The growing global energy demand and environmental concerns like greenhouse gas emissions call for clean energy solutions.Hydrogen energy,with high caloric value and low environmental impact,is a promising alternative...The growing global energy demand and environmental concerns like greenhouse gas emissions call for clean energy solutions.Hydrogen energy,with high caloric value and low environmental impact,is a promising alternative,especially when produced via proton exchange membrane water electrolysis(PEMWE).This process relies on the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),both requiring efficient electrocatalysts.Platinum(Pt),the most effectiveHER catalyst,is limited by high cost and scarcity,prompting research into Pt alternatives like ruthenium-based,transition metal derivatives,and metal-free catalysts that balance cost,efficiency,and stability.This review explores HER mechanisms,Pt-free catalyst innovations,and the impact of structural and interfacial electrode optimization on performance of HER in acidic media.It also examines electrochemical evaluation techniques,material characterization,and the role ofmachine learning in catalyst design.By providing a framework for Pt-free HER catalyst development,this review supports advancements in efficient and sustainable hydrogen energy technologies.展开更多
The COVID-19 pandemic has exposed the limitations of traditional preventative measures and underscored the essential role of face masks in controlling virus transmission.More effective and recyclable facial masks usin...The COVID-19 pandemic has exposed the limitations of traditional preventative measures and underscored the essential role of face masks in controlling virus transmission.More effective and recyclable facial masks using various materials have been developed.In this work,vertically aligned carbon nanotubes(VACNTs)are employed as effective facial mask filters,particularly aimed at preventing SARS-CoV-2 virus infection in preparation for future COVID-19 pandemics.This study assesses six critical aspects of facial masks:hydrophobicity,industrial viability,breathability,hyperthermal antiviral effect,toxicity,and reusability.The VACNT alone exhibits superhydrophobicity with a contact angle of 175.53◦,and an average of 142.7◦for a large area on spun-bonded polypropylene.VACNTs are processed using a roll-to-roll method,eliminating the need for adhesives.Due to the aligned tubes,VACNT filters demonstrate exceptional breathability and moisture ventilation compared to previously reported CNT and conventional filters.Hyperthermal tests of VACNT filters under sunlight confirm that up to 99.8%of the HCoV 229E virus denatures even in cold environments.The safety of using VACNTs is corroborated through histopathological evaluation and subcutaneous implantation tests,addressing concerns of respiratory and skin inflammation.VACNT masks efficiently transmit moisture and rapidly return to their initial dry state under sunlight maintaining their properties after 10000 bending cycles.In addition,the unique capability of VACNT filters to function as respiratory sensors,signaling dampness and facilitating reuse,is assessed,alongside their Joule heating effect.展开更多
The synergistic effect of bi-component support catalysts via facile synthesis remains a pivotal challenge in catalysis,particularly under mild conditions.Therefore,this study reports an ultrasonication-plasma strategy...The synergistic effect of bi-component support catalysts via facile synthesis remains a pivotal challenge in catalysis,particularly under mild conditions.Therefore,this study reports an ultrasonication-plasma strategy to produce a PtGaPCoCoO@TiO_(x)site catalyst encapsulated within a high-entropy alloy framework.This approach harnesses instantaneous high-temperature plasma generated using an electrical field and ultrasonication under ambient conditions in H_(2)O.This study also elucidates the origin of the bifunctional effect in high-loading,ultra-stable,and ultra-fine PtGaPCoCoO catalysts,which are coated with a reducible TiO_(x)layer,thereby achieving optimal catalytic activity and hydrogen evolution reaction(HER)performance.PtGaPCo intimacy in PtGaPCoCoO@TiO_(x)is tuned and distributed on the porous titania coating based on strong metal-support interactions by leveraging the instantaneous high-energy input from plasma discharge and ultrasonication under ambient conditions in H_(2)O.PtGaPCoCoO@TiO_(x)exhibits remarkable selectivity and durability in the hydrogenation of 3-nitrophenylacetylene,even after 25 cycles with high conversion rates,significantly outperforming comparative catalysts lacking the ultrasonication plasma treatment and other reported catalysts.Furthermore,the catalyst exhibits exceptional HER activity,demonstrated by an overpotential of 187 mV at a current density of 10 mA cm^(-2)and a Tafel slope of 152 mV dec-1.This enhancement can be attributed to an increased electron density on the Pt surface within the PtGaPCo alloy.These findings highlight the potential of achieving synergistic chemical interactions among active metal sites in stable,industry-applicable catalysts.展开更多
For the first time,a printable,miniaturized,and gate-controlled electrochemical capacitor-diode(G-CAPode)is presented.The heart of the device consists of a recently developed asymmetric electrical double-layer capacit...For the first time,a printable,miniaturized,and gate-controlled electrochemical capacitor-diode(G-CAPode)is presented.The heart of the device consists of a recently developed asymmetric electrical double-layer capacitor system based on selective,sizedependent ion adsorption.Due to the introduction of a sieving carbon with ultramicroporous pores(d=0.69 nm)as one electrode material,an effective blocking of ions with sizes below the pore size of the carbon can be achieved,leading to a unidirectional charging comparable to a diode(CAPode).This“working capacitor”(W-Cap)was further expanded by introducing a third(“gate”)electrode enabling a control of the current and voltage output of the W-Cap depending on the applied gate bias between the gate electrode and counter electrode of the W-Cap resembling transistor features.By varying the gate bias voltage,the potentials and therefore the working window of theW-Cap electrodes are shifted to more positive or negative potentials,leading to an increase or decrease of the G-CAPode capacitance.The printed G-CAPode was tested as a switchable device analogous to an I-MOS varactor for the adjustable filtering ofACsignals in a high-pass filter and band-pass filter application.This investigation opens the possibility to couple capacitive(energy storage),diodic(current rectification),and transistor(voltage-controlled switching)characteristics in one device and also addresses its process integration via 3D printing.展开更多
Anode-free sodium batteries(AFSBs)have attracted increasing attention for their high energy density.However,they suffer from rapid capacity decline resulting from sodium dendrite growth at the sodium/host interface an...Anode-free sodium batteries(AFSBs)have attracted increasing attention for their high energy density.However,they suffer from rapid capacity decline resulting from sodium dendrite growth at the sodium/host interface and irreversible side reactions at the electrolyte/sodium interface.Herein,a GaInSn-coated Cu foil(G-Cu),prepared by a simple brush coating method,was applied as the sodiophilic current collector to regulate sodium nucleation behavior.In addition,a nonexpendable functional electrolyte additive,hexamethyldisiloxane(HMDSO),was introduced,which could be absorbed on the sodium surface and serve as a protective layer against corrosion side reactions at the electrolyte/sodium interface.It is interesting to note that this additive barely participated in forming the solid electrolyte interphase.The synergetic effects of sodiophilic interface design and electrolyte regulation enable reversible sodium plating and stripping.Ultimately,the AFSB assembled using G-Cu and HMDSO electrolyte with a highly loaded Na_(3)V_(2)(PO_(4))_(3) cathode(≈12.5 mg cm^(−2))delivers a discharge capacity of 84.5 mAh g^(−1) after 200 cycles with a high capacity retention of 87.6%,significantly extending its operation lifespan.展开更多
