV decay after 20,000 potential cycles for HER.The integration strategy of single-atomic sites coupled IMCs paves the way for enhancing the activity and durability of Pt-based electrocatalysts.
基金the National Natural Science Foundation of China (No. 22201087) for the financial support。
文摘Catalytic electron donor-acceptor(EDA) complex photochemistry has recently emerged as a popular and sustainable alternative to photoredox synthetic methods. Yet, the catalytic EDA strategy is still in its infancy for organic synthesis due to the challenges of designing novel catalytic paradigm and expanding the substrate and reaction scope. Here, we disclose a catalytic EDA/Cu cooperative strategy by employing Na I as a catalytic donor for copper-catalyzed radical asymmetric carbocyanation. A diverse range of synthetically useful chiral benzyl nitriles are produced with high enantioselectivities. This synergetic EDA/copper catalysis enables the decarboxylative cyanation without request of any photoredox catalysts, further expanding the synthetic potential of catalytic EDA chemistry in organic synthesis.
文摘Electrochemical CO_(2) reduction(ECR)driven by intermittent renewable energy sources is an emerging technology to achieve net-zero CO_(2) emissions.Tandem electrochemical CO_(2) reduction(T-ECR),employs tandem catalysts with synergistic or complementary functions to efficiently convert CO_(2) into multi-carbon(C^(2+))products in a succession of reactions within single or sequentially coupled reactors.However,the lack of clear interpretation and systematic understanding of T-ECR mechanisms has resulted in suboptimal current outcomes.This review presents new perspectives and summarizes recent advancements in efficient T-ECR across various scales,including synergistic tandem catalysis at the microscopic scale,relay tandem catalysis at the mesoscopic scale,and tandem reactors at the macroscopic scale.We begin by outlining the principle of tandem catalysis,followed by discuss on tandem catalyst design,the electrode construction,and reactor configuration.Additionally,we address the challenges and prospects of tandem strategies,emphasizing the integration of machine learning,theoretical calculations,and advanced characterization techniques for developing industry-scale CO_(2) valorization.
基金National Natural Science Foundation of China(Nos.22072050,22372066 and 22301090)the Open Research Fund(No.2024JYBKF05)of Key Laboratory of Material Chemistry for Energy Conversion and Storage(HUST)Ministry of Educationthe China Postdoctoral Science Foundation(No.2023M731189)for financial support,and thank the Analytical and Testing Centre at Huazhong University of Science and Technology for measurement.
文摘To get large dissymmetric factor(g_(lum))of organic circularly polarized luminescence(CPL)materials is still a great challenge.Although helical chirality and planar chirality are usual efficient access to enhancement of CPL,they are not combined together to boost CPL.Here,a new tetraphenylethylene(TPE)tetracycle acid helicate bearing both helical chirality and planar chirality was designed and synthesized.Uniquely,synergy of the helical chirality and planar chirality was used to boost CPL signals both in solution and in helical self-assemblies.In the presence of octadecylamine,the TPE helicate could form helical nanofibers that emitted strong CPL signals with an absolute g_(lum)value up to 0.237.Exceptionally,followed by addition of para-phenylenediamine,the g_(lum)value was successively increased to 0.387 due to formation of bigger helical nanofibers.Compared with that of TPE helicate itself,the CPL signal of the self-assemblies was not only magnified by 104-fold but also inversed,which was very rare result for CPL-active materials.Surprisingly,the interaction of TPE helicate with xylylenediamine even gave a gel,which was transformed into suspension by shaking.Unexpectedly,the suspension showed 40-fold stronger CPL signals than the gel with signal direction inversion each other.Using synergy of the helical chirality and planar chirality to significantly boost CPL intensity provides a new strategy in preparation of organic CPL materials having very large g_(lum)value.
