As global energy demand increases and environmental standards tighten,the development of efficient,eco-friendly energy conversion and storage technologies becomes crucial.Solid oxide cells(SOCs)show great promise beca...As global energy demand increases and environmental standards tighten,the development of efficient,eco-friendly energy conversion and storage technologies becomes crucial.Solid oxide cells(SOCs)show great promise because of their high energy conversion efficiency and wide range of applications.Highentropy materials(HEMs),a novel class of materials comprising several principal elements,have attracted significant interest within the materials science and energy sectors.Their distinctive structural features and adaptable functional properties offer immense potential for innovation across various applications.This review systematically covers the basic concepts,crystal structures,element selection,and major synthesis strategies of HEMs,and explores in detail the specific applications of these materials in SOCs,including its potential as air electrodes,fuel electrodes,electrolytes,and interconnects(including barrier coatings).By analyzing existing studies,this review reveals the significant advantages of HEMs in enhancing the performance,anti-poisoning,and stability of SOCs;highlights the key areas and challenges for future research;and looks into possible future directions.展开更多
Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3...Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe oxide.It is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe oxide.Considering the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.展开更多
Layer-structured Ruddlesden–Popper(RP)perovskites(RPPs)with decent stability have captured the imagination of the photovoltaic research community and bring hope for boosting the development of perovskite solar cell(P...Layer-structured Ruddlesden–Popper(RP)perovskites(RPPs)with decent stability have captured the imagination of the photovoltaic research community and bring hope for boosting the development of perovskite solar cell(PSC)technology.However,two-dimensional(2D)or quasi-2D RP PSCs are encountered with some challenges of the large exciton binding energy,blocked charge transport and poor film quality,which restrict their photovoltaic performance.Fortunately,these issues can be readily resolved by rationally designing spacer cations of RPPs.This review mainly focuses on how to design the molecular structures of organic spacers and aims to endow RPPs with outstanding photovoltaic applications.We firstly elucidated the important roles of organic spacers in impacting crystallization kinetics,charge transporting ability and stability of RPPs.Then we brought three aspects to attention for designing organic spacers.Finally,we presented the specific molecular structure design strategies for organic spacers of RPPs aiming to improve photovoltaic performance of RP PSCs.These proposed strategies in this review will provide new avenues to develop novel organic spacers for RPPs and advance the development of RPP photovoltaic technology for future applications.展开更多
Seawater electrolysis is promising for green hydrogen production, while its application is inhibited by sluggish anodic oxygen evolution reaction (OER) and rapid chloride corrosion‐induced electrode deactivation. Her...Seawater electrolysis is promising for green hydrogen production, while its application is inhibited by sluggish anodic oxygen evolution reaction (OER) and rapid chloride corrosion‐induced electrode deactivation. Herein, we report a conductive and ion‐ selective OER electrocatalyst with a CoFe alloy core and microporous metal‐doped carbon shell. Co/Fe‐N_(4)‐C active sites in the shell optimize the adsorption strength of intermediates and synergize with the metal core to endow the catalyst with high OER activity and selectivity, while the rich ultra‐micropores in the shell demonstrate a significant sieving effect to hinder Cl− transfer, thus protecting the inner Co/Fe‐N_(4)‐C active sites and metal core from Cl− corrosion. The catalyst is assembled in an alkaline seawater electrolyzer with an electrode geometric area of 254 cm^(2) and delivers a current density of 3000 A m^(-2) at 1.85 V for 330 h. Such catalysts can be synthesized in a large batch (100 g), providing sound opportunities for industrial seawater splitting.展开更多
Ni-rich LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM)cathodes in layered oxide cathodes are attractive for high-energy lithium-ion batteries but suffer from rapid capacity fade and thermal instability at high charge voltages.I...Ni-rich LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM)cathodes in layered oxide cathodes are attractive for high-energy lithium-ion batteries but suffer from rapid capacity fade and thermal instability at high charge voltages.In this study,we propose an entropy-assisted multi-element doping strategy to mitigate these issues.Specifically,two routes are designed and compared:bulk-like localized high-entropy doping(BHE-NCM)and surface-distributed high-entropy-zone doping(SHE-NCM).The surface entropy-doped NCM cathode delivers enhanced electrochemical performance,including higher capacity retention under 4.5 V cycling and superior rate capability,compared to both bulk-like and pristine counterparts.Comprehensive material characterization reveals that surface-localized doping stabilizes the layered structure with reduced microcrack formation and creates a uniform dopant-rich surface region with improved thermal and electrochemical stability.Overall,entropy-assisted doping at the near surface zone effectively alleviates structural degradation and interface reactions in Ni-rich NCM,enabling improved cycling performance at high voltage.This work highlights the significance of surface entropy engineering as a promising strategy for designing high-voltage cathodes with improved safety and longevity.展开更多