Conductive gels are utilized as wearable sensors in flexible electronic materials due to their human skin-like adaptability.However,achieving high strength,durability,and sustainability simultaneously remains a challe...Conductive gels are utilized as wearable sensors in flexible electronic materials due to their human skin-like adaptability.However,achieving high strength,durability,and sustainability simultaneously remains a challenge.In this study,a tough,durable,recyclable,green,and multifunctional semi-interpenetrating network organohydrogel was developed and enhanced by lignin@polypyrrole core-shell nanoparticles(LP9).The semi-interpenetrating network organohydrogel was constructed using environmentally friendly poly(vinyl alcohol)and bio-based gelatin.The LP9 was synthesized via in-situ polymerization of pyrrole on lignin nanoparticles,serving as rigid anchors to enhance the gel’s properties and eliminate heterogeneity through hydrogen bonding.With 5%of LP9,the organohydrogel(5LP9)demonstrated a tensile strength of 2.5MPa,elongation of 700%,conductivity of 432 mS/m,and a gauge factor of 1.7 with a good linearity,highlighting its excellent performance as an electronic conductive material.In addition,the organohydrogel exhibited remarkable environmental stability,antimicrobial properties,recyclability,and biocompatibility.When applied to human motion detection,voice recognition,and gesture recognition,the organohydrogel showcased excellent recognition ability,responsive functionality,and long-term monitoring stability.These findings provide a theoretical foundation for developing green and programmable wearable sensors for human-machine interaction,incorporating deep learning such as letter-writing recognition.展开更多
Metal organic frameworks(MOFs)have a promising perspective as oxygen evolution reaction(OER)electrocatalysts due to their high surface areas and tunable structures.However,one of the main challenges for their further ...Metal organic frameworks(MOFs)have a promising perspective as oxygen evolution reaction(OER)electrocatalysts due to their high surface areas and tunable structures.However,one of the main challenges for their further application is inferior stability during alkaline OER.Herein,operando x-ray absorption spectroscopy and operando x-ray diffraction of NiCo-MOF-74 materials unveil their electrochemical transformations differentiating between electrolyte-induced,beam-induced,and electrochemically induced changes of the electronic state and local structure around the transition metal centers in addition to their overall crystal structure.An inferior electrolyte-and beam stability of Co-MOF-74 is revealed in comparison to a more stable performance of Ni-MOF-74 and Ni0.25Co0.75-MOF-74.Based on the operando measurement results,good experimental practices for future MOF OER electrocatalyst studies are presented.展开更多
Artificial intelligence(AI)is revolutionizing sustainable materials science,yet a comprehensive and timely evaluation of the rapidly evolving AI techniques applied across the entire materials lifecycle remains lacking...Artificial intelligence(AI)is revolutionizing sustainable materials science,yet a comprehensive and timely evaluation of the rapidly evolving AI techniques applied across the entire materials lifecycle remains lacking.Thiswork reviews AI-driven advances in sustainable materials,specifically focusing on battery materials,thermal management materials,energy conversion materials,and catalysts.The key patterns,capabilities,and limitations of AI are identified across three interconnected phases:sustainable materials design(leveraging predictive and generative models for accelerated discovery),green processing(integrating adaptive synthesis optimization and autonomous experimentation),and extending to lifecycle management(encompassing real-time monitoring,predictive maintenance,and intelligent recycling).Then,the persistent challenges,including data sparsity,domainspecific knowledge integration,and limited model generalizability,are investigated,followed by an exploration of emerging solutions such as federated learning for privacy-preserving data sharing,physics-informed neural networks for knowledge integration,and multimodal AI for cross-modal knowledge transfer.Finally,the computational sustainability challenges of AI methods themselves are also discussed.This review highlights key bottlenecks impeding scalable adoption and discuss pathways for realizing the full potential of AI in sustainable materials development.展开更多
Polymer-derived SiOC materials are widely regarded as a new generation of anodes owing to their high specific capacity,low discharge platform,tunable chemical/structural composition,and good structural stability.Howev...Polymer-derived SiOC materials are widely regarded as a new generation of anodes owing to their high specific capacity,low discharge platform,tunable chemical/structural composition,and good structural stability.However,tailoring the structure of SiOC to improve its electrochemical performance while simultaneously achieving elemental doping remains a challenge.Besides,the lithium storage mechanism and the structural evolution process of SiOC are still not fully understood due to its complex structure.In this study,a hollow porous SiOCN(Hp-SiOCN)featuring abundant oxygen defects is successfully prepared,achieving both the creation of a hollow porous structure and nitrogen element doping in one step,finally enhancing the structural stability and improving the lithium storage kinetics of Hp-SiOCN.In addition,the formation of a fully reversible structural unit,SiO3C─N,through the chemical interaction between N and Si/C,showcases a strong lithium adsorption capacity.Taking advantage of these combined benefits,the as-prepared Hp-SiOCN electrode delivers a reversible specific capacity of 412 mAh g^(−1)(93%capacity retention)after 500 cycles at 1.0 A g^(−1) and exhibited only 4%electrode expansion.This work offers valuable mechanistic insights into the synergistic optimization of elemental doping and structural design in SiOC,paving the way for advanced developments in battery technology.展开更多
Sandwiched composites with a combination of electromagnetic interference(EMI)shielding performance,thermal conductivity,and electrical insulation show significant potential in electronic packaging.However,the fabricat...Sandwiched composites with a combination of electromagnetic interference(EMI)shielding performance,thermal conductivity,and electrical insulation show significant potential in electronic packaging.However,the fabrication of such composites using high-performance thermosets as matrices presents challenges due to their permanently crosslinked structures.Here,we relied on the dynamic covalent chemistry to propose an innovative interface-welding strategy to fabricate a sandwiched thermoset(covalent adaptable network)/carbon nanotubes/boron nitride(CAN/CNTs/BN)composite.To sustainability,theCANmatrixwas derived fromrenewable biobased resources,such as vanillin,glycerol triglycidyl ether,and 1,10-diaminodecane.The incorporation of CAN/BN composites as the outer layers bolstered thermal conductivity while maintaining electrical insulation,while the CAN/CNTs interlayer efficiently attenuated electromagnetic waves.With a BN and CNT content of 30 wt%,the CAN/CNTs/BN composite achieved a thermal conductivity of 1.79W⋅m^(−1)⋅K^(−1),an EMI shielding effectiveness exceeding 55 dB in the X-band,and an ultra-low electrical conductivity of 1.6×10^(−13)S⋅m^(−1).Leveraging dynamic covalent chemistry,the interface-welding technique fostered fully integrated interfaces,ensuring superior mechanical properties of CAN/CNTs/BN composite including a tensile modulus of 3837.8±196.9 MPa and tensile strength of 62.1±3.7 MPa.Additionally,its exceptional heat dissipation performance positions CAN/CNTs/BN composite as a promising contender for electronic packaging applications.展开更多