基金supported by the Guizhou Provincial Basic Research Program(Natural Science) Youth Guidance(Nos.[2024]110,[2024]378)Science and Technology Innovation Team of Natural Science Foundation of Guizhou Province(No.CXTD[2023]005)+3 种基金Science and Technology Innovation Team of Higher Education Department of Guizhou Province(No.QJJ[2023]053)Natural Science Special of Guizhou University(No.202137)Guizhou Provincial Key Laboratory Platform Project(No.ZSYS[2025]008)PhD Foundation of Guizhou University(No.[2021]83)。
文摘Pyridine(Py) and 3-methylpyridine(3-MP) are crucial intermediates in chemical industrial processes.Here,we provide a simple and energy-efficient approach for the isolation of Py and 3-MP by employing crystalline cucurbit[6]uril(Q[6]).The crystal exhibit high selectivity for Py from the mixture of Py and 3-MP in both vapor and liquid phases,with separation purities close to 100%.The selectivity is attributed to the varying stability of the host-vip complexes after the absorption of Py or 3-MP,as revealed by the single-crystal structure analysis.ITC experimental results and DFT calculations indicate that,compared to3-MP,Q[6] has a higher binding strength and lower binding energy with Py.In addition,pyridine can be removed from the Q[6] cavity through vacuum heating or organic solvent immersion,enabling Q[6]reuse via reversible vip loading.This method offers a promising approach for high-purity Py and 3-MP separation with significant economic and environmental benefits.
基金supported by the National Natural Science Foundation of China(No.52373099)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(No.B21003)。
文摘The integrated technology of interfacial solar steam generation and photo-Fenton oxidation has emerged as a promising way to simultaneously mitigate freshwater scarcity and degrade organic pollutants.However,fabricating low-cost,multi-functional evaporators with high water evaporation and catalytic ability still presents a significant challenge.Herein,we report the functional upcycling of waste polyimide into semiconducting Fe-BTEC and subsequently construct Fe-BTEC-based composite evaporators for simultaneous freshwater production and photo-Fenton degradation of pollutants.Firstly,through a two-step solvothermal-solution stirring method,Fe-BTEC nanoparticles with the size of 20-100 nm are massively produced from waste polyimide,with a band gap energy of 2.2 eV.The composite evaporator based on Fe-BTEC and graphene possesses wide solar-spectrum absorption capacity,high photothermal conversion capacity,rapid delivery of water,and low enthalpy of evaporation.Benefiting from the merits above,the composite evaporator achieves a high evaporation rate of 2.72kgm^(-2) h^(-1) from tetracycline solution,as well as the photothermal conversion efficiency of 97%when exposed to irradiation of 1 Sun,superior to many evaporators.What is more,the evaporator exhibits the tetracycline degradation rate of 99.6%with good recycling stability,ranking as one of the most powerful heterogeneous Fenton catalysts.COMSOL Multiphysics and density functional theory calculation results prove the synergistic effect of the concentrated heat produced by interfacial solar steam generation and catalytic active sites of Fe-BTEC on promoting H_(2)O_(2) activation to form reactive oxidation radicals.This work not only provides a green strategy for upcycling waste polyimide,but also proposes a new approach to fabricate multi-functional evaporators.
基金supported by National Key Research and Development Program of China(2021YFB4000604)National Natural Science Foundation of China(52271220)+1 种基金111 Project(B12015)the Fundamental Research Funds for the Central Universities.
文摘High entropy alloy(HEA)based materials have been extensively investigated as viable catalysts in hydrogen storage for their unique properties.Herein,we demonstrate a relatively mild synthesis strategy for constructing carbon-supported by NiCoFeCuMg HEA(NiCoFe-CuMg@C)nanocatalysts by utilizing polymetallic metal-organic frameworks(MOFs)as precursors.The incorporation of prepared catalysts into MgH_(2) greatly improved the hydrogen storage performance:the MgH_(2)+NiCoFeCuMg@C composite can rapidly desorb 6.01 wt%H2 at 325℃,and the initial dehydrogenation temperature decreased to 167.2℃,nearly 163.8℃ lower than that of the pure MgH_(2).Besides,the composite exhibits a fairly stable reversible capacity with 97%capacity retention after 20 cycles.Most importantly,ex-situ structural characterization reveals that the synergistic effects of the“hydrogen pump”role of Mg_(2)Ni(Cu)/Mg_(2)Ni(Cu)H_(4) and“hydrogen gateway”role of Co3Fe7,as well as the excellent dispersion function of carbon material,contribute to the outstanding hydrogen storage properties of the MgH_(2)+NiCoFeCuMg@C composite.This study provides valuable insights into the performance improvement of carbon-supported HEA catalysts in modification of MgH_(2).
