Elucidation of a reaction mechanism is the most critical aspect for designing electrodes for highperformance secondary batteries.Herein,we investigate the sodium insertion/extraction into an iron fluoride hydrate(FeF_...Elucidation of a reaction mechanism is the most critical aspect for designing electrodes for highperformance secondary batteries.Herein,we investigate the sodium insertion/extraction into an iron fluoride hydrate(FeF_(3)·0.5H_(2)O)electrode for sodium-ion batteries(SIBs).The electrode material is prepared by employing an ionic liquid 1-butyl-3-methylimidazolium-tetrafluoroborate,which serves as a reaction medium and precursor for F^(-)ions.The crystal structure of FeF_(3)·0.5H_(2)O is observed as pyrochlore type with large open 3-D tunnels and a unit cell volume of 1129A^(3).The morphology of FeF_(3)·0.5H_(2)O is spherical shape with a mesoporous structure.The microstructure analysis reveals primary particle size of around 10 nm.The FeF_(3)·0.5H_(2)O cathode exhibits stable discharge capacities of 158,210,and 284 mA h g^(-1) in three different potential ranges of 1.5-4.5,1.2-4.5,and 1.0-4.5 V,respectively at 0.05 C rate.The specific capacities remained stable in over 50 cycles in all three potential ranges,while the rate capability was best in the potential range of 1.5-4.5 V.The electrochemical sodium storage mechanism is studied using X-ray absorption spectroscopy,indicating higher conversion at a more discharged state.Ex-situ M?ssbauer spectroscopy strengthens the results for reversible reduction/oxidation of Fe.These results will be favorable to establish high-performance cathode materials with selective voltage window for SIBs.展开更多
There has been increasing demand for high-energy density and longcycle life rechargeable batteries to satisfy the ever-growing requirements for nextgeneration energy storage systems.Among all available candidates,dual...There has been increasing demand for high-energy density and longcycle life rechargeable batteries to satisfy the ever-growing requirements for nextgeneration energy storage systems.Among all available candidates,dual-ion batteries(DIBs)have drawn tremendous attention in the past few years from both academic and industrial battery communities because of their fascinating advantages of high working voltage,excellent safety,and environmental friendliness.However,the dynamic imbalance between the electrodes and the mismatch of traditional electrolyte systems remain elusive.To fully employ the advantages of DIBs,the overall optimization of anode materials,cathode materials,and compatible electrolyte systems is urgently needed.Here,we review the development history and the reaction mechanisms involved in DIBs.Afterward,the optimization strategies toward DIB materials and electrolytes are highlighted.In addition,their energy-related applications are also provided.Lastly,the research challenges and possible development directions of DIBs are outlined.展开更多
Electrochemical water splitting to produce hydrogen fuel is a promising renewable energy-conversion technique.Large-scale electrolysis of freshwater may deplete water resources and cause water scarcity worldwide.Thus,...Electrochemical water splitting to produce hydrogen fuel is a promising renewable energy-conversion technique.Large-scale electrolysis of freshwater may deplete water resources and cause water scarcity worldwide.Thus,seawater electrolysis is a potential solution to the future energy and water crisis.In seawater electrolysis,it is critical to develop cost-effective electrocatalysts to split seawater without chloride corrosion.Herein,we present zinc-doped nickel iron(oxy)hydroxide nanocubes passivated by negatively charged polyanions(NFZ-PBA-S)that exhibits outstanding catalytic activity,stability,and selectivity for seawater oxidation.Zn dopants and polyanion-rich passivated surface layers in NFZ-PBA-S could effectively repel chlorine ions and enhance corrosion resistance,enabling its excellent catalytic activity and stability for seawater oxidation.展开更多
Oxygen evolution reaction(OER)as a half-anodic reaction of water splitting hinders the overall reaction efficiency owing to its thermodynamic and kinetic limitations.Iodide oxidation reaction(IOR)with low thermodynami...Oxygen evolution reaction(OER)as a half-anodic reaction of water splitting hinders the overall reaction efficiency owing to its thermodynamic and kinetic limitations.Iodide oxidation reaction(IOR)with low thermodynamic barrier and rapid reaction kinetics is a promising alternative to the OER.Herein,we present a molybdenum disulfide(MoS_(2))electrocatalyst for a high-efficiency and remarkably durable anode enabling IOR.MoS_(2)nanosheets deposited on a porous carbon paper via atomic layer deposition show an IOR current density of 10 mA cm^(–2)at an anodic potential of 0.63 V with respect to the reversible hydrogen electrode owing to the porous substrate as well as the intrinsic iodide oxidation capability of MoS_(2)as confirmed by theoretical calculations.The lower positive potential applied to the MoS_(2)-based heterostructure during IOR electrocatalysis prevents deterioration of the active sites on MoS_(2),resulting in exceptional durability of 200 h.Subsequently,we fabricate a two-electrode system comprising a MoS_(2)anode for IOR combined with a commercial Pt@C catalyst cathode for hydrogen evolution reaction.Moreover,the photovoltaic–electrochemical hydrogen production device comprising this electrolyzer and a single perovskite photovoltaic cell shows a record-high current density of 21 mA cm^(–2)at 1 sun under unbiased conditions.展开更多
To overcome the serious technological issues affecting lithium-sulfur(Li-S) batteries,such as sluggish sulfur redox kinetics and the detrimental shuttle effect,heterostructure engineering has been investigated as a st...To overcome the serious technological issues affecting lithium-sulfur(Li-S) batteries,such as sluggish sulfur redox kinetics and the detrimental shuttle effect,heterostructure engineering has been investigated as a strategy to effectively capture soluble lithium polysulfide intermediates and promote their conversion reaction by integrating highly polar metal oxides with catalytically active metals sulfides.However,to fully exploit the outstanding properties of heterostructure-based composites,their detailed structure and interfacial contacts should be designed rationally.Herein,optimally arranged TiO_(2)and MoS_(2)-based heterostructures(TiO_(2)@MoS_(2)) are fabricated on carbon cloth as a multifunctional interlayer to efficiently trap polysulfide intermediates and accelerate their redox kinetics.Owing to the synergistic effects between TiO_(2)and MoS_(2)and the uniform heterointerface distribution that induces the ideally oriented built-in electric field,Li-S batteries with TiO_(2)@MoS_(2)interlayers exhibit high rate capability(601 mA h g^(-1)at 5 C),good cycling stability(capacity-fade rate of 0.067% per cycle over 500 cycles at2 C),and satisfactory areal capacity(5.2 mA h cm^(-2)) under an increased sulfur loading of 5.2 mg cm^(-2).Moreover,by comparing with a MoS_(2)@TiO_(2)interlayer composed of reversely arranged heterostructures,the effect of the built-in electric field’s direction on the electrocatalytic reactions of polysulfide intermediates is thoroughly investigated for the first time.The superior electrocatalytic activities of the rationally arranged TiO_(2)@MoS_(2)interlayer demonstrate the importance of optimizing the built-in electric field of heterostructures for producing high-performance Li-S batteries.展开更多