Low-ionic conductivity within high-loading cathode has greatly limited the application of solid polymer electrolytes in rechargeable batteries.Herein,solid polymer electrolyte with a three-dimensionally conducting net...Low-ionic conductivity within high-loading cathode has greatly limited the application of solid polymer electrolytes in rechargeable batteries.Herein,solid polymer electrolyte with a three-dimensionally conducting network is obtained by in situ polymerization of vinyl ethylene carbonate(VEC)with the aid of dipentaerythritol hexaacrylate(DPHA)crosslinker in the solidstate lithium(Li)metal batteries(LMBs).The weak coordination of Li^(+)with C═O and C─O groups promotes the dissociation and transport of Li^(+).The obtained P(VEC–DPHA)electrolyte enables a fast and orderly Li^(+)transport path and hinders the transport of TFSI^(-),rendering a remarkable ionic conductivity(2.53×10^(-4)S cm^(-1)),high Li+transference number(0.47),and wide electrochemical window(5.1 V).A total of 87.38%capacity retention rate of LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)||Li is achieved after 200 cycles at 0.2 C.P(VEC–DPHA)can also provide stable cycles under harsh conditions of high rate(1 C),high-cathode loading(10.83 mg cm^(-2)),and high-energy-density pouch cell(421.8Wh kg^(-1),cathode loading of 25 mg cm^(-2)).This work provides novel insights for the design of highly conductive polymer electrolytes and high-energy-density LMBs.展开更多
MXenes,a family of emerging two-dimensional materials offer enriched surface chemistry,high electrical conductivities,large specific surface area,intrinsic physicochemical properties,and excellent mechanical stability...MXenes,a family of emerging two-dimensional materials offer enriched surface chemistry,high electrical conductivities,large specific surface area,intrinsic physicochemical properties,and excellent mechanical stability.However,restacking of MXene sheets limit their electrochemical performance.To overcome this limitation,recent advancements have focused on developing MXene composites with metal phosphates/phosphides(MXene/MPs).This review discusses the applications of MXene/MPs composites in energy storage and conversion applications.The incorporation ofMPs intoMXenes not only addresses the restacking issue and aggregation problems,but also enhances the overall electrochemical performance of energy storage and conversion systems.The review concludes with a summary of the current research status and future prospects for MXene/MPs-based composites in energy applications.展开更多
Constructing an interlayer between perovskite and zinc oxide(ZnO)electron transporting layer to passivate the implacable interfacial defects for upgrading the efficiency and stability of flexible perovskite solar cell...Constructing an interlayer between perovskite and zinc oxide(ZnO)electron transporting layer to passivate the implacable interfacial defects for upgrading the efficiency and stability of flexible perovskite solar cells(f-PSC)is a daunting challenge and remains under explored.Herein,we present a cascade bridge interlayer strategy of zeolitic imidazole framework-8(ZIF-8)at the ZnO/perovskite interface.The ZIF-8 interlayer uplifts thework function,creating a cascade pathway and bridges through nitrogen bonding with Pb^(2+)ions of perovskite,thereby facilitating electron transport and reducing interfacial charge recombination.Consequently,the ZnO surface defects are passivated by alleviating the OH‒species,and thus the device stability is significantly improved.The f-PSC with ZIF-8 interlayer delivers a stable conversion efficiency of 17.10%with minimal hysteresis.By utilizing the piezo-phototronic effect and subjecting the f-PSC to a tensile strain of 1.6%,a stable efficiency of 18.47%was achieved,representing one of the highest reported efficiencies for ZnO nanorods-based f-PSC.Furthermore,the ZnO‒ZIF-8 exhibits high adsorption capacity toward lead and traps the mobile Pb^(2+)ions at the ZnO/perovskite interface,preventing the negative impact of lead leaching on environmental sustainability.展开更多
While sodium metal batteries(SMBs)possess remarkable superiority for next-generation energy storage systems,interfacial reactions,and dendrite growth due to the dissolution of solid electrolyte interphase(SEI)have ser...While sodium metal batteries(SMBs)possess remarkable superiority for next-generation energy storage systems,interfacial reactions,and dendrite growth due to the dissolution of solid electrolyte interphase(SEI)have seriously hindered the large-scale application of SMBs,especially at high temperatures.Here,a vinyl ethylene carbonate-based quasi-solid electrolyte(PVEC-QSPE)capable of enhancing the high-temperature stability of Na anodes is successfully synthesized by in situ curing of oligomeric poly(vinyl ethylene carbonate)(PVEC).The increased steric hindrance of PVEC reduces the coordination ability of C=O toward Na+,which promotes the cooperative migration of Na+with anions and the decomposition of anions to form the SEI.Furthermore,PVEC-QSPE significantly reduces the dissolution of SEI,which contains more organic components and fewer inorganic components,thereby minimizing the release of gases including CO_(2) and inhibiting the growth of sodium dendrites.The stable interface between PVEC-QSPE and Na helps Na|PVEC-QSPE|Na_(3)V_(2)(PO_(4))_(3)(NVP)batteries to operate stably at high temperatures,whose capacity retention rate reaches 80%at 80◦C and 93.3%at 60℃ after 3000 cycles employing high rate of 10 C.This work provides an efficient strategy to solve the problems of unstable SEI and dendrite growth,thereby promoting the development of safe and practical SMBs.展开更多
All-polymer solar cells(all-PSCs)are of interest owing to their unique advantages,including remarkably improved device stability and exceptional mechanical stretchability.Over recent years,there has been a notable inc...All-polymer solar cells(all-PSCs)are of interest owing to their unique advantages,including remarkably improved device stability and exceptional mechanical stretchability.Over recent years,there has been a notable increase in the power conversion efficiency(PCE)of all-PSCs,largely attributed to advancements in the morphology control of the active layer.Notably,the domain size is of paramount importance as it impacts critical factors such as exciton dissociation,charge transport,and collection.However,the low glass transition temperature of conjugated polymers,coupled with a minimal change in mixing entropy,often results in an excessive degree of phase separation.Consequently,it is essential to comprehend the evolution of phase separation and develop strategies to regulate the domain size.In this review,we elucidate the key parameters that contribute to the enhancement of phase separation and present qualitative and quantitative characterization techniques for domain size.Building on this foundation,we introduce the strategies and principles for regulating domain sizes,encompassing factors such as crystallinity,miscibility,and molecular conformation from a thermodynamic perspective,as well as the film-forming kinetics and the crystallization sequence from a kinetic perspective.Lastly,we offer insights into the current challenges and potential future prospects for the evolution of all-PSCs.展开更多