Microbial fuel cells(MFCs)are promising for realizing wastewater remediation and electricity co-generation,which may significantly promote the formation of an environmentally friendly,clean energy society.Unfortunatel...Microbial fuel cells(MFCs)are promising for realizing wastewater remediation and electricity co-generation,which may significantly promote the formation of an environmentally friendly,clean energy society.Unfortunately,most of the available MFCs show relatively low electricity generation.Anodes,the major component of MFCs,play the most critical role in electron transfer and organic decomposition,which directly determine the performance of MFCs.In the past decades,various carbonaceous materials and carbon-supported conductive composites have been extensively exploited to optimize the electron transfer on the anode due to their versatile properties,such as large surface area and excellent electrical conductivity.The development of anode materials with a particular structure and performance to satisfy field-scale long-term operation of MFCs remains a huge research challenge,which attracts great attention and urgently needs in-depth exploration of the material engineering of anodes for MFCs.In this review,recent advances in the development and optimization of anodes for MFCs are summarized,and applications of MFCs with advanced anodes in the remediation of different types of wastewater are discussed.Advances of anodes for promoting electron transfer,microbial attachment and organic decomposition are the main focuses.The superiorities of MFCs on different aspects of wastewater remediation are elucidated,along with perspectives on future research of MFCs,aiming to provide useful guidance in related fields.展开更多
Reversible proton ceramic electrochemical cell(R-PCEC)is regarded as the most promising energy conversion device,which can realize efficient mutual conversion of electrical and chemical energy and to solve the problem...Reversible proton ceramic electrochemical cell(R-PCEC)is regarded as the most promising energy conversion device,which can realize efficient mutual conversion of electrical and chemical energy and to solve the problem of large-scale energy storage.However,the development of robust electrodes with high catalytic activity is the main bottleneck for the commercialization of R-PCECs.Here,a novel type of high-entropy perovskite oxide consisting of six equimolar metals in the A-site,Pr_(1/6)La_(1/6)Nd_(1/6)Ba_(1/6)Sr_(1/6)Ca_(1/6)CoO_(3−δ)(PLN-BSCC),is reported as a high-performance bifunctional air electrode for R-PCEC.By harnessing the unique functionalities of multiple ele-ments,high-entropy perovskite oxide can be anticipated to accelerate reaction rates in both fuel cell and electrolysis modes.Especially,an R-PCEC utilizing the PLNBSCC air electrode achieves exceptional electrochemical performances,demonstrating a peak power density of 1.21 W cm^(−2)for the fuel cell,while simultaneously obtaining an astonishing current density of−1.95 A cm^(−2)at an electrolysis voltage of 1.3 V and a temperature of 600℃.The significantly enhanced electrochemical performance and durability of the PLNBSCC air electrode is attributed mainly to the high electrons/ions conductivity,fast hydration reactivity and high configurational entropy.This research explores to a new avenue to develop optimally active and stable air electrodes for R-PCECs.展开更多
Electrochemical water splitting represents one of the most promising technologies to produce green hydrogen,which can help to realize the goal of achieving carbon neutrality.While substantial efforts on a laboratory s...Electrochemical water splitting represents one of the most promising technologies to produce green hydrogen,which can help to realize the goal of achieving carbon neutrality.While substantial efforts on a laboratory scale have been made for understanding fundamental catalysis and developing high-performance electrocatalysts for the two half-reactions involved in water electrocatalysis,much less attention has been paid to doing relevant research on a larger scale.For example,few such researches have been done on an industrial scale.Herein,we review the very recent endeavors to bridge the gaps between fundamental research and industrial applications for water electrolysis.We begin by introducing the fundamentals of electrochemical water splitting and then present comparisons of testing protocol,figure of merit,catalyst of interest,and manufacturing cost for laboratory and industry-based water-electrolysis research.Special attention is paid to tracking the surface reconstruction process and identifying real catalytic species under different testing conditions,which highlight the significant distinctions of corresponding electrochemical reconstruction mechanisms.Advances in catalyst designs for industry-relevant water electrolysis are also summarized,which reveal the progress of moving the practical applications forward and accelerating synergies between material science and engineering.Perspectives and challenges of electrocatalyst design strategies are proposed finally to further bridge the gaps between lab-scale research and large-scale electrocatalysis applications.展开更多