Commercialization of Zn-metal anodes with low cost and high theoretical capacity is hindered by the poor reversibility caused by dendrites growth,side reactions,and the slow Zn^(2+)-transport and reaction kinetics.Her...Commercialization of Zn-metal anodes with low cost and high theoretical capacity is hindered by the poor reversibility caused by dendrites growth,side reactions,and the slow Zn^(2+)-transport and reaction kinetics.Herein,a reversible heterogeneous electrode of Zn-nanocrystallites/polyvinylphosphonic acrylamide(Zn/PPAm)with fast electrochemical kinetics is designed for the first time:phosphonic acid groups with strong polarity and chelation effect ensure structural reversibility and stability of the threedimensional Zn-storage-host PPAm network and the Zn/PPAm hybrid;hydrophobic carbon chains suppress side reactions such as hydrogen evolution and corrosion;weak electron-donating amide groups constitute Zn^(2+)-transport channels and promote“desolvation”and“solvation”effects of Zn^(2+)by dragging the PPAm network on the Zn-metal surface to compress/stretch during Zn plating/stripping,respectively;and the heterostructure and Zn nanocrystallites suppress dendrite growth and enhance electrochemical reactivity,respectively.Thus,the Zn/PPAm electrode shows cycle reversibility of over 6000 h with a hysteresis voltage as low as 31 mV in symmetrical cells and excellent durability and flexibility in fiber-shaped batteries.展开更多
In this work,we developed the PM6:Y6-based inverted structure organic photovoltaic(i-OPV)with improved power conversion efficiency(PCE)and long-term stability by resolving the origins of the performance deterioration....In this work,we developed the PM6:Y6-based inverted structure organic photovoltaic(i-OPV)with improved power conversion efficiency(PCE)and long-term stability by resolving the origins of the performance deterioration.The deep defects between the metal oxide-based electron transport layer and bulk-heterojunction photoactive layer interface were responsible for suboptimal PCE and facilitated degradation of devices.While the density of deep traps is increased during the storage of i-OPV,the penetrative oxygen-containing defects additionally generated shallow traps below the band-edge of Y6,causing an additional loss in the open-circuit voltage.The suppression of interfacial defects by chemical modification effectively improved the PCE and long-term stability of i-OPV.The modified i-OPV(mi-OPV)achieved a PCE of 17.42%,which is the highest value among the reported PM6:Y6-based i-OPV devices.Moreover,long-term stability was significantly improved:~90%and~80%retention of its initial PCE after 1200 h of air storage and illumination,respectively.展开更多
Bulk heterojunction(BHJ)composites show improved power conversion efficiencies when optimized in terms of morphology using various film processing methods.A reduced carrier recombination loss in an optimized BHJ was c...Bulk heterojunction(BHJ)composites show improved power conversion efficiencies when optimized in terms of morphology using various film processing methods.A reduced carrier recombination loss in an optimized BHJ was characterized previously.However,the driving force that leads to this reduction was not clearly understood.In this study,we focus on the decreased carrier recombination loss and its driving force in optimized nonfullerene acceptor-based PTB7-Th:IEICO-4F BHJ composites.We demonstrate that the optimized BHJ shows deactivation in the sub-nanosecond nongeminate carrier recombination process.The driving force for this deactivation was determined to be the improved interchain hole delocalization between the polymers.An enhanced interchain hole delocalization was observed using steady-state photoinduced absorption(PIA)spectroscopy.In particular,increased splitting between the polaron PIA bands was noted.Moreover,improved interchain hole delocalization was observed for other state-of-the-art BHJ materials,including D18:Y6 with optimized morphologies.展开更多
Ceria-based heterostructure composite(CHC)has become a new stream to develop advanced low-temperature(300–600°C)solid oxide fuel cells(LTSOFCs)with excellent power outputs at 1000 mW cm−2 level.The state-ofthe-a...Ceria-based heterostructure composite(CHC)has become a new stream to develop advanced low-temperature(300–600°C)solid oxide fuel cells(LTSOFCs)with excellent power outputs at 1000 mW cm−2 level.The state-ofthe-art ceria–carbonate or ceria–semiconductor heterostructure composites have made the CHC systems significantly contribute to both fundamental and applied science researches of LTSOFCs;however,a deep scientific understanding to achieve excellent fuel cell performance and high superionic conduction is still missing,which may hinder its wide application and commercialization.This review aims to establish a new fundamental strategy for superionic conduction of the CHC materials and relevant LTSOFCs.This involves energy band and built-in-field assisting superionic conduction,highlighting coupling effect among the ionic transfer,band structure and alignment impact.Furthermore,theories of ceria–carbonate,e.g.,space charge and multi-ion conduction,as well as new scientific understanding are discussed and presented for functional CHC materials.展开更多
The practical applications of aqueous Zn metal batteries are currently restricted by the inherent drawbacks of Zn such as the hydrogen evolution reaction,sluggish kinetics,and dendrite formation.To address these probl...The practical applications of aqueous Zn metal batteries are currently restricted by the inherent drawbacks of Zn such as the hydrogen evolution reaction,sluggish kinetics,and dendrite formation.To address these problems,herein,a limitedly Zn-doped MgF_(2)interphase comprising an upper region of pure,porous MgF_(2)and a lower region of gradient Zn-doped MgF_(2)is achieved via radio frequency sputtering technique.The porous MgF_(2)region is a polar insulator whose high corrosion resistance facilitates the de-solvation of the solvated Zn ions and suppression of hydrogen evolution,resulting in Zn metal electrodes with a low interfacial resistance.The Zn-doped MgF_(2)region facilitates fast transfer kinetics and homogeneous deposition of Zn ions owing to the interfacial polarization between the Zn dopant and MgF_(2)matrix,and the high concentration of the Zn dopant on the surface of the metal substrate as fine nuclei.Consequently,a symmetric cell incorporating the proposed Zn metal exhibits low overpotentials of~27.2 and~99.7 mV without Zn dendrites over 250 to 8000 cycles at current densities of 1.0 and 10.0 mA cm−2,respectively.The developed Zn/MnO2 full cell exhibits superior capacity retentions of 97.5%and 84.0%with average Coulombic efficiencies of 99.96%after 1000 and 3000 cycles,respectively.展开更多