The internal electric field(IEF)is key in speeding up the separation and transfer of photogenerated carriers,which boosts the production of reactive oxygen species(ROS).In this study,we present a novel silver iodide/N...The internal electric field(IEF)is key in speeding up the separation and transfer of photogenerated carriers,which boosts the production of reactive oxygen species(ROS).In this study,we present a novel silver iodide/N-rich carbon nitride(AgI/C_(3)N_(5))heterojunction catalyst with an IEF directed from AgI to C_(3)N_(5).We confirmed this IEF using density functional theory(DFT)calculations and various characterization methods.This IEF induces and reinforces the Type II transfer pathway for carrier separation and transfer,significantly increasing the production of ROS,particularly singlet oxygen(1O_(2)).As a result,the AgI/C_(3)N_(5)catalysts achieve 10.1 times the disinfection efficiency of C_(3)N_(5)and 5.6 times that of AgI,under one-min reaction time,107 CFU/mL of E.coli,visible light,and room temperature.It also outperforms most other AgI and carbon nitride-based heterojunction photocatalysts.Notably,the photogenerated holes(h+)selectively oxidize superoxide radicals(·O_(2)^(-))to 1O_(2)due to favorable energy alignment,minimizing O_(2)reduction effects and enhancing photocorrosion resistance,as demonstrated in five consecutive cycling experiments.In addition,the actual water disinfection tests confirmed its practical application potential.This work highlights the AgI/C_(3)N_(5)heterojunction catalyst’s promise as an efficient disinfection agent and sheds light on the photocatalytic disinfection mechanism.展开更多
Understanding and regulating the electronic states of single-atom sites near the Fermi energy level are essential for developing effective electrocatalysts for lithium–oxygen batteries(LOBs).In this study,we introduc...Understanding and regulating the electronic states of single-atom sites near the Fermi energy level are essential for developing effective electrocatalysts for lithium–oxygen batteries(LOBs).In this study,we introduce an axial oxygen ligand at the metal center of cobalt porphyrin(CoPP)to adjust the electronic state of the Co center.Theoretical calculations and experimental findings show that this axial interaction disrupts the planar tetragonal crystal field of CoPP,resulting in enhanced spin polarization and electronic rearrangement.This rearrangement of d orbitals causes an upward shift in the frontier orbitals,which facilitates electron exchange during reactions.Additionally,the increased number of unpaired electrons in the d orbitals enhances the adsorption of CoPPO-MXene to various oxygen species,promoting the formation of a thin film-like Li2O2.These thin film-like discharge products improve contact with the electrode surfaces,leading to easier decomposition during the charging process.Consequently,CoPP-OMXene-based LOBs demonstrate a high discharge capacity of 11035mAh g−1,a low overpotential of 0.76 V,and remarkable cycling stability(445 cycles).展开更多
Recent advancements in lithium-oxygen(Li-O_(2))batteries have focused on incorporating redox mediators(RMs)into the electrolyte to address challenges of low energy efficiency and poor cycle life.However,various solubl...Recent advancements in lithium-oxygen(Li-O_(2))batteries have focused on incorporating redox mediators(RMs)into the electrolyte to address challenges of low energy efficiency and poor cycle life.However,various soluble RMs induce parasitic reactions with Li,compromising the anode stability.In this study,we design optimized Li-O_(2)batteries by introducing ZnI_(2)into the electrolyte,which serves a dual function:facilitating a stable LiZn/Zn protective layer on the Li metal anode and acting as an effective RM.The in situ formed LiZn/Zn layer prevents I_(3)^(-)shuttle effects,stabilizing the Li anode and promoting uniform Li plating and stripping.Additionally,the ZnI_(2)mediator facilitates rapid conversion of the I^(-)/I_(3)^(-)and I_(3)-/I_(2)redox couples at the cathode,contributing to amore reversible and lower overpotential Li_(2)O_(2)cycle.Notably,ZnI_(2)enhances early-stage LiO_(2)formation,verified by in situ Raman spectroscopy,which supports uniform sheet-like Li_(2)O_(2)deposition and contributes to stable cycling.These synergistic effects caused a significant reduction in the charge potential to less than 3.4 V,enabling over 800 stable cycles.This approach provides a viable pathway to achieving high energy density and long cycle life in Li-O_(2)batteries,positioning them for practical applications.展开更多
Inorganic lead halide perovskites,especially CsPbI3,have witnessed significant progress in photovoltaic field due to their outstanding optoelectronic properties and high thermal stability.However,high-performance inor...Inorganic lead halide perovskites,especially CsPbI3,have witnessed significant progress in photovoltaic field due to their outstanding optoelectronic properties and high thermal stability.However,high-performance inorganic perovskite solar cells(IPSCs)are generally realized by strictly controlling the environmental humidity(mostly lower than 40%)during fabrication,which is undesirable for reducing fabrication cost and promoting further industrial production.Herein,a synergistic in situ hydrolysis polymerization strategy through 3,3,3-(trifluoropropyl)trichlorosilane(TFCS)and(3-2-aminoethylamino)propyltrimethoxysilane(AEMS)treatment is reported to prevent water invasion and realize efficient CsPbI3 IPSCs in highly humid air.TFCS not only regulates the crystallization process via hydrolysis reaction,but also stabilizes the phase structure by passivating the defects and producing a hydrophobic protection layer.Additionally,TFCS facilitates in situ polymerization of upper layer AEMS,thus promoting further enhanced protection of perovskites against ambient moisture.As a result,the CsPbI3 IPSCs fabricated at 45%humidity exhibit a dramatically improved efficiency of 20.09%,representing a record value for the inverted IPSCs fabricated in air with humidity over 40%.Moreover,the environmental humidity window for device fabrication can be broadened to 60%.This work provides an effective approach to stabilizing air-processedCsPbI3 and favoring the practical industrialmanufacture to further boost their cost-effective applications.展开更多
Semiconducting phase is extremely rare and difficult to be realized in two-dimensional(2D)aluminum borides.Here,we for the first time report the discovery of a rarely semiconducting allotrope(labeled as AlB4-1)in 2D A...Semiconducting phase is extremely rare and difficult to be realized in two-dimensional(2D)aluminum borides.Here,we for the first time report the discovery of a rarely semiconducting allotrope(labeled as AlB4-1)in 2D AlB4 nanosheets.This semiconductor is the global minimum structure in 2D space with two layers stacked together connected by strong Al-B bonds.Systematic studies demonstrate the high thermodynamic,lattice dynamic,thermal,and mechanical stabilities of AlB4-1.More importantly,this semiconducting AlB4-1 shows fascinating properties and promising applications,such as,the optimal band gap(1.156 eV at HSE06 level),high carrier mobility(up to 3.14×103 cm2V−1s−1),substantially high solar energy conversion efficiency(21.9%)and large optical response(106 cm−1)in the visible region.Extensive studies indiate that h-BN can serve as an effective substrate to support and encapsulate AlB4-1 with minimal impact on the electronic properties of AlB4-1,laying the foundation for the real application of AlB4-1 in electronic devices.Besides this semiconducting phase,other low-lying allotropes(AlB4-2 to-11)also display high stabilities,exotic properties and diverse applications.For example,the metallic AlB4-4 shows Dirac cone near Fermi level and superconductivity with TC as high as 23.4K,which can be substantially enhanced to 34.1K at tensile strain of 11%.These allotropes with different shapes show diverse hypercoordinate motifs with unusual bonding patterns.Comprehensive studies demonstrate that 2D AlB4 nanosheets is a class of highly stable,multifunctional nanomaterials for diverse applications in electronics,optics,optoelectronics,nanodevices,solar energy conversion,superconductivity,nanomechanics,and so on.The present study will provide useful guidance in fabricating these interesting nanostructures and stimulate both experimental and computational efforts in this direction.展开更多
基金supported by the Resources Technology and Critical Minerals Trailblazer and the Commonwealth Government through the Trailblazer Universities Program as well as the Higher Degree by Research(HDR 2024)Scholarship by Curtin University,Perth,Australia.