Rational construction of carbon-based materials with high-efficiency bifunctionality and low cost as the substitute of precious metal catalyst shows a highly practical value for rechargeable Zn-air batteries(ZABs)yet ...Rational construction of carbon-based materials with high-efficiency bifunctionality and low cost as the substitute of precious metal catalyst shows a highly practical value for rechargeable Zn-air batteries(ZABs)yet it still remains challenging.Herein,this study employs a simple mixing-calcination strategy to fabricate a high-performance bifunctional composite catalyst composed of N-doped graphitic carbon encapsulating Co nanoparticles(Co@NrC).Benefiting from the core-shell architectural and compositional advantages of favorable electronic configuration,more exposed active sites,sufficient electric conductivity,rich defects,and excellent charge transport,the optimal Co@NrC hybrid(Co@NrC-0.3)presents outstanding catalytic activity and stability toward oxygen-related electrochemical reactions(oxygen reduction and evolution reactions,i.e.,ORR and OER),with a low potential gap of 0.766 V.Besides,the rechargeable liquid ZAB assembled with this hybrid electrocatalyst delivers a high peak power density of 168 mW cm^(−2),a small initial discharge-charge potential gap of 0.45 V at 10 mA cm^(−2),and a good rate performance.Furthermore,a relatively large power density of 108 mW cm^(−2) is also obtained with the Co@NrC-0.3-based flexible solid-state ZAB,which can well power LED lights.Such work offers insights in developing excellent bifunctional electrocatalysts for both OER and ORR and highlights their potential applications in metal-air batteries and other energy-conversion/storage devices.展开更多
High-temperature solid-state electrolyte is a key component of several important electrochemical devices,such as oxygen sensors for automobile exhaust control,solid oxide fuel cells(SOFCs) for power generation,and sol...High-temperature solid-state electrolyte is a key component of several important electrochemical devices,such as oxygen sensors for automobile exhaust control,solid oxide fuel cells(SOFCs) for power generation,and solid oxide electrolysis cells for H_(2) production from water electrolysis or CO_(2) electrochemical reduction to value-added chemicals.In particular,internal diffusion of protons or oxygen ions is a fundamental and crucial issue in the research of SOFCs,hypothetically based on either oxygen-ionconducting electrolytes or proton-conducting electrolytes.Up to now,some electrolyte materials based on fluorite or perovskite structure were found to show certain degree of dual-ion transportation capability,while in available electrolyte database,particularly in the field of SOFCs,such dual-ion conductivity was seriously overlooked.Actually,few concerns arising to the simultaneous proton and oxygen-ion conductivities in electrolyte of SOFCs inevitably induce various inadequate and confusing results in literature.Understanding dual-ion transportation behavior in electrolyte is indisputably of great importance to explain some unusual fuel cell performance as reported in literature and enrich the knowledge of solid state ionics.On the other hand,exploration of novel dual-ion conducting electrolytes will benefit the development of SOFCs.In this review,we provide a comprehensive summary of the understanding of dual-ion transportation in solid electrolyte and recent advances of dual-ion conducting SOFCs.The oxygen ion and proton conduction mechanisms at elevated temperature inside oxide-based electrolyte materials are first introduced,and then(mixed) oxygen ion and proton conduction behaviors of fluorite and perovskite-type oxides are discussed.Following on,recent advances in the development of dual-ion conducting SOFCs based on fluorite and perovskite-type single-phase or composite electrolytes,are reviewed.Finally,the challenges in the development of dual-ion conducting SOFCs are discussed and future prospects are proposed.展开更多
High-entropy oxides(HEOs)are gaining prominence in the field of electrochemistry due to their distinctive structural characteristics,which give rise to their advanced stable and modifiable functional properties.This r...High-entropy oxides(HEOs)are gaining prominence in the field of electrochemistry due to their distinctive structural characteristics,which give rise to their advanced stable and modifiable functional properties.This review presents fundamental preparations,incidental characterizations,and typical structures of HEOs.The prospective applications of HEOs in various electrochemical aspects of electrocatalysis and energy conversion-storage are also summarized,including recent developments and the general trend of HEO structure design in the catalysis containing oxygen evolution reaction(OER)and oxygen reduction reaction(ORR),supercapacitors(SC),lithium-ion batteries(LIBs),solid oxide fuel cells(SOFCs),and so forth.Moreover,this review notes some apparent challenges and multiple opportunities for the use of HEOs in the wide field of energy to further guide the development of practical applications.The influence of entropy is significant,and high-entropy oxides are expected to drive the improvement of energy science and technology in the near future.展开更多
Molybdenum carbide(MoxC)with variable phase structure possesses flexible hydrogen-binding energy(HBE),which is a promising hydrogen evolution reaction(HER)catalyst.Herein,a hybrid multiphase MoxC freestanding film cou...Molybdenum carbide(MoxC)with variable phase structure possesses flexible hydrogen-binding energy(HBE),which is a promising hydrogen evolution reaction(HER)catalyst.Herein,a hybrid multiphase MoxC freestanding film coupled with Co3Mo(CM/MoxC@NC)is synthesized through the electrospinning method supplemented by the heteroatom incorporation.CM/MoxC@NC surpasses its pure phase counterparts and exhibits remarkable catalytic activity at 114mV to deliver a current density of 10mA cm^(−2) in acid,which is among the first-rate level performance reported for MoxC-based catalysts.The subsequent ex situ and in situ characterizations reveal a phase transition mechanism based on self-catalysis that CoOx depletes the coordinated C ofα-MoC via the interaction,which realizes the assembly of weak HBEα-MoC and strong HBEβ-Mo2C,and the enhanced utilization of active materials as well.The multiple structures with optimal HBE are in favor of the stepwise reactions of HER,as the study of the correlation between HBE and phase structure revealed.This study discloses the underlying phase transition mechanism and highlights the HBE–structure relationship that should be considered for catalyst design.展开更多