Nickel-iron nanocrystalline alloys with different compositions and grain sizes were fabricated by electroplating for MEMS devices. The iron content of the deposits was changed by varying the nickel/iron ion ratio in t...Nickel-iron nanocrystalline alloys with different compositions and grain sizes were fabricated by electroplating for MEMS devices. The iron content of the deposits was changed by varying the nickel/iron ion ratio in the electrolyte. X-ray diffraction (XRD) analysis was applied for measuring the strength of the texture and grain size of the deposits. The nickel/iron atom ratio of the deposits was analyzed by EDS. The hardness of the alloys was evaluated by Vickers hardness indenter. The internal stress of the deposits was measured by thin film stress measurement using Stoney's formula. Surface morphology and roughness were investigated by scanning electron microscopy (SEM) and atomic force microscopy (AFM). Hardness and internal stress mechanism of the electroplated structure as a function of Fe ion content and current density were revealed. With increasing the iron content, the hardness and internal stress of the deposits increase. An excellent correlation between the increase in the internal stress and the loss of (200) texture were found.展开更多
In the original version of the article affiliation 1 has been missed out for an author and affiliation 1 superscript has been added in this correction.The Original article has been corrected.Joong Kee Lee1,5Open Acces...In the original version of the article affiliation 1 has been missed out for an author and affiliation 1 superscript has been added in this correction.The Original article has been corrected.Joong Kee Lee1,5Open Access This article is licensed under a Creative Commons Attribution 4.0 International License,which permits use,sharing,adaptation,distribution and reproduction in any medium or format,as long as you give appropriate credit to the original author(s)and the source,provide a link to the Creative Commons licence,and indicate if changes were made.展开更多
Semiconductors and the associated methodologies applied to electrochemistry have recently grown as an emerging field in energy materials and technologies.For example,semiconductor membranes and heterostructure fuel ce...Semiconductors and the associated methodologies applied to electrochemistry have recently grown as an emerging field in energy materials and technologies.For example,semiconductor membranes and heterostructure fuel cells are new technological trend,which differ from the traditional fuel cell electrochemistry principle employing three basic functional components:anode,electrolyte,and cathode.The electrolyte is key to the device performance by providing an ionic charge flow pathway between the anode and cathode while preventing electron passage.In contrast,semiconductors and derived heterostructures with electron(hole)conducting materials have demonstrated to be much better ionic conductors than the conventional ionic electrolytes.The energy band structure and alignment,band bending and built-in electric field are all important elements in this context to realize the necessary fuel cell functionalities.This review further extends to semiconductor-based electrochemical energy conversion and storage,describing their fundamentals and working principles,with the intention of advancing the understanding of the roles of semiconductors and energy bands in electrochemical devices for energy conversion and storage,as well as applications to meet emerging demands widely involved in energy applications,such as photocatalysis/water splitting devices,batteries and solar cells.This review provides new ideas and new solutions to problems beyond the conventional electrochemistry and presents new interdisciplinary approaches to develop clean energy conversion and storage technologies.展开更多
Highly active and stable electrocatalysts are mandatory for developing high-performance and longlasting fuel cells.The current study demonstrates a high oxygen reduction reaction(ORR)electrocatalytic activity of a nov...Highly active and stable electrocatalysts are mandatory for developing high-performance and longlasting fuel cells.The current study demonstrates a high oxygen reduction reaction(ORR)electrocatalytic activity of a novel spinel-structured LaFe_(2)O_(4)via a self-doping strategy.The LaFe_(2)O_(4)demonstrates excellent ORR activity in a protonic ceramic fuel cell(PCFC)at temperature range of 350-500℃.The high ORR activity of LaFe_(2)O_(4)is mainly attributed to the facile release of oxide and proton ions,and improved synergistic incorporation abilities associated with interplay of multivalent Fe^(3+)/Fe^(2+)and La^(3+)ions.Using LaFe_(2)O_(4)as cathode over proton conducting BaZr_(0.4)Ce_(0.4)Y_(0.2)O_(3)(BZCY)electrolyte,the fuel cell has delivered a high-power density of 806 mW/cm^(2)operating at 500℃.Different spectroscopic and calculations methods such as UV-visible,Raman,X-ray photoelectron spectroscopy and density functional theory(DFT)calculations were performed to screen the potential application of LaFe_(2)O_(4)as cathode.This study would help in developing functional cobalt-free ORR electrocatalysts for low temperature-PCFCs(LT-PCFCs)and solid oxide fuel cells(SOFCs)applications.展开更多
Ceramic fuel cells hold an important position for the sustainable energy future using renewable energy sources with high efficiency.The design and synthesis of active materials,interface engineering and having capabil...Ceramic fuel cells hold an important position for the sustainable energy future using renewable energy sources with high efficiency.The design and synthesis of active materials,interface engineering and having capability of low operating temperature is considered as an important factor to further increase the power output and stability of ceramic fuel cell devices.A novel methodology has vital importance to develop new functionalities of existing materials by introducing new different effects.The built-in electric field(BIEF) is one of the most recently used approaches to improve charge transfer and ionic conductivity of solid oxide materials.Herein,we demonstrate gradient doping strategy in CeO_(2)-δstructure to produce BIEF effect and to modulate the proton transport effectively at the surface layer rather than bulk structure.The inclusions of La and Sr metal ions at the surface and Co-metal ions into bulk-layer of CeO_(2)form the gradiently doped structure.The gradient doping into CeO_(2)highly improves the proton transport properties through the surface layer by modifying the energy levels.Moreover,unbalanced charge distribution due to gradient doping produces built-in electric-field to provide extra driving force for protons transport through surface layer.The acquired gradiently doped fluorite structure exhibits remarkable proton conductivity of>0.2 S/cm,as a result ceramic fuel cell shows power output of>1000 mW/cm2while operating at 500℃.This unique work highlights the critical role of gradiently doped electrolyte in electrochemical conversion energy devices and offers new understanding and practices for sustainable energy future.展开更多