文摘The growing global energy demand and environmental concerns like greenhouse gas emissions call for clean energy solutions.Hydrogen energy,with high caloric value and low environmental impact,is a promising alternative,especially when produced via proton exchange membrane water electrolysis(PEMWE).This process relies on the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),both requiring efficient electrocatalysts.Platinum(Pt),the most effectiveHER catalyst,is limited by high cost and scarcity,prompting research into Pt alternatives like ruthenium-based,transition metal derivatives,and metal-free catalysts that balance cost,efficiency,and stability.This review explores HER mechanisms,Pt-free catalyst innovations,and the impact of structural and interfacial electrode optimization on performance of HER in acidic media.It also examines electrochemical evaluation techniques,material characterization,and the role ofmachine learning in catalyst design.By providing a framework for Pt-free HER catalyst development,this review supports advancements in efficient and sustainable hydrogen energy technologies.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.2021R1A2C1004131 and RS-2024-00406152)supported by the Institute of Information&Communications Technology Planning&Evaluation(IITP)-ITRC(Information Technology Research Center)grant funded by the Korea government(MSIT)(IITP-2025-RS-2023-00258971,20%,and RS-2023-00228994).
文摘The COVID-19 pandemic has exposed the limitations of traditional preventative measures and underscored the essential role of face masks in controlling virus transmission.More effective and recyclable facial masks using various materials have been developed.In this work,vertically aligned carbon nanotubes(VACNTs)are employed as effective facial mask filters,particularly aimed at preventing SARS-CoV-2 virus infection in preparation for future COVID-19 pandemics.This study assesses six critical aspects of facial masks:hydrophobicity,industrial viability,breathability,hyperthermal antiviral effect,toxicity,and reusability.The VACNT alone exhibits superhydrophobicity with a contact angle of 175.53◦,and an average of 142.7◦for a large area on spun-bonded polypropylene.VACNTs are processed using a roll-to-roll method,eliminating the need for adhesives.Due to the aligned tubes,VACNT filters demonstrate exceptional breathability and moisture ventilation compared to previously reported CNT and conventional filters.Hyperthermal tests of VACNT filters under sunlight confirm that up to 99.8%of the HCoV 229E virus denatures even in cold environments.The safety of using VACNTs is corroborated through histopathological evaluation and subcutaneous implantation tests,addressing concerns of respiratory and skin inflammation.VACNT masks efficiently transmit moisture and rapidly return to their initial dry state under sunlight maintaining their properties after 10000 bending cycles.In addition,the unique capability of VACNT filters to function as respiratory sensors,signaling dampness and facilitating reuse,is assessed,alongside their Joule heating effect.
基金supported by two Mid-Level Researcher National Projects of the National Research Foundation(NRF)funded by the Ministry of Science and ICT,Republic of Korea(NRF-2022R1A2C1004392).
文摘The synergistic effect of bi-component support catalysts via facile synthesis remains a pivotal challenge in catalysis,particularly under mild conditions.Therefore,this study reports an ultrasonication-plasma strategy to produce a PtGaPCoCoO@TiO_(x)site catalyst encapsulated within a high-entropy alloy framework.This approach harnesses instantaneous high-temperature plasma generated using an electrical field and ultrasonication under ambient conditions in H_(2)O.This study also elucidates the origin of the bifunctional effect in high-loading,ultra-stable,and ultra-fine PtGaPCoCoO catalysts,which are coated with a reducible TiO_(x)layer,thereby achieving optimal catalytic activity and hydrogen evolution reaction(HER)performance.PtGaPCo intimacy in PtGaPCoCoO@TiO_(x)is tuned and distributed on the porous titania coating based on strong metal-support interactions by leveraging the instantaneous high-energy input from plasma discharge and ultrasonication under ambient conditions in H_(2)O.PtGaPCoCoO@TiO_(x)exhibits remarkable selectivity and durability in the hydrogenation of 3-nitrophenylacetylene,even after 25 cycles with high conversion rates,significantly outperforming comparative catalysts lacking the ultrasonication plasma treatment and other reported catalysts.Furthermore,the catalyst exhibits exceptional HER activity,demonstrated by an overpotential of 187 mV at a current density of 10 mA cm^(-2)and a Tafel slope of 152 mV dec-1.This enhancement can be attributed to an increased electron density on the Pt surface within the PtGaPCo alloy.These findings highlight the potential of achieving synergistic chemical interactions among active metal sites in stable,industry-applicable catalysts.
基金from the European Union’s Horizon 2020 Research and Innovation Programme(Grant Agreement No.101054940).
文摘For the first time,a printable,miniaturized,and gate-controlled electrochemical capacitor-diode(G-CAPode)is presented.The heart of the device consists of a recently developed asymmetric electrical double-layer capacitor system based on selective,sizedependent ion adsorption.Due to the introduction of a sieving carbon with ultramicroporous pores(d=0.69 nm)as one electrode material,an effective blocking of ions with sizes below the pore size of the carbon can be achieved,leading to a unidirectional charging comparable to a diode(CAPode).This“working capacitor”(W-Cap)was further expanded by introducing a third(“gate”)electrode enabling a control of the current and voltage output of the W-Cap depending on the applied gate bias between the gate electrode and counter electrode of the W-Cap resembling transistor features.By varying the gate bias voltage,the potentials and therefore the working window of theW-Cap electrodes are shifted to more positive or negative potentials,leading to an increase or decrease of the G-CAPode capacitance.The printed G-CAPode was tested as a switchable device analogous to an I-MOS varactor for the adjustable filtering ofACsignals in a high-pass filter and band-pass filter application.This investigation opens the possibility to couple capacitive(energy storage),diodic(current rectification),and transistor(voltage-controlled switching)characteristics in one device and also addresses its process integration via 3D printing.
基金financially supported by the National Natural Science Foundation of China(No.22279164)the Hunan Provincial Science and Technology Plan Projects of China(No.2022RC3050 and No.2017TP1001)the cooperation project from Guangdong DFP New Material Group Co.Ltd.
文摘Anode-free sodium batteries(AFSBs)have attracted increasing attention for their high energy density.However,they suffer from rapid capacity decline resulting from sodium dendrite growth at the sodium/host interface and irreversible side reactions at the electrolyte/sodium interface.Herein,a GaInSn-coated Cu foil(G-Cu),prepared by a simple brush coating method,was applied as the sodiophilic current collector to regulate sodium nucleation behavior.In addition,a nonexpendable functional electrolyte additive,hexamethyldisiloxane(HMDSO),was introduced,which could be absorbed on the sodium surface and serve as a protective layer against corrosion side reactions at the electrolyte/sodium interface.It is interesting to note that this additive barely participated in forming the solid electrolyte interphase.The synergetic effects of sodiophilic interface design and electrolyte regulation enable reversible sodium plating and stripping.Ultimately,the AFSB assembled using G-Cu and HMDSO electrolyte with a highly loaded Na_(3)V_(2)(PO_(4))_(3) cathode(≈12.5 mg cm^(−2))delivers a discharge capacity of 84.5 mAh g^(−1) after 200 cycles with a high capacity retention of 87.6%,significantly extending its operation lifespan.
基金financially supported by the Fundamental Research Funds for the National Natural Science Foundation of China(Project No.U23A20692).