基金supported by the National Science Foundation (NSF) of China (No. 51773010)the Weifang Science and Technology Development Plan Program (No. 2023GX005)。
文摘Polyphosphazene with phenoxy or 4-ester phenoxy as pendent groups are demonstrated as both ligands and host matrices for CsPbBr_(3) perovskite nanocrystals(NCs). These polymers produced fiexible nanocomposite films with excellent NCs dispersion, optical transparency and stability in various extreme conditions. Both films remained stable even after 30 days of air storage. CsPbBr_(3) /poly[bis(phenoxy phosphazene)](PBPP) delivered better air and light stability, and CsPbBr_(3) /poly[bis(4-esterphenoxy)phosphazene](PBEPP) exhibited superior water and heat resistance. CsPbBr_(3) /PBEPP showed a greater increase in fiuorescence intensity under 365 nm UV light and demonstrated a 10% luminescence increase after 96 h of water immersion and even at high temperature(150℃). These findings thus provide new insight into fiexible luminescent CsPbBr_(3) films with high stability in optoelectronic applications.
基金the National Key Research and Development Program of China(Grant No.2022YFC3901902)the National Natural Science Foundation of China(Grant Nos.52203037,52103031,and 52073107)。
文摘Fiber fabrics have been wildly utilized for solar interracial evaporators to address freshwater scarcity.However,the complex and expensive manufacturing processes remain limited to their scalable development.Herein,a fabric-based Janus interracial evaporator is efficiently fabricated on a large scale by integrating an extremely innovative self-designed melt-centrifugal spinning technology with spray coating technology.The prepared fabric-based Janus interfacial evaporator has differential hydrophilicity,uneven surfaces,and channels that allow moisture escape.Benefiting from the excellent photothermai conversion of graphene oxide and the charge transfer actions of titanium dioxide,such a multifunction evaporator can reach a high evaporation rate of 1.72 kg m^(-2)h^(-1)under 1 sun irradiation,a superior antibacterial rate of 99%,excellent photocatalytic degradation,and effective thermoelectric ability simultaneously.Moreover,it also shows fantastic performance in salt resistance,recyclable evaporation,and real desalination,This work demonstrates a high-efficiency,cost-effective,multifunctional,and scalable strategy for high-performance fiber fabrics solar interfacial evaporation.
基金supported by the Jiangxi University of Water Resources and Electric Power Doctoral Research Initiation Fund(Grant No.2024kyqd030)。
文摘Ships experience rolling motion under the action of sea waves and may even face the risk of capsizing.Anti-rolling devices are designed to reduce this motion and enhance vessel safety.This is especially critical for engineering ships operating at sea under zero-speed conditions,where a stable posture is essential for efficient performance.Gyro stabilizers can suppress roll motion at zero speed;however,their high cost typically makes them unsuitable for large civilian vessels.Additionally,most existing anti-rolling devices rely on a certain water speed to function,which results in increased drag.In this study,an anti-rolling system incorporating swing control is proposed.Inspired by the human body's ability to maintain balance by swinging arms during walking or running,the system generates an antirolling moment by oscillating a water tank.This approach operates independently of water speed and does not generate additional drag.The mechanical design of the anti-rolling system is introduced,and a corresponding control system model is derived.The swing-tank mechanism provides phase lead compensation and reduces the system's sensitivity to wave disturbances.To enhance performance,robust control techniques are applied.Simulation results demonstrate that the proposed anti-rolling system delivers effective roll reduction for ships.