Simultaneously enhancing the reaction kinetics,mass transport,and gas release during alkaline hydrogen evolution reaction(HER)is critical to minimizing the reaction polarization resistance,but remains a big challenge....Simultaneously enhancing the reaction kinetics,mass transport,and gas release during alkaline hydrogen evolution reaction(HER)is critical to minimizing the reaction polarization resistance,but remains a big challenge.Through rational design of a hierarchical multiheterogeneous three-dimensionally(3D)ordered macroporous Mo_(2)C-embedded nitrogen-doped carbon with ultrafine Ru nanoclusters anchored on its surface(OMS Mo_(2)C/NC-Ru),we realize both electronic and morphologic engineering of the catalyst to maximize the electrocatalysis performance.The formed Ru-NC heterostructure shows regulative electronic states and optimized adsorption energy with the intermediate H*,and the Mo_(2)C-NC heterostructure accelerates the Volmer reaction due to the strong water dissociation ability as confirmed by theoretical calculations.Consequently,superior HER activity in alkaline solution with an extremely low overpotential of 15.5 mV at 10 mAcm^(−2)with the mass activity more than 17 times higher than that of the benchmark Pt/C,an ultrasmall Tafel slope of 22.7 mV dec−1,and excellent electrocatalytic durability were achieved,attributing to the enhanced mass transport and favorable gas release process endowed from the unique OMS Mo_(2)C/NC-Ru structure.By oxidizing OMS Mo_(2)C/NC-Ru into OMS MoO_(3)-RuO_(2)catalyst,it can also be applied as efficient oxygen evolution electrocatalyst,enabling the construction of a quasi-symmetric electrolyzer for overall water splitting.Such a device's performance surpassed the state-of-the-art Pt/C||RuO2 electrolyzer.This study provides instructive guidance for designing 3D-ordered macroporous multicomponent catalysts for efficient catalytic applications.展开更多
Fuel flexibility is one of the most distinguished advantages of solid oxide fuel cells(SOFCs)over other low-temperature fuel cells.Furthermore,the combination of ammonia fuel and SOFCs technology should be a promising...Fuel flexibility is one of the most distinguished advantages of solid oxide fuel cells(SOFCs)over other low-temperature fuel cells.Furthermore,the combination of ammonia fuel and SOFCs technology should be a promising clean energy system after considering the high energy density,easy transportation/storage,matured synthesis technology and carbon-free nature of NH_(3) as well as high efficiency of SOFCs.However,the large-scale applications of direct-ammonia SOFCs(DASOFCs)are strongly limited by the inferior anti-sintering capability and catalytic activity for ammonia decomposition reaction of conventional nickel-based cermet anode.Herein,a slightly ruthenium(Ru)doping in perovskite oxides is proposed to promote the alloy nanoparticle exsolution,enabling better DA-SOFCs with enhanced power outputs and operational stability.After treating Ru-doped Pr_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.75)Ru_(0.05)O_(3-δ) single-phase perovskite in a reducing atmosphere,in addition to the formation of two layered Ruddlesden-Popper perovskites and Pr_(2)O_(3) nanoparticles(the same as the Ru-free counterpart,Pr_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)),the exsolution of CoFeRu-based alloy nanoparticles is remarkably promoted.Such reduced Pr_(0.6)Sr0.4Co_(0.2)Fe_(0.75)Ru_(0.05)O_(3-δ) composite anode shows superior catalytic activity and stability for NH_(3) decomposition reaction as well as anti-sintering capability in DA-SOFCs to those of reduced Pr0.6Sr0.4Co0.2Fe0.8O_(3-δ)due to the facilitated nanoparticle exsolution and stronger nanoparticle/substrate interaction.This work provides a facile and effective strategy to design highly active and durable anodes for DA-SOFCs,promoting large-scale applications of this technology.展开更多
Aluminum-metal batteries show great potential as next-generation energy storage due to their abundant resources and intrinsic safety.However,the crucial limitations of metallic Al anodes,such as dendrite and corrosion...Aluminum-metal batteries show great potential as next-generation energy storage due to their abundant resources and intrinsic safety.However,the crucial limitations of metallic Al anodes,such as dendrite and corrosion problems in conventional aluminum-metal batteries,remain challenging and elusive.Here,we report a novel electrodeposition strategy to prepare an optimized 3D Al anode on carbon cloth with an uniform deposition morphology,low local current density,and mitigatory volume change.The symmetrical cells with the 3D Al anode show superior stable cycling(>450 h)and low-voltage hysteresis(~170 mV)at 0.5 mA cm^(−2).High reversibility(~99.7%)is achieved for the Al plating/stripping.The graphite||Al‐4/CC full batteries show a long lifespan of 800 cycles with 54 mAh g^(−1) capacity at a high current density of 1000 mA g^(−1),benefiting from the high capacitive-controlled distribution.This study proposes a novel strategy to design 3D Al anodes for metallic-Al-based batteries by eliminating the problems of planar Al anodes and realizing the potential applications of aluminum-graphite batteries.展开更多
The development of bi-functional electrocatalyst with high catalytic activity and stable performance for both oxygen evolution/reduction reactions(OER/ORR)in aqueous alkaline solution is key to realize practical appli...The development of bi-functional electrocatalyst with high catalytic activity and stable performance for both oxygen evolution/reduction reactions(OER/ORR)in aqueous alkaline solution is key to realize practical application of zinc-air batteries(ZABs).In this study,we reported a new porous nano-micro-composite as a bifunctional electrocatalyst for ZABs,devised by the in situ growth of metal-organic framework(MOF)nanocrystals onto the micrometersized Ba0.5Sr0.5Co0.8Fe0.2O3(BSCF)perovskite oxide.Upon carbonization,MOF was converted to porous nitrogen-doped carbon nanocages and ultrafine cobalt oxides and CoN4 nanoparticles dispersing inside the carbon nanocages,which further anchored on the surface of BSCF oxide.We homogeneously dispersed BSCF perovskite particles in the surfactant;subsequently,ZIF-67 nanocrystals were grown onto the BSCF particles.In this way,leaching of metallic or organic species in MOFs and the aggregation of BSCF were effectively suppressed,thus maximizing the number of active sites for improving OER.The BSCF in turn acted as catalyst to promote the graphitization of carbon during pyrolysis,as well as to optimize the transition metal-tocarbon ratio,thus enhancing the ORR catalytic activity.A ZAB fabricated from such air electrode showed outstanding performance with a potential gap of only 0.83 V at 5 mA cm-2 for OER/ORR.Notably,no obvious performance degradation was observed for the continuous charge-discharge operation for 1800 cycles over an extended period of 300 h.展开更多