Solid-state lithium-metal batteries(SLMBs)have been regarded as one of the most promising next-generation devices because of their potential high safety,high energy density,and simple packing procedure.However,the pra...Solid-state lithium-metal batteries(SLMBs)have been regarded as one of the most promising next-generation devices because of their potential high safety,high energy density,and simple packing procedure.However,the practical applications of SLMBs are restricted by a series of static and dynamic interfacial issues,including poor interfacial contact,(electro-)chemical incompatibility,dynamic Li dendrite penetration,etc.In recent years,considerable attempts have been made to obtain mechanistic insight into interfacial failures and to develop possible strategies towards excellent interfacial properties for SLMBs.The static and dynamic failure mechanisms at interfaces between solid electrolytes(SEs)and electrodes are comprehensively summarized,and design strategies involving interfacial modification,electrode/SE engineering,and the monolithic construction of SLMBs are discussed in detail.Finally,possible research methodologies such as theoretical calcu-lations,advanced characterization techniques,and versatile design strategies are provided to tackle these interfacial problems.展开更多
In this work, the friction characteristics of single-layer MoS_2 prepared with chemical vapor deposition(CVD) at three different temperatures were quantitatively investigated and compared to those of single-layer MoS_...In this work, the friction characteristics of single-layer MoS_2 prepared with chemical vapor deposition(CVD) at three different temperatures were quantitatively investigated and compared to those of single-layer MoS_2 prepared using mechanical exfoliation. The surface and crystalline qualities of the MoS_2 specimens were characterized using an optical microscope, atomic force microscope(AFM), and Raman spectroscopy. The surfaces of the MoS2 specimens were generally flat and smooth. However, the Raman data showed that the crystalline qualities of CVD-grown single-layer MoS2 at 800 °C and 850 °C were relatively similar to those of mechanically exfoliated MoS2 whereas the crystalline quality of the CVD-grown single-layer MoS_2 at 900 °C was lower. The CVD-grown single-layer MoS_2 exhibited higher friction than mechanically exfoliated single-layer MoS_2, which might be related to the crystalline imperfections in the CVD-grown MoS_2. In addition, the friction of CVD-grown single-layer MoS_2 increased as the CVD growth temperature increased. In terms of tribological properties, 800 °C was the optimal temperature for the CVD process used in this work. Furthermore, it was observed that the friction at the grain boundary was significantly larger than that at the grain, potentially due to defects at the grain boundary. This result indicates that the temperature used during CVD should be optimized considering the grain size to achieve low friction characteristics. The outcomes of this work will be useful for understanding the intrinsic friction characteristics of single-layer MoS2 and elucidating the feasibility of single-layer MoS_2 as protective or lubricant layers for micro- and nano-devices.展开更多
With the rapid development of the wearable electronics,the flexible supercapacitor with high energy density has attracted more and more attentions.From the viewpoint of outdoor and underwater application,this research...With the rapid development of the wearable electronics,the flexible supercapacitor with high energy density has attracted more and more attentions.From the viewpoint of outdoor and underwater application,this research tried to impart the superhydrophobicity to the flexible supercapacitors.The polyvinyl alcohol/HN0_(3) hydrogel was utilized as the electrolyte,which could achieve self-healing capability without the freezing/thawing process.Both microscale graphene and nanoscale carbon nanotubes were utilized as the electrode materials.After surface modification,the hydrophobic suspension composed of graphene and carbon nanotubes was sprayed onto the two sides of hydrogel electrolyte to construct superhydrophobic electrode.Hence,the superhydrophobicity endows the supercapacitor with outstanding self-cleaning performance.The all-in-one structure endows the supercapacitor with improved capacitive ability,outstanding flexibility,good anti-abrasion property,and reliable self-healing capability.The combination of superhydro-phobicity and flexible energy storage might have a broad application for the outdoor and underwater wearable electronics applications.展开更多
基金supported by the Basic Science Research Program of the National Research Foundation(NRF)of South Koreafunded by the Ministry of Science&ICT and Future Planning(NRF-2020M3H4A3081889)KIST Institutional Program of South Korea(Project Nos.2E31860)。
文摘Elucidation of a reaction mechanism is the most critical aspect for designing electrodes for highperformance secondary batteries.Herein,we investigate the sodium insertion/extraction into an iron fluoride hydrate(FeF_(3)·0.5H_(2)O)electrode for sodium-ion batteries(SIBs).The electrode material is prepared by employing an ionic liquid 1-butyl-3-methylimidazolium-tetrafluoroborate,which serves as a reaction medium and precursor for F^(-)ions.The crystal structure of FeF_(3)·0.5H_(2)O is observed as pyrochlore type with large open 3-D tunnels and a unit cell volume of 1129A^(3).The morphology of FeF_(3)·0.5H_(2)O is spherical shape with a mesoporous structure.The microstructure analysis reveals primary particle size of around 10 nm.The FeF_(3)·0.5H_(2)O cathode exhibits stable discharge capacities of 158,210,and 284 mA h g^(-1) in three different potential ranges of 1.5-4.5,1.2-4.5,and 1.0-4.5 V,respectively at 0.05 C rate.The specific capacities remained stable in over 50 cycles in all three potential ranges,while the rate capability was best in the potential range of 1.5-4.5 V.The electrochemical sodium storage mechanism is studied using X-ray absorption spectroscopy,indicating higher conversion at a more discharged state.Ex-situ M?ssbauer spectroscopy strengthens the results for reversible reduction/oxidation of Fe.These results will be favorable to establish high-performance cathode materials with selective voltage window for SIBs.