文摘Conductive gels are utilized as wearable sensors in flexible electronic materials due to their human skin-like adaptability.However,achieving high strength,durability,and sustainability simultaneously remains a challenge.In this study,a tough,durable,recyclable,green,and multifunctional semi-interpenetrating network organohydrogel was developed and enhanced by lignin@polypyrrole core-shell nanoparticles(LP9).The semi-interpenetrating network organohydrogel was constructed using environmentally friendly poly(vinyl alcohol)and bio-based gelatin.The LP9 was synthesized via in-situ polymerization of pyrrole on lignin nanoparticles,serving as rigid anchors to enhance the gel’s properties and eliminate heterogeneity through hydrogen bonding.With 5%of LP9,the organohydrogel(5LP9)demonstrated a tensile strength of 2.5MPa,elongation of 700%,conductivity of 432 mS/m,and a gauge factor of 1.7 with a good linearity,highlighting its excellent performance as an electronic conductive material.In addition,the organohydrogel exhibited remarkable environmental stability,antimicrobial properties,recyclability,and biocompatibility.When applied to human motion detection,voice recognition,and gesture recognition,the organohydrogel showcased excellent recognition ability,responsive functionality,and long-term monitoring stability.These findings provide a theoretical foundation for developing green and programmable wearable sensors for human-machine interaction,incorporating deep learning such as letter-writing recognition.
基金supported by the NCCR MARVEL,a National Centre of Competence in Research,funded by the Swiss National Science Foundation(grant number 51NF40-205602).
文摘Metal organic frameworks(MOFs)have a promising perspective as oxygen evolution reaction(OER)electrocatalysts due to their high surface areas and tunable structures.However,one of the main challenges for their further application is inferior stability during alkaline OER.Herein,operando x-ray absorption spectroscopy and operando x-ray diffraction of NiCo-MOF-74 materials unveil their electrochemical transformations differentiating between electrolyte-induced,beam-induced,and electrochemically induced changes of the electronic state and local structure around the transition metal centers in addition to their overall crystal structure.An inferior electrolyte-and beam stability of Co-MOF-74 is revealed in comparison to a more stable performance of Ni-MOF-74 and Ni0.25Co0.75-MOF-74.Based on the operando measurement results,good experimental practices for future MOF OER electrocatalyst studies are presented.
基金supported by the National Key Research and Development Program of China(2021YFB3802100)National Natural Science Foundation of China(Grants 52173228,52271190,and 524B2165)National Advanced Rare Metal Materials Technology Innovation Center Project(Program No.2024ZG-GCZX-01(1)-06).
文摘Artificial intelligence(AI)is revolutionizing sustainable materials science,yet a comprehensive and timely evaluation of the rapidly evolving AI techniques applied across the entire materials lifecycle remains lacking.Thiswork reviews AI-driven advances in sustainable materials,specifically focusing on battery materials,thermal management materials,energy conversion materials,and catalysts.The key patterns,capabilities,and limitations of AI are identified across three interconnected phases:sustainable materials design(leveraging predictive and generative models for accelerated discovery),green processing(integrating adaptive synthesis optimization and autonomous experimentation),and extending to lifecycle management(encompassing real-time monitoring,predictive maintenance,and intelligent recycling).Then,the persistent challenges,including data sparsity,domainspecific knowledge integration,and limited model generalizability,are investigated,followed by an exploration of emerging solutions such as federated learning for privacy-preserving data sharing,physics-informed neural networks for knowledge integration,and multimodal AI for cross-modal knowledge transfer.Finally,the computational sustainability challenges of AI methods themselves are also discussed.This review highlights key bottlenecks impeding scalable adoption and discuss pathways for realizing the full potential of AI in sustainable materials development.
基金supported by the National Natural Science Foundation of China(52472242,52272021,22005247)the Knowledge Innovation Project of Wuhan,China(2023020201010131)the central government guides local science and technology development projects(23zd3184).
文摘Polymer-derived SiOC materials are widely regarded as a new generation of anodes owing to their high specific capacity,low discharge platform,tunable chemical/structural composition,and good structural stability.However,tailoring the structure of SiOC to improve its electrochemical performance while simultaneously achieving elemental doping remains a challenge.Besides,the lithium storage mechanism and the structural evolution process of SiOC are still not fully understood due to its complex structure.In this study,a hollow porous SiOCN(Hp-SiOCN)featuring abundant oxygen defects is successfully prepared,achieving both the creation of a hollow porous structure and nitrogen element doping in one step,finally enhancing the structural stability and improving the lithium storage kinetics of Hp-SiOCN.In addition,the formation of a fully reversible structural unit,SiO3C─N,through the chemical interaction between N and Si/C,showcases a strong lithium adsorption capacity.Taking advantage of these combined benefits,the as-prepared Hp-SiOCN electrode delivers a reversible specific capacity of 412 mAh g^(−1)(93%capacity retention)after 500 cycles at 1.0 A g^(−1) and exhibited only 4%electrode expansion.This work offers valuable mechanistic insights into the synergistic optimization of elemental doping and structural design in SiOC,paving the way for advanced developments in battery technology.
基金supported by the National Natural Science Foundation of China(Grant No.52273093)the Fundamental Research Funds for the Central Universities(Grant No.SWU-XDJH202314).
文摘Sandwiched composites with a combination of electromagnetic interference(EMI)shielding performance,thermal conductivity,and electrical insulation show significant potential in electronic packaging.However,the fabrication of such composites using high-performance thermosets as matrices presents challenges due to their permanently crosslinked structures.Here,we relied on the dynamic covalent chemistry to propose an innovative interface-welding strategy to fabricate a sandwiched thermoset(covalent adaptable network)/carbon nanotubes/boron nitride(CAN/CNTs/BN)composite.To sustainability,theCANmatrixwas derived fromrenewable biobased resources,such as vanillin,glycerol triglycidyl ether,and 1,10-diaminodecane.The incorporation of CAN/BN composites as the outer layers bolstered thermal conductivity while maintaining electrical insulation,while the CAN/CNTs interlayer efficiently attenuated electromagnetic waves.With a BN and CNT content of 30 wt%,the CAN/CNTs/BN composite achieved a thermal conductivity of 1.79W⋅m^(−1)⋅K^(−1),an EMI shielding effectiveness exceeding 55 dB in the X-band,and an ultra-low electrical conductivity of 1.6×10^(−13)S⋅m^(−1).Leveraging dynamic covalent chemistry,the interface-welding technique fostered fully integrated interfaces,ensuring superior mechanical properties of CAN/CNTs/BN composite including a tensile modulus of 3837.8±196.9 MPa and tensile strength of 62.1±3.7 MPa.Additionally,its exceptional heat dissipation performance positions CAN/CNTs/BN composite as a promising contender for electronic packaging applications.
基金supported by the National Natural Science Foundation of China(Grant No.92372111,22179070,and 22075269)National Natural Science Fund for Excellent Young Scientists Fund(Overseas)Program(GG2090007003)+1 种基金the Natural Science Foundation of Jiangsu Province(Grant No.BK20220073)the Fundamental Research Funds for the Central Universities(Grant No.RF1028623157).