Electrochemical conversion of CO_(2)to CO is an economically feasible method for mitigating greenhouse gas emissions.Among various electrochemical approaches,solid oxide electrolysis cells(SOECs)show high potential fo...Electrochemical conversion of CO_(2)to CO is an economically feasible method for mitigating greenhouse gas emissions.Among various electrochemical approaches,solid oxide electrolysis cells(SOECs)show high potential for CO_(2)reduction reaction(CO_(2)-RR)due to their ability to operate at high temperatures,resulting in fast reaction kinetics and increased efficiency.Considering their main energy loss is still associated with the large overpotential at the fuel electrode,the development of the highly efficient and durable cathode for SOECs has been extensively searched after.Here,we propose an A-site doping strategy to enhance the properties of Sr_(2)Fe_(1.5)Mo_(0.5)O_(6−δ)(SFM),which improve its performance as a cathode in SOECs for CO_(2)-RR,demonstrating favorable activity and durability.The structural and physiochemical characterizations,together with DFT calculations,show that the partial replacement of Sr by Bi in the SFM double perovskite not only improves CO_(2) adsorption capability at the catalyst surface but also enhances oxygen ionic conduction inside the bulk oxide,resulting in enhanced CO_(2)electrocatalysis performance in SOECs.Specifically,a La_(0.8)Sr_(0.2)Ga_(0.8)Mg_(0.2)O_(3−δ) (LSGM)electrolyte-supported single cell with the new Bi-doped SFM cathode demonstrates a large current density of 1620 mA cm^(−2) at a cell potential of 1.6 V at 850°C with good operational stability up to 200 h.Bi-doped SFM thus represents a highly promising cathode for ceramic CO_(2)electrolyzers and could accelerate our transition towards a carbon-neutral society.展开更多
The oxygen evolution reaction(OER) plays a crucial role in many electrochemical energy technologies,and creating multiple beneficial factors for OER catalysis is desirable for achieving high catalytic efficiency.Here,...The oxygen evolution reaction(OER) plays a crucial role in many electrochemical energy technologies,and creating multiple beneficial factors for OER catalysis is desirable for achieving high catalytic efficiency.Here,we highlight a new halogen-chlorine(Cl)-anion doping strategy to boost the OER activity of perovskite oxides.As a proof-of-concept,proper Cl doping at the oxygen site of LaFeO3(LFO) perovskite can induce multiple favorable characteristics for catalyzing the OER,including rich oxygen vacancies,increased electrical conductivity and enhanced Fe-O covalency.Benefiting from these factors,the LaFeO2.9-δCl0.1(LFOCl) perovskite displays significant intrinsic activity enhancement by a factor of around three relative to its parent LFO.This work uncovers the effect of Cl-anion doping in perovskites on promoting OER performance and paves a new way to design highly efficient electrocatalysts.展开更多
Before the practical application of rechargeable Zn-air batteries(ZABs),a critical issue regarding the inherent slow reaction kinetics of the oxygen reduction(ORR)and oxygen evolution(OER)must be addressed.Here,we fab...Before the practical application of rechargeable Zn-air batteries(ZABs),a critical issue regarding the inherent slow reaction kinetics of the oxygen reduction(ORR)and oxygen evolution(OER)must be addressed.Here,we fabricate a cost-effective bifunctional oxygen electrocatalyst with a self-antistacking structure,where three-dimensional(3D)Fe-Co bimetallic oxide particles(FeCoO_(x))are directly grown on 2D N-doped graphene(NG).The in situ grown FeCoO_(x)particles can alleviate the NG interlaminar restacking,ensuring abundant channels for diffusion of O_(2)/OH−species,while the NG allows rapid electron flow.Benefiting from this self-antistacking 3D-on-2D structure and synergetic electrocatalysis,FeCoO_(x)@NG demonstrated excellent activity for both ORR and OER(ΔE=0.78 V),which is superior to that of the binary mixtures of Pt/C and RuO_(2)(ΔE=0.83 V).A homemade ZAB with 20%-FeCoO_(x)@NG delivers a specific capacity of 758.9 mAh g^(−1),a peak power density of 215 mW cm^(−2),and long-term cyclability for over 400 h.These research results suggest that designing a bimetallic oxide/N-doped carbon 3D-on-2D nanoarchitecture using an in situ growth strategy is an attractive and feasible solution to overcome electrocatalytic problems in ZABs.展开更多