基金support from the National Key R&D Program of China(2022YFB2402600)National Natural Science Foundation of China(52125105,51972329)+2 种基金NSFC/RGC Joint Research Scheme(Project No:N_CityU104/20 and 52061160484)Shenzhen Science and Technology Planning Project(JCYJ20200109115624923,JSGG20220831104004008)Science and Technology Planning Project of Guangdong Province(2019TX05L389).
文摘There has been increasing demand for high-energy density and longcycle life rechargeable batteries to satisfy the ever-growing requirements for nextgeneration energy storage systems.Among all available candidates,dual-ion batteries(DIBs)have drawn tremendous attention in the past few years from both academic and industrial battery communities because of their fascinating advantages of high working voltage,excellent safety,and environmental friendliness.However,the dynamic imbalance between the electrodes and the mismatch of traditional electrolyte systems remain elusive.To fully employ the advantages of DIBs,the overall optimization of anode materials,cathode materials,and compatible electrolyte systems is urgently needed.Here,we review the development history and the reaction mechanisms involved in DIBs.Afterward,the optimization strategies toward DIB materials and electrolytes are highlighted.In addition,their energy-related applications are also provided.Lastly,the research challenges and possible development directions of DIBs are outlined.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea (NRF)funded by the Ministry of Science,ICT and Future Planning (2021R1A2C2091497 and 2022R1A2C2010162)supported by“Regional Innovation Strategy (RIS)”through the National Research Foundation of Korea (NRF)funded by the Ministry of Education (MOE) (2022RIS-005)+1 种基金supported by the Ministry of Trade,Industry,and Energy (20018145)supported by KIST Institutional Program (Project Nos.2V09781)。
文摘Electrochemical water splitting to produce hydrogen fuel is a promising renewable energy-conversion technique.Large-scale electrolysis of freshwater may deplete water resources and cause water scarcity worldwide.Thus,seawater electrolysis is a potential solution to the future energy and water crisis.In seawater electrolysis,it is critical to develop cost-effective electrocatalysts to split seawater without chloride corrosion.Herein,we present zinc-doped nickel iron(oxy)hydroxide nanocubes passivated by negatively charged polyanions(NFZ-PBA-S)that exhibits outstanding catalytic activity,stability,and selectivity for seawater oxidation.Zn dopants and polyanion-rich passivated surface layers in NFZ-PBA-S could effectively repel chlorine ions and enhance corrosion resistance,enabling its excellent catalytic activity and stability for seawater oxidation.
基金the National R&D Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(Grant Nos.2021R1A3B10689202021M3H4A1A03049662)+1 种基金the Materials and Components Technology Development Program of MOTIE/KEIT(10080527)the Yonsei Signature Research Cluster Program of 2021(2021-22-0002)。
文摘Oxygen evolution reaction(OER)as a half-anodic reaction of water splitting hinders the overall reaction efficiency owing to its thermodynamic and kinetic limitations.Iodide oxidation reaction(IOR)with low thermodynamic barrier and rapid reaction kinetics is a promising alternative to the OER.Herein,we present a molybdenum disulfide(MoS_(2))electrocatalyst for a high-efficiency and remarkably durable anode enabling IOR.MoS_(2)nanosheets deposited on a porous carbon paper via atomic layer deposition show an IOR current density of 10 mA cm^(–2)at an anodic potential of 0.63 V with respect to the reversible hydrogen electrode owing to the porous substrate as well as the intrinsic iodide oxidation capability of MoS_(2)as confirmed by theoretical calculations.The lower positive potential applied to the MoS_(2)-based heterostructure during IOR electrocatalysis prevents deterioration of the active sites on MoS_(2),resulting in exceptional durability of 200 h.Subsequently,we fabricate a two-electrode system comprising a MoS_(2)anode for IOR combined with a commercial Pt@C catalyst cathode for hydrogen evolution reaction.Moreover,the photovoltaic–electrochemical hydrogen production device comprising this electrolyzer and a single perovskite photovoltaic cell shows a record-high current density of 21 mA cm^(–2)at 1 sun under unbiased conditions.