基金supported by the National Natural Science Foundation of China(Nos.52301025,52371065,52301179)the Fundamental Research Program of Shanxi Province,China(Nos.202203021222039,202203021212124)。
文摘The heterogeneity ofα-Al(Fe,Mn)Si dispersoids andβ″precipitates was tuned to enhance the strength−ductility synergy of air-cooled Al−Mg−Si alloys.Scanning electron microscopy(SEM)and transmission electron microscopy(TEM)were employed to elucidate the microstructural parameters of these two strengthening phases.The results show that the microstructural heterogeneity can be triggered by the absence of homogenization,resulting in the presence of dispersoid-free zones(DFZs)and dispersoid zones(DZs),in conjunction with bimodalβ″precipitates.Further analytical calculations,from the strengthening model,clarify that the strategically dispersedα-Al(Fe,Mn)Si andβ″particles create“soft”and“hard”domains within the alloy,resultantly improving the mechanical properties.
文摘Light-driven CO_(2) reduction reaction(CO_(2)RR)to value-added ethylene(C2H4)holds significant promise for addressing energy and environmental challenges.While the high energy barriers for*CO intermediates hydrogenation and C–C coupling limit the C_(2)H_(4)generation.Herein,CuxP/g-C_(3)N_(4) heterojunction prepared by an in-situ phosphating technique,achieved collaborative photocatalytic CO_(2) and H2O,producing CO and C_(2)H_(4)as the main products.Notably,the selectivity of C_(2)H_(4)produced by CuxP/g-C_(3)N_(4) attained to 64.25%,which was 9.85 times that of CuxP(6.52%).Detailed time-resolution photoluminescence spectra,femtosecond transient absorption spectroscopy tests and density functional theory(DFT)calculation validate the ultra-fast interfacial electron transfer mechanism in CuxP/g-C_(3)N_(4) heterojunction.Successive*H on P sites caused by adsorbed H2O splitting with moderate hydrogenation ability enables the multi-step hydrogenation during CO_(2)RR process over CuxP/g-C_(3)N_(4).With the aid of mediated asymmetric Cu and P dual sites by g-C_(3)N_(4) nanosheet,the produced*CHO shows an energetically favorable for C–C coupling.The coupling formed*CHOCHO further accepts photoexcited efficient e–and*H to deeply produce C_(2)H_(4)according to the C^(2+)intermediates,which has been detected by in-situ diffuse reflectance infrared Fourier transform spectroscopy and interpreted by DFT calculation.The novel insight mechanism offers an essential understanding for the development of CuxP-based heterojunctions for photocatalytic CO_(2) to C^(2+)value-added fuels.
基金the National Key Research and Development Program of China(no.2021YFA1600800 and 2021YFA1501000)the Fundamental Research Funds for the Central Universities(YCJJ20242227)+3 种基金the Research Plan of International Collaboration Fund for Creative Research Teams(ICFCRT)of NSFC(No.W2441008)the open research fund of Suzhou Laboratory(No.SZLAB-1308-2024-ZD010)the Innovation and Talent Recruitment Base of New Energy Chemistry and Devices(B21003)supported by the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement(Grant No.101102946 and Grant No.945422).
文摘Rechargeable metal-air batteries have gained significant interest due to their high energy density and environmental benignity.However,these batteries face significant challenges,particularly related to the air-breathing electrode,resulting in poor cycle life,low efficiency,and catalyst degradation.Developing a robust bifunctional electrocatalyst remains difficult,as oxygen electrocatalysis involves sluggish kinetics and follows different reaction pathways,often requiring distinct active sites.Consequently,the poorly understood mechanisms and irreversible surface reconstruction in the catalyst’s microenvironment,such as atomic modulation,nano-/microscale,and surface interfaces,lead to accelerated degradation during charge and discharge cycles.Overcoming these barriers requires advancements in the development and understanding of bifunctional electrocatalysts.In this review,the critical components of metal-air batteries,the associated challenges,and the current engineering approaches to address these issues are discussed.Additionally,the mechanisms of oxygen electrocatalysis on the air electrodes are examined,along with insights into how chemical characteristics of materials influence these mechanisms.Furthermore,recent advances in bifunctional electrocatalysts are highlighted,with an emphasis on the synthesis strategies,microenvironmental modulations,and stabilized systems demonstrating efficient performance,particularly zinc-and lithium-air batteries.Finally,perspectives and future research directions are provided for designing efficient and durable bifunctional electrocatalysts for metal-air batteries.