The requirement for a sustainable and renewable energy has inspired substantial interests in designing and developing earth-abundant and high-effectiveness electrocatalysts/electrodes for fuel cells and metal-air batt...The requirement for a sustainable and renewable energy has inspired substantial interests in designing and developing earth-abundant and high-effectiveness electrocatalysts/electrodes for fuel cells and metal-air batteries,in which oxygen reduction reaction(ORR)plays a crucial role.Perovskite oxides have acquired rapid attention as ORR electrocatalysts to replace noble-metal-based catalysts owing to their intrinsic electrocatalytic activity,compositional and structural flexibility.Herein,we report a new Sc and P co-doped perovskite oxide(La0.8Sr0.2Mn0.95Sc0.025P0.025O3-δ,LSMSP)as an active and robust electrocatalyst for the ORR in an alkaline solution.LSMSP electrocatalyst shows superior ORR activity and stability than those of pristine La0.8Sr0.2MnO3-δ(LSM),Sc-doped LSM and P-doped LSM due to the optimized average valence of Mn ions,the large surface area,the smaller particle size and the synergetic effect introduced by the co-doping.Moreover,compared to the benchmark Pt/C electrocatalyst,LSMSP electrocatalyst displays comparable ORR activity and superior durability.These above results suggest that the co-doping strategy of Sc and P into perovskites is a useful method to design high-performance electrocatalysts for the ORR,which can be used in other electrocatalysis-based applications.展开更多
基金supported by the National Key R&D Program of China(2022YFB4004000)National Natural Science Foundation of China(U24A20542,52472210,22279057)+3 种基金Natural Science Foundation of Jiangsu Province(BK20221312)Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX23_1465)Cultivation Program for the Excellent Doctoral Dissertation of Nanjing Tech University(2023-09)the grant of Hydrogen Energy Laboratory(No.FEUZ-2024-0009)。
文摘As global energy demand increases and environmental standards tighten,the development of efficient,eco-friendly energy conversion and storage technologies becomes crucial.Solid oxide cells(SOCs)show great promise because of their high energy conversion efficiency and wide range of applications.Highentropy materials(HEMs),a novel class of materials comprising several principal elements,have attracted significant interest within the materials science and energy sectors.Their distinctive structural features and adaptable functional properties offer immense potential for innovation across various applications.This review systematically covers the basic concepts,crystal structures,element selection,and major synthesis strategies of HEMs,and explores in detail the specific applications of these materials in SOCs,including its potential as air electrodes,fuel electrodes,electrolytes,and interconnects(including barrier coatings).By analyzing existing studies,this review reveals the significant advantages of HEMs in enhancing the performance,anti-poisoning,and stability of SOCs;highlights the key areas and challenges for future research;and looks into possible future directions.
基金Research Institute for Smart Energy(CDB2)the grant from the Research Institute for Advanced Manufacturing(CD8Z)+4 种基金the grant from the Carbon Neutrality Funding Scheme(WZ2R)at The Hong Kong Polytechnic Universitysupport from the Hong Kong Polytechnic University(CD9B,CDBZ and WZ4Q)the National Natural Science Foundation of China(22205187)Shenzhen Municipal Science and Technology Innovation Commission(JCYJ20230807140402006)Start-up Foundation for Introducing Talent of NUIST and Natural Science Foundation of Jiangsu Province of China(BK20230426).
文摘Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe oxide.It is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe oxide.Considering the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.
基金funding from National Science Foundation of China(52202337 and 22178015)the Young Taishan Scholars Program of Shandong Province(tsqn202211082)+1 种基金Natural Science Foundation of Shandong Province(ZR2023MB051)Independent Innovation Research Project of China University of Petroleum(East China)(22CX06023A).
文摘Layer-structured Ruddlesden–Popper(RP)perovskites(RPPs)with decent stability have captured the imagination of the photovoltaic research community and bring hope for boosting the development of perovskite solar cell(PSC)technology.However,two-dimensional(2D)or quasi-2D RP PSCs are encountered with some challenges of the large exciton binding energy,blocked charge transport and poor film quality,which restrict their photovoltaic performance.Fortunately,these issues can be readily resolved by rationally designing spacer cations of RPPs.This review mainly focuses on how to design the molecular structures of organic spacers and aims to endow RPPs with outstanding photovoltaic applications.We firstly elucidated the important roles of organic spacers in impacting crystallization kinetics,charge transporting ability and stability of RPPs.Then we brought three aspects to attention for designing organic spacers.Finally,we presented the specific molecular structure design strategies for organic spacers of RPPs aiming to improve photovoltaic performance of RP PSCs.These proposed strategies in this review will provide new avenues to develop novel organic spacers for RPPs and advance the development of RPP photovoltaic technology for future applications.
基金Funding provided by the National Key R&D Program of China(Grant No.2021YFB3801301)National Natural Science Foundation of China(Grant Nos.22378119,22075076,and 22208092)the Key R&D Plan for Science and Technology in Huai'an City(Industrial Category,HAG202301).
文摘Seawater electrolysis is promising for green hydrogen production, while its application is inhibited by sluggish anodic oxygen evolution reaction (OER) and rapid chloride corrosion‐induced electrode deactivation. Herein, we report a conductive and ion‐ selective OER electrocatalyst with a CoFe alloy core and microporous metal‐doped carbon shell. Co/Fe‐N_(4)‐C active sites in the shell optimize the adsorption strength of intermediates and synergize with the metal core to endow the catalyst with high OER activity and selectivity, while the rich ultra‐micropores in the shell demonstrate a significant sieving effect to hinder Cl− transfer, thus protecting the inner Co/Fe‐N_(4)‐C active sites and metal core from Cl− corrosion. The catalyst is assembled in an alkaline seawater electrolyzer with an electrode geometric area of 254 cm^(2) and delivers a current density of 3000 A m^(-2) at 1.85 V for 330 h. Such catalysts can be synthesized in a large batch (100 g), providing sound opportunities for industrial seawater splitting.