基金supported by the National R&D Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (2018M3D1A1058793 and 2021R1A3B1068920)supported by the Creative Materials Discovery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (2018M3D1A1058744)the Yonsei Signature Research Cluster Program of 2021 (2021-22-0002)。
文摘To overcome the serious technological issues affecting lithium-sulfur(Li-S) batteries,such as sluggish sulfur redox kinetics and the detrimental shuttle effect,heterostructure engineering has been investigated as a strategy to effectively capture soluble lithium polysulfide intermediates and promote their conversion reaction by integrating highly polar metal oxides with catalytically active metals sulfides.However,to fully exploit the outstanding properties of heterostructure-based composites,their detailed structure and interfacial contacts should be designed rationally.Herein,optimally arranged TiO_(2)and MoS_(2)-based heterostructures(TiO_(2)@MoS_(2)) are fabricated on carbon cloth as a multifunctional interlayer to efficiently trap polysulfide intermediates and accelerate their redox kinetics.Owing to the synergistic effects between TiO_(2)and MoS_(2)and the uniform heterointerface distribution that induces the ideally oriented built-in electric field,Li-S batteries with TiO_(2)@MoS_(2)interlayers exhibit high rate capability(601 mA h g^(-1)at 5 C),good cycling stability(capacity-fade rate of 0.067% per cycle over 500 cycles at2 C),and satisfactory areal capacity(5.2 mA h cm^(-2)) under an increased sulfur loading of 5.2 mg cm^(-2).Moreover,by comparing with a MoS_(2)@TiO_(2)interlayer composed of reversely arranged heterostructures,the effect of the built-in electric field’s direction on the electrocatalytic reactions of polysulfide intermediates is thoroughly investigated for the first time.The superior electrocatalytic activities of the rationally arranged TiO_(2)@MoS_(2)interlayer demonstrate the importance of optimizing the built-in electric field of heterostructures for producing high-performance Li-S batteries.
基金National Research Foundation of Korea,Grant/Award Numbers:2022R1F1A1074441,2022R1F1A1074707KIST Institutional Program,Grant/Award Numbers:2V09480,2E32582。
文摘Commercialization of Zn-metal anodes with low cost and high theoretical capacity is hindered by the poor reversibility caused by dendrites growth,side reactions,and the slow Zn^(2+)-transport and reaction kinetics.Herein,a reversible heterogeneous electrode of Zn-nanocrystallites/polyvinylphosphonic acrylamide(Zn/PPAm)with fast electrochemical kinetics is designed for the first time:phosphonic acid groups with strong polarity and chelation effect ensure structural reversibility and stability of the threedimensional Zn-storage-host PPAm network and the Zn/PPAm hybrid;hydrophobic carbon chains suppress side reactions such as hydrogen evolution and corrosion;weak electron-donating amide groups constitute Zn^(2+)-transport channels and promote“desolvation”and“solvation”effects of Zn^(2+)by dragging the PPAm network on the Zn-metal surface to compress/stretch during Zn plating/stripping,respectively;and the heterostructure and Zn nanocrystallites suppress dendrite growth and enhance electrochemical reactivity,respectively.Thus,the Zn/PPAm electrode shows cycle reversibility of over 6000 h with a hysteresis voltage as low as 31 mV in symmetrical cells and excellent durability and flexibility in fiber-shaped batteries.
基金supported by a National Research Foundation of Korea(grant#:2020R1A2C1003929,2019R1A6A1A11053838,2020M1A2A2080746,2021M2E8A1044198,2016R1A5A1012966,2021M3H4A1A03051379).
文摘In this work,we developed the PM6:Y6-based inverted structure organic photovoltaic(i-OPV)with improved power conversion efficiency(PCE)and long-term stability by resolving the origins of the performance deterioration.The deep defects between the metal oxide-based electron transport layer and bulk-heterojunction photoactive layer interface were responsible for suboptimal PCE and facilitated degradation of devices.While the density of deep traps is increased during the storage of i-OPV,the penetrative oxygen-containing defects additionally generated shallow traps below the band-edge of Y6,causing an additional loss in the open-circuit voltage.The suppression of interfacial defects by chemical modification effectively improved the PCE and long-term stability of i-OPV.The modified i-OPV(mi-OPV)achieved a PCE of 17.42%,which is the highest value among the reported PM6:Y6-based i-OPV devices.Moreover,long-term stability was significantly improved:~90%and~80%retention of its initial PCE after 1200 h of air storage and illumination,respectively.
基金supported by the National Research Foundation of Korea(NRF)grants funded by the Korea government(MSIT)(2022R1F1A1065586,2019R1A6A1A11053838)the GIST Research Institute(GRI)APRI grant funded by the GIST in 2022.
文摘Bulk heterojunction(BHJ)composites show improved power conversion efficiencies when optimized in terms of morphology using various film processing methods.A reduced carrier recombination loss in an optimized BHJ was characterized previously.However,the driving force that leads to this reduction was not clearly understood.In this study,we focus on the decreased carrier recombination loss and its driving force in optimized nonfullerene acceptor-based PTB7-Th:IEICO-4F BHJ composites.We demonstrate that the optimized BHJ shows deactivation in the sub-nanosecond nongeminate carrier recombination process.The driving force for this deactivation was determined to be the improved interchain hole delocalization between the polymers.An enhanced interchain hole delocalization was observed using steady-state photoinduced absorption(PIA)spectroscopy.In particular,increased splitting between the polaron PIA bands was noted.Moreover,improved interchain hole delocalization was observed for other state-of-the-art BHJ materials,including D18:Y6 with optimized morphologies.
文摘Ceria-based heterostructure composite(CHC)has become a new stream to develop advanced low-temperature(300–600°C)solid oxide fuel cells(LTSOFCs)with excellent power outputs at 1000 mW cm−2 level.The state-ofthe-art ceria–carbonate or ceria–semiconductor heterostructure composites have made the CHC systems significantly contribute to both fundamental and applied science researches of LTSOFCs;however,a deep scientific understanding to achieve excellent fuel cell performance and high superionic conduction is still missing,which may hinder its wide application and commercialization.This review aims to establish a new fundamental strategy for superionic conduction of the CHC materials and relevant LTSOFCs.This involves energy band and built-in-field assisting superionic conduction,highlighting coupling effect among the ionic transfer,band structure and alignment impact.Furthermore,theories of ceria–carbonate,e.g.,space charge and multi-ion conduction,as well as new scientific understanding are discussed and presented for functional CHC materials.