文摘Low-ionic conductivity within high-loading cathode has greatly limited the application of solid polymer electrolytes in rechargeable batteries.Herein,solid polymer electrolyte with a three-dimensionally conducting network is obtained by in situ polymerization of vinyl ethylene carbonate(VEC)with the aid of dipentaerythritol hexaacrylate(DPHA)crosslinker in the solidstate lithium(Li)metal batteries(LMBs).The weak coordination of Li^(+)with C═O and C─O groups promotes the dissociation and transport of Li^(+).The obtained P(VEC–DPHA)electrolyte enables a fast and orderly Li^(+)transport path and hinders the transport of TFSI^(-),rendering a remarkable ionic conductivity(2.53×10^(-4)S cm^(-1)),high Li+transference number(0.47),and wide electrochemical window(5.1 V).A total of 87.38%capacity retention rate of LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)||Li is achieved after 200 cycles at 0.2 C.P(VEC–DPHA)can also provide stable cycles under harsh conditions of high rate(1 C),high-cathode loading(10.83 mg cm^(-2)),and high-energy-density pouch cell(421.8Wh kg^(-1),cathode loading of 25 mg cm^(-2)).This work provides novel insights for the design of highly conductive polymer electrolytes and high-energy-density LMBs.
基金supported by the Hong Kong Research Grants Council(project number CityU 11201522).
文摘MXenes,a family of emerging two-dimensional materials offer enriched surface chemistry,high electrical conductivities,large specific surface area,intrinsic physicochemical properties,and excellent mechanical stability.However,restacking of MXene sheets limit their electrochemical performance.To overcome this limitation,recent advancements have focused on developing MXene composites with metal phosphates/phosphides(MXene/MPs).This review discusses the applications of MXene/MPs composites in energy storage and conversion applications.The incorporation ofMPs intoMXenes not only addresses the restacking issue and aggregation problems,but also enhances the overall electrochemical performance of energy storage and conversion systems.The review concludes with a summary of the current research status and future prospects for MXene/MPs-based composites in energy applications.
基金supported by City University of Hong Kong(grant no.7020038).
文摘Constructing an interlayer between perovskite and zinc oxide(ZnO)electron transporting layer to passivate the implacable interfacial defects for upgrading the efficiency and stability of flexible perovskite solar cells(f-PSC)is a daunting challenge and remains under explored.Herein,we present a cascade bridge interlayer strategy of zeolitic imidazole framework-8(ZIF-8)at the ZnO/perovskite interface.The ZIF-8 interlayer uplifts thework function,creating a cascade pathway and bridges through nitrogen bonding with Pb^(2+)ions of perovskite,thereby facilitating electron transport and reducing interfacial charge recombination.Consequently,the ZnO surface defects are passivated by alleviating the OH‒species,and thus the device stability is significantly improved.The f-PSC with ZIF-8 interlayer delivers a stable conversion efficiency of 17.10%with minimal hysteresis.By utilizing the piezo-phototronic effect and subjecting the f-PSC to a tensile strain of 1.6%,a stable efficiency of 18.47%was achieved,representing one of the highest reported efficiencies for ZnO nanorods-based f-PSC.Furthermore,the ZnO‒ZIF-8 exhibits high adsorption capacity toward lead and traps the mobile Pb^(2+)ions at the ZnO/perovskite interface,preventing the negative impact of lead leaching on environmental sustainability.
基金supported by the National Natural Science Foundation of China(52471227,52071144,and 52231009)Guangdong Basic and Applied Basic Research Foundation(2023B1515040011),Fundamental Research Funds for the Central Universities(2023A04J1566,2023ZYGXZR105,2023G008)TCL Science and Technology Innovation Fund(No.20222055).
文摘While sodium metal batteries(SMBs)possess remarkable superiority for next-generation energy storage systems,interfacial reactions,and dendrite growth due to the dissolution of solid electrolyte interphase(SEI)have seriously hindered the large-scale application of SMBs,especially at high temperatures.Here,a vinyl ethylene carbonate-based quasi-solid electrolyte(PVEC-QSPE)capable of enhancing the high-temperature stability of Na anodes is successfully synthesized by in situ curing of oligomeric poly(vinyl ethylene carbonate)(PVEC).The increased steric hindrance of PVEC reduces the coordination ability of C=O toward Na+,which promotes the cooperative migration of Na+with anions and the decomposition of anions to form the SEI.Furthermore,PVEC-QSPE significantly reduces the dissolution of SEI,which contains more organic components and fewer inorganic components,thereby minimizing the release of gases including CO_(2) and inhibiting the growth of sodium dendrites.The stable interface between PVEC-QSPE and Na helps Na|PVEC-QSPE|Na_(3)V_(2)(PO_(4))_(3)(NVP)batteries to operate stably at high temperatures,whose capacity retention rate reaches 80%at 80◦C and 93.3%at 60℃ after 3000 cycles employing high rate of 10 C.This work provides an efficient strategy to solve the problems of unstable SEI and dendrite growth,thereby promoting the development of safe and practical SMBs.
基金supported by Shaanxi Provincial High level Talent Introduction Project(5113220044)the Shaanxi Outstanding Youth Project(2023-JC-JQ-33)+6 种基金the Youth Science and Technology Talent Promotion Project of Jiangsu Association for Science and Technology(TJ-2022-088)the Project funded by China Postdoctoral Science Foundation(2023TQ0273,2023TQ0274,2023M742833)the Natural Science Basic Research Program of Shaanxi(2023-JC-QN-0726)Guangdong Basic and Applied Basic Research Foundation(2022A1515110286,2024A1515012538)the Suzhou Science and Technology Development Plan Innovation Leading Talent Project(ZXL2023183)the Fundamental Research Funds for the Central Universities(G2022KY05108,G2024KY0605,G2023KY0601)the Aeronautical Science Foundation of China(2018ZD53047).
文摘All-polymer solar cells(all-PSCs)are of interest owing to their unique advantages,including remarkably improved device stability and exceptional mechanical stretchability.Over recent years,there has been a notable increase in the power conversion efficiency(PCE)of all-PSCs,largely attributed to advancements in the morphology control of the active layer.Notably,the domain size is of paramount importance as it impacts critical factors such as exciton dissociation,charge transport,and collection.However,the low glass transition temperature of conjugated polymers,coupled with a minimal change in mixing entropy,often results in an excessive degree of phase separation.Consequently,it is essential to comprehend the evolution of phase separation and develop strategies to regulate the domain size.In this review,we elucidate the key parameters that contribute to the enhancement of phase separation and present qualitative and quantitative characterization techniques for domain size.Building on this foundation,we introduce the strategies and principles for regulating domain sizes,encompassing factors such as crystallinity,miscibility,and molecular conformation from a thermodynamic perspective,as well as the film-forming kinetics and the crystallization sequence from a kinetic perspective.Lastly,we offer insights into the current challenges and potential future prospects for the evolution of all-PSCs.
基金supported by National Natural Science Foundation of China(Grant No.52300218 and 22476066)Yunnan Fundamental Research Projects(Grant No.202401CF070197).