基金supported by the Australian Research Council via Discovery Projects(Nos.DP200103315,DP200103332 and DP230100685)Linkage Projects(No.LP220200920)+1 种基金support from the IONTOF M6 ToF-SIMS(funded by ARC LIEF,LE190100053)the Kratos Axis Ultra XPS(ARC LIEF,LE120100026)。
文摘Ni-rich LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NCM)cathodes in layered oxide cathodes are attractive for high-energy lithium-ion batteries but suffer from rapid capacity fade and thermal instability at high charge voltages.In this study,we propose an entropy-assisted multi-element doping strategy to mitigate these issues.Specifically,two routes are designed and compared:bulk-like localized high-entropy doping(BHE-NCM)and surface-distributed high-entropy-zone doping(SHE-NCM).The surface entropy-doped NCM cathode delivers enhanced electrochemical performance,including higher capacity retention under 4.5 V cycling and superior rate capability,compared to both bulk-like and pristine counterparts.Comprehensive material characterization reveals that surface-localized doping stabilizes the layered structure with reduced microcrack formation and creates a uniform dopant-rich surface region with improved thermal and electrochemical stability.Overall,entropy-assisted doping at the near surface zone effectively alleviates structural degradation and interface reactions in Ni-rich NCM,enabling improved cycling performance at high voltage.This work highlights the significance of surface entropy engineering as a promising strategy for designing high-voltage cathodes with improved safety and longevity.
文摘Microbial fuel cells(MFCs)are promising for realizing wastewater remediation and electricity co-generation,which may significantly promote the formation of an environmentally friendly,clean energy society.Unfortunately,most of the available MFCs show relatively low electricity generation.Anodes,the major component of MFCs,play the most critical role in electron transfer and organic decomposition,which directly determine the performance of MFCs.In the past decades,various carbonaceous materials and carbon-supported conductive composites have been extensively exploited to optimize the electron transfer on the anode due to their versatile properties,such as large surface area and excellent electrical conductivity.The development of anode materials with a particular structure and performance to satisfy field-scale long-term operation of MFCs remains a huge research challenge,which attracts great attention and urgently needs in-depth exploration of the material engineering of anodes for MFCs.In this review,recent advances in the development and optimization of anodes for MFCs are summarized,and applications of MFCs with advanced anodes in the remediation of different types of wastewater are discussed.Advances of anodes for promoting electron transfer,microbial attachment and organic decomposition are the main focuses.The superiorities of MFCs on different aspects of wastewater remediation are elucidated,along with perspectives on future research of MFCs,aiming to provide useful guidance in related fields.
基金The work was supported by National Natural Science Foundation of China(21878158 and 21706129)State Key Laboratory of Clean Energy Utilization(Open Fund Project No.ZJUCEU2021001)Natural Science Foundation of Jiangsu Province(BK20221312).
文摘Reversible proton ceramic electrochemical cell(R-PCEC)is regarded as the most promising energy conversion device,which can realize efficient mutual conversion of electrical and chemical energy and to solve the problem of large-scale energy storage.However,the development of robust electrodes with high catalytic activity is the main bottleneck for the commercialization of R-PCECs.Here,a novel type of high-entropy perovskite oxide consisting of six equimolar metals in the A-site,Pr_(1/6)La_(1/6)Nd_(1/6)Ba_(1/6)Sr_(1/6)Ca_(1/6)CoO_(3−δ)(PLN-BSCC),is reported as a high-performance bifunctional air electrode for R-PCEC.By harnessing the unique functionalities of multiple ele-ments,high-entropy perovskite oxide can be anticipated to accelerate reaction rates in both fuel cell and electrolysis modes.Especially,an R-PCEC utilizing the PLNBSCC air electrode achieves exceptional electrochemical performances,demonstrating a peak power density of 1.21 W cm^(−2)for the fuel cell,while simultaneously obtaining an astonishing current density of−1.95 A cm^(−2)at an electrolysis voltage of 1.3 V and a temperature of 600℃.The significantly enhanced electrochemical performance and durability of the PLNBSCC air electrode is attributed mainly to the high electrons/ions conductivity,fast hydration reactivity and high configurational entropy.This research explores to a new avenue to develop optimally active and stable air electrodes for R-PCECs.
基金supported by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)supported by National R&D Program through the National Research Foundation of Korea(NRF),grant number 2021M3H4A1A01079300the Korea Research Institute of Chemical Technology Core Research Program funded by the Korea Research Council for Industrial Science and Technology,grant number KS2222-10.