基金supported by research grants from the National Research Foundation(NRF-2019H1D3A1A01069779)funded by the Ministry of Science and ICT,Republic of Korea,and by the Institutional Program(2E31863)and Bridge Program-KIST(2V09284).
文摘The practical applications of aqueous Zn metal batteries are currently restricted by the inherent drawbacks of Zn such as the hydrogen evolution reaction,sluggish kinetics,and dendrite formation.To address these problems,herein,a limitedly Zn-doped MgF_(2)interphase comprising an upper region of pure,porous MgF_(2)and a lower region of gradient Zn-doped MgF_(2)is achieved via radio frequency sputtering technique.The porous MgF_(2)region is a polar insulator whose high corrosion resistance facilitates the de-solvation of the solvated Zn ions and suppression of hydrogen evolution,resulting in Zn metal electrodes with a low interfacial resistance.The Zn-doped MgF_(2)region facilitates fast transfer kinetics and homogeneous deposition of Zn ions owing to the interfacial polarization between the Zn dopant and MgF_(2)matrix,and the high concentration of the Zn dopant on the surface of the metal substrate as fine nuclei.Consequently,a symmetric cell incorporating the proposed Zn metal exhibits low overpotentials of~27.2 and~99.7 mV without Zn dendrites over 250 to 8000 cycles at current densities of 1.0 and 10.0 mA cm−2,respectively.The developed Zn/MnO2 full cell exhibits superior capacity retentions of 97.5%and 84.0%with average Coulombic efficiencies of 99.96%after 1000 and 3000 cycles,respectively.
文摘Nickel-iron nanocrystalline alloys with different compositions and grain sizes were fabricated by electroplating for MEMS devices. The iron content of the deposits was changed by varying the nickel/iron ion ratio in the electrolyte. X-ray diffraction (XRD) analysis was applied for measuring the strength of the texture and grain size of the deposits. The nickel/iron atom ratio of the deposits was analyzed by EDS. The hardness of the alloys was evaluated by Vickers hardness indenter. The internal stress of the deposits was measured by thin film stress measurement using Stoney's formula. Surface morphology and roughness were investigated by scanning electron microscopy (SEM) and atomic force microscopy (AFM). Hardness and internal stress mechanism of the electroplated structure as a function of Fe ion content and current density were revealed. With increasing the iron content, the hardness and internal stress of the deposits increase. An excellent correlation between the increase in the internal stress and the loss of (200) texture were found.
文摘In the original version of the article affiliation 1 has been missed out for an author and affiliation 1 superscript has been added in this correction.The Original article has been corrected.Joong Kee Lee1,5Open Access This article is licensed under a Creative Commons Attribution 4.0 International License,which permits use,sharing,adaptation,distribution and reproduction in any medium or format,as long as you give appropriate credit to the original author(s)and the source,provide a link to the Creative Commons licence,and indicate if changes were made.
基金the National Natural Science Foundation of China(51772080,51672208,51774259,and 51402093)the Natural Science Foundation of Guangdong Province(2021A1515012356 and 2017A030313289)+4 种基金the project foundation from the Ministry of Education of Guangdong Province(2019KTSCX151)Shenzhen Government Plan of Science and Technology(JCYJ20180305125247308)the National Laboratory of Solid State Microstructures,Nanjing University,EPSRC(EP/I013229/1)Royal Society and Newton Fund(NAF\R1\191294)Key Program for International S&T Cooperation Projects of Shaanxi Province(2019JZ-20,2019KWZ-03)。
文摘Semiconductors and the associated methodologies applied to electrochemistry have recently grown as an emerging field in energy materials and technologies.For example,semiconductor membranes and heterostructure fuel cells are new technological trend,which differ from the traditional fuel cell electrochemistry principle employing three basic functional components:anode,electrolyte,and cathode.The electrolyte is key to the device performance by providing an ionic charge flow pathway between the anode and cathode while preventing electron passage.In contrast,semiconductors and derived heterostructures with electron(hole)conducting materials have demonstrated to be much better ionic conductors than the conventional ionic electrolytes.The energy band structure and alignment,band bending and built-in electric field are all important elements in this context to realize the necessary fuel cell functionalities.This review further extends to semiconductor-based electrochemical energy conversion and storage,describing their fundamentals and working principles,with the intention of advancing the understanding of the roles of semiconductors and energy bands in electrochemical devices for energy conversion and storage,as well as applications to meet emerging demands widely involved in energy applications,such as photocatalysis/water splitting devices,batteries and solar cells.This review provides new ideas and new solutions to problems beyond the conventional electrochemistry and presents new interdisciplinary approaches to develop clean energy conversion and storage technologies.
基金Project supported by the National Natural Science Foundation of China(51772080,11604088,51706093)Jiangsu Provence Talent Program(JSSCRC2021491)。
文摘Highly active and stable electrocatalysts are mandatory for developing high-performance and longlasting fuel cells.The current study demonstrates a high oxygen reduction reaction(ORR)electrocatalytic activity of a novel spinel-structured LaFe_(2)O_(4)via a self-doping strategy.The LaFe_(2)O_(4)demonstrates excellent ORR activity in a protonic ceramic fuel cell(PCFC)at temperature range of 350-500℃.The high ORR activity of LaFe_(2)O_(4)is mainly attributed to the facile release of oxide and proton ions,and improved synergistic incorporation abilities associated with interplay of multivalent Fe^(3+)/Fe^(2+)and La^(3+)ions.Using LaFe_(2)O_(4)as cathode over proton conducting BaZr_(0.4)Ce_(0.4)Y_(0.2)O_(3)(BZCY)electrolyte,the fuel cell has delivered a high-power density of 806 mW/cm^(2)operating at 500℃.Different spectroscopic and calculations methods such as UV-visible,Raman,X-ray photoelectron spectroscopy and density functional theory(DFT)calculations were performed to screen the potential application of LaFe_(2)O_(4)as cathode.This study would help in developing functional cobalt-free ORR electrocatalysts for low temperature-PCFCs(LT-PCFCs)and solid oxide fuel cells(SOFCs)applications.