文摘The internal electric field(IEF)is key in speeding up the separation and transfer of photogenerated carriers,which boosts the production of reactive oxygen species(ROS).In this study,we present a novel silver iodide/N-rich carbon nitride(AgI/C_(3)N_(5))heterojunction catalyst with an IEF directed from AgI to C_(3)N_(5).We confirmed this IEF using density functional theory(DFT)calculations and various characterization methods.This IEF induces and reinforces the Type II transfer pathway for carrier separation and transfer,significantly increasing the production of ROS,particularly singlet oxygen(1O_(2)).As a result,the AgI/C_(3)N_(5)catalysts achieve 10.1 times the disinfection efficiency of C_(3)N_(5)and 5.6 times that of AgI,under one-min reaction time,107 CFU/mL of E.coli,visible light,and room temperature.It also outperforms most other AgI and carbon nitride-based heterojunction photocatalysts.Notably,the photogenerated holes(h+)selectively oxidize superoxide radicals(·O_(2)^(-))to 1O_(2)due to favorable energy alignment,minimizing O_(2)reduction effects and enhancing photocorrosion resistance,as demonstrated in five consecutive cycling experiments.In addition,the actual water disinfection tests confirmed its practical application potential.This work highlights the AgI/C_(3)N_(5)heterojunction catalyst’s promise as an efficient disinfection agent and sheds light on the photocatalytic disinfection mechanism.
基金supported by The National Natural Science Foundation of China(Grant Nos.21905033,52271201)the Science and Technology Department of Sichuan Province(Grant Nos.2025NSFTD0005,2022YFG0100,2022ZYD0045).
文摘Understanding and regulating the electronic states of single-atom sites near the Fermi energy level are essential for developing effective electrocatalysts for lithium–oxygen batteries(LOBs).In this study,we introduce an axial oxygen ligand at the metal center of cobalt porphyrin(CoPP)to adjust the electronic state of the Co center.Theoretical calculations and experimental findings show that this axial interaction disrupts the planar tetragonal crystal field of CoPP,resulting in enhanced spin polarization and electronic rearrangement.This rearrangement of d orbitals causes an upward shift in the frontier orbitals,which facilitates electron exchange during reactions.Additionally,the increased number of unpaired electrons in the d orbitals enhances the adsorption of CoPPO-MXene to various oxygen species,promoting the formation of a thin film-like Li2O2.These thin film-like discharge products improve contact with the electrode surfaces,leading to easier decomposition during the charging process.Consequently,CoPP-OMXene-based LOBs demonstrate a high discharge capacity of 11035mAh g−1,a low overpotential of 0.76 V,and remarkable cycling stability(445 cycles).
基金supported by Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(RS-2022-NR070534)funded by the Ministry of Education(RS-2020-NR049594).
文摘Recent advancements in lithium-oxygen(Li-O_(2))batteries have focused on incorporating redox mediators(RMs)into the electrolyte to address challenges of low energy efficiency and poor cycle life.However,various soluble RMs induce parasitic reactions with Li,compromising the anode stability.In this study,we design optimized Li-O_(2)batteries by introducing ZnI_(2)into the electrolyte,which serves a dual function:facilitating a stable LiZn/Zn protective layer on the Li metal anode and acting as an effective RM.The in situ formed LiZn/Zn layer prevents I_(3)^(-)shuttle effects,stabilizing the Li anode and promoting uniform Li plating and stripping.Additionally,the ZnI_(2)mediator facilitates rapid conversion of the I^(-)/I_(3)^(-)and I_(3)-/I_(2)redox couples at the cathode,contributing to amore reversible and lower overpotential Li_(2)O_(2)cycle.Notably,ZnI_(2)enhances early-stage LiO_(2)formation,verified by in situ Raman spectroscopy,which supports uniform sheet-like Li_(2)O_(2)deposition and contributes to stable cycling.These synergistic effects caused a significant reduction in the charge potential to less than 3.4 V,enabling over 800 stable cycles.This approach provides a viable pathway to achieving high energy density and long cycle life in Li-O_(2)batteries,positioning them for practical applications.
基金supported by the National Natural Science Foundation of China(no.52402128)Basic Research Programs of Taicang,2024(no.TC2024JC02)+1 种基金Natural Science Basic Research Program of Shaanxi(program no.2024JC-YBQN-0443)Natural Science Foundation of Chongqing,China(CSTB2022NSCQ-MSX0926 and CSTB2022NSCQ-MSX1335).
文摘Inorganic lead halide perovskites,especially CsPbI3,have witnessed significant progress in photovoltaic field due to their outstanding optoelectronic properties and high thermal stability.However,high-performance inorganic perovskite solar cells(IPSCs)are generally realized by strictly controlling the environmental humidity(mostly lower than 40%)during fabrication,which is undesirable for reducing fabrication cost and promoting further industrial production.Herein,a synergistic in situ hydrolysis polymerization strategy through 3,3,3-(trifluoropropyl)trichlorosilane(TFCS)and(3-2-aminoethylamino)propyltrimethoxysilane(AEMS)treatment is reported to prevent water invasion and realize efficient CsPbI3 IPSCs in highly humid air.TFCS not only regulates the crystallization process via hydrolysis reaction,but also stabilizes the phase structure by passivating the defects and producing a hydrophobic protection layer.Additionally,TFCS facilitates in situ polymerization of upper layer AEMS,thus promoting further enhanced protection of perovskites against ambient moisture.As a result,the CsPbI3 IPSCs fabricated at 45%humidity exhibit a dramatically improved efficiency of 20.09%,representing a record value for the inverted IPSCs fabricated in air with humidity over 40%.Moreover,the environmental humidity window for device fabrication can be broadened to 60%.This work provides an effective approach to stabilizing air-processedCsPbI3 and favoring the practical industrialmanufacture to further boost their cost-effective applications.
基金supported by the National Natural Science Foundation of China(21873032,21903032,22073033,21673087)startup fund from Huazhong University of Science and Technology(2006013118 and 3004013105)+1 种基金the Fundamental Research Funds for the Central Universities(2019kfyRCPY116)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003).
文摘Semiconducting phase is extremely rare and difficult to be realized in two-dimensional(2D)aluminum borides.Here,we for the first time report the discovery of a rarely semiconducting allotrope(labeled as AlB4-1)in 2D AlB4 nanosheets.This semiconductor is the global minimum structure in 2D space with two layers stacked together connected by strong Al-B bonds.Systematic studies demonstrate the high thermodynamic,lattice dynamic,thermal,and mechanical stabilities of AlB4-1.More importantly,this semiconducting AlB4-1 shows fascinating properties and promising applications,such as,the optimal band gap(1.156 eV at HSE06 level),high carrier mobility(up to 3.14×103 cm2V−1s−1),substantially high solar energy conversion efficiency(21.9%)and large optical response(106 cm−1)in the visible region.Extensive studies indiate that h-BN can serve as an effective substrate to support and encapsulate AlB4-1 with minimal impact on the electronic properties of AlB4-1,laying the foundation for the real application of AlB4-1 in electronic devices.Besides this semiconducting phase,other low-lying allotropes(AlB4-2 to-11)also display high stabilities,exotic properties and diverse applications.For example,the metallic AlB4-4 shows Dirac cone near Fermi level and superconductivity with TC as high as 23.4K,which can be substantially enhanced to 34.1K at tensile strain of 11%.These allotropes with different shapes show diverse hypercoordinate motifs with unusual bonding patterns.Comprehensive studies demonstrate that 2D AlB4 nanosheets is a class of highly stable,multifunctional nanomaterials for diverse applications in electronics,optics,optoelectronics,nanodevices,solar energy conversion,superconductivity,nanomechanics,and so on.The present study will provide useful guidance in fabricating these interesting nanostructures and stimulate both experimental and computational efforts in this direction.