基金Project supported by the Fundamental Research Funds for the Central Universities (3203002105A2,4303002184)Jiangsu Provincial Program (JSSCRC2021491)。
文摘Ceramic fuel cells hold an important position for the sustainable energy future using renewable energy sources with high efficiency.The design and synthesis of active materials,interface engineering and having capability of low operating temperature is considered as an important factor to further increase the power output and stability of ceramic fuel cell devices.A novel methodology has vital importance to develop new functionalities of existing materials by introducing new different effects.The built-in electric field(BIEF) is one of the most recently used approaches to improve charge transfer and ionic conductivity of solid oxide materials.Herein,we demonstrate gradient doping strategy in CeO_(2)-δstructure to produce BIEF effect and to modulate the proton transport effectively at the surface layer rather than bulk structure.The inclusions of La and Sr metal ions at the surface and Co-metal ions into bulk-layer of CeO_(2)form the gradiently doped structure.The gradient doping into CeO_(2)highly improves the proton transport properties through the surface layer by modifying the energy levels.Moreover,unbalanced charge distribution due to gradient doping produces built-in electric-field to provide extra driving force for protons transport through surface layer.The acquired gradiently doped fluorite structure exhibits remarkable proton conductivity of>0.2 S/cm,as a result ceramic fuel cell shows power output of>1000 mW/cm2while operating at 500℃.This unique work highlights the critical role of gradiently doped electrolyte in electrochemical conversion energy devices and offers new understanding and practices for sustainable energy future.
基金supported by the National Key R&D Program of China(2022YFB2402600)the National Natural Science Foundation of China(11904379,51972329,52061160484,52125105,52188101)+1 种基金the Shenzhen Science and Technology Planning Project(JCYJ20210324101203009,JCYJ2020010911562492,JCYJ20190807171803813)the Guangdong Basic and Applied Basic Research Foundation(2022A1515011493,2019A1515011902,2019TX05L389,2020B0301030002).
文摘Solid-state lithium-metal batteries(SLMBs)have been regarded as one of the most promising next-generation devices because of their potential high safety,high energy density,and simple packing procedure.However,the practical applications of SLMBs are restricted by a series of static and dynamic interfacial issues,including poor interfacial contact,(electro-)chemical incompatibility,dynamic Li dendrite penetration,etc.In recent years,considerable attempts have been made to obtain mechanistic insight into interfacial failures and to develop possible strategies towards excellent interfacial properties for SLMBs.The static and dynamic failure mechanisms at interfaces between solid electrolytes(SEs)and electrodes are comprehensively summarized,and design strategies involving interfacial modification,electrode/SE engineering,and the monolithic construction of SLMBs are discussed in detail.Finally,possible research methodologies such as theoretical calcu-lations,advanced characterization techniques,and versatile design strategies are provided to tackle these interfacial problems.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea (NRF)funded by the Ministry of Science, ICT and Future Planning (NRF-2017R1A2B4009651)
文摘In this work, the friction characteristics of single-layer MoS_2 prepared with chemical vapor deposition(CVD) at three different temperatures were quantitatively investigated and compared to those of single-layer MoS_2 prepared using mechanical exfoliation. The surface and crystalline qualities of the MoS_2 specimens were characterized using an optical microscope, atomic force microscope(AFM), and Raman spectroscopy. The surfaces of the MoS2 specimens were generally flat and smooth. However, the Raman data showed that the crystalline qualities of CVD-grown single-layer MoS2 at 800 °C and 850 °C were relatively similar to those of mechanically exfoliated MoS2 whereas the crystalline quality of the CVD-grown single-layer MoS_2 at 900 °C was lower. The CVD-grown single-layer MoS_2 exhibited higher friction than mechanically exfoliated single-layer MoS_2, which might be related to the crystalline imperfections in the CVD-grown MoS_2. In addition, the friction of CVD-grown single-layer MoS_2 increased as the CVD growth temperature increased. In terms of tribological properties, 800 °C was the optimal temperature for the CVD process used in this work. Furthermore, it was observed that the friction at the grain boundary was significantly larger than that at the grain, potentially due to defects at the grain boundary. This result indicates that the temperature used during CVD should be optimized considering the grain size to achieve low friction characteristics. The outcomes of this work will be useful for understanding the intrinsic friction characteristics of single-layer MoS2 and elucidating the feasibility of single-layer MoS_2 as protective or lubricant layers for micro- and nano-devices.
基金the National Natural Science Foundation of China(Nos.51977079,51777076,51607067)the Youth Elite Scientists Sponsorship Program by the Chinese Society for Electrical Engineering(No.CSEE-YESS-2017002)the Fundamental Research Funds for the Central Universities(Nos.2020MS115,2017MS149).
文摘With the rapid development of the wearable electronics,the flexible supercapacitor with high energy density has attracted more and more attentions.From the viewpoint of outdoor and underwater application,this research tried to impart the superhydrophobicity to the flexible supercapacitors.The polyvinyl alcohol/HN0_(3) hydrogel was utilized as the electrolyte,which could achieve self-healing capability without the freezing/thawing process.Both microscale graphene and nanoscale carbon nanotubes were utilized as the electrode materials.After surface modification,the hydrophobic suspension composed of graphene and carbon nanotubes was sprayed onto the two sides of hydrogel electrolyte to construct superhydrophobic electrode.Hence,the superhydrophobicity endows the supercapacitor with outstanding self-cleaning performance.The all-in-one structure endows the supercapacitor with improved capacitive ability,outstanding flexibility,good anti-abrasion property,and reliable self-healing capability.The combination of superhydro-phobicity and flexible energy storage might have a broad application for the outdoor and underwater wearable electronics applications.