文摘Electrochemical water splitting represents one of the most promising technologies to produce green hydrogen,which can help to realize the goal of achieving carbon neutrality.While substantial efforts on a laboratory scale have been made for understanding fundamental catalysis and developing high-performance electrocatalysts for the two half-reactions involved in water electrocatalysis,much less attention has been paid to doing relevant research on a larger scale.For example,few such researches have been done on an industrial scale.Herein,we review the very recent endeavors to bridge the gaps between fundamental research and industrial applications for water electrolysis.We begin by introducing the fundamentals of electrochemical water splitting and then present comparisons of testing protocol,figure of merit,catalyst of interest,and manufacturing cost for laboratory and industry-based water-electrolysis research.Special attention is paid to tracking the surface reconstruction process and identifying real catalytic species under different testing conditions,which highlight the significant distinctions of corresponding electrochemical reconstruction mechanisms.Advances in catalyst designs for industry-relevant water electrolysis are also summarized,which reveal the progress of moving the practical applications forward and accelerating synergies between material science and engineering.Perspectives and challenges of electrocatalyst design strategies are proposed finally to further bridge the gaps between lab-scale research and large-scale electrocatalysis applications.
基金the Theme-based Scheme(project number:T23-601/17-R)from Research Grant Council,University Grants Committee,Hong Kong SAR,China.
文摘Rational construction of carbon-based materials with high-efficiency bifunctionality and low cost as the substitute of precious metal catalyst shows a highly practical value for rechargeable Zn-air batteries(ZABs)yet it still remains challenging.Herein,this study employs a simple mixing-calcination strategy to fabricate a high-performance bifunctional composite catalyst composed of N-doped graphitic carbon encapsulating Co nanoparticles(Co@NrC).Benefiting from the core-shell architectural and compositional advantages of favorable electronic configuration,more exposed active sites,sufficient electric conductivity,rich defects,and excellent charge transport,the optimal Co@NrC hybrid(Co@NrC-0.3)presents outstanding catalytic activity and stability toward oxygen-related electrochemical reactions(oxygen reduction and evolution reactions,i.e.,ORR and OER),with a low potential gap of 0.766 V.Besides,the rechargeable liquid ZAB assembled with this hybrid electrocatalyst delivers a high peak power density of 168 mW cm^(−2),a small initial discharge-charge potential gap of 0.45 V at 10 mA cm^(−2),and a good rate performance.Furthermore,a relatively large power density of 108 mW cm^(−2) is also obtained with the Co@NrC-0.3-based flexible solid-state ZAB,which can well power LED lights.Such work offers insights in developing excellent bifunctional electrocatalysts for both OER and ORR and highlights their potential applications in metal-air batteries and other energy-conversion/storage devices.
基金supported by the Australian Research Council Discovery Projects(DP150104365 and DP160104835)the financial support by the China Scholarship Council(201808340038) for his visiting at Curtin University,Australiathe ARC Discovery Early Career Researcher Award(DE180100773)。
文摘High-temperature solid-state electrolyte is a key component of several important electrochemical devices,such as oxygen sensors for automobile exhaust control,solid oxide fuel cells(SOFCs) for power generation,and solid oxide electrolysis cells for H_(2) production from water electrolysis or CO_(2) electrochemical reduction to value-added chemicals.In particular,internal diffusion of protons or oxygen ions is a fundamental and crucial issue in the research of SOFCs,hypothetically based on either oxygen-ionconducting electrolytes or proton-conducting electrolytes.Up to now,some electrolyte materials based on fluorite or perovskite structure were found to show certain degree of dual-ion transportation capability,while in available electrolyte database,particularly in the field of SOFCs,such dual-ion conductivity was seriously overlooked.Actually,few concerns arising to the simultaneous proton and oxygen-ion conductivities in electrolyte of SOFCs inevitably induce various inadequate and confusing results in literature.Understanding dual-ion transportation behavior in electrolyte is indisputably of great importance to explain some unusual fuel cell performance as reported in literature and enrich the knowledge of solid state ionics.On the other hand,exploration of novel dual-ion conducting electrolytes will benefit the development of SOFCs.In this review,we provide a comprehensive summary of the understanding of dual-ion transportation in solid electrolyte and recent advances of dual-ion conducting SOFCs.The oxygen ion and proton conduction mechanisms at elevated temperature inside oxide-based electrolyte materials are first introduced,and then(mixed) oxygen ion and proton conduction behaviors of fluorite and perovskite-type oxides are discussed.Following on,recent advances in the development of dual-ion conducting SOFCs based on fluorite and perovskite-type single-phase or composite electrolytes,are reviewed.Finally,the challenges in the development of dual-ion conducting SOFCs are discussed and future prospects are proposed.
基金The authors are thankful for the financial support from the Beijing Natural Science Foundation(No.3222050)the National Natural Science Foundation of China(Nos.22075304 and 52202324).
文摘High-entropy oxides(HEOs)are gaining prominence in the field of electrochemistry due to their distinctive structural characteristics,which give rise to their advanced stable and modifiable functional properties.This review presents fundamental preparations,incidental characterizations,and typical structures of HEOs.The prospective applications of HEOs in various electrochemical aspects of electrocatalysis and energy conversion-storage are also summarized,including recent developments and the general trend of HEO structure design in the catalysis containing oxygen evolution reaction(OER)and oxygen reduction reaction(ORR),supercapacitors(SC),lithium-ion batteries(LIBs),solid oxide fuel cells(SOFCs),and so forth.Moreover,this review notes some apparent challenges and multiple opportunities for the use of HEOs in the wide field of energy to further guide the development of practical applications.The influence of entropy is significant,and high-entropy oxides are expected to drive the improvement of energy science and technology in the near future.
基金This study was supported by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
文摘Molybdenum carbide(MoxC)with variable phase structure possesses flexible hydrogen-binding energy(HBE),which is a promising hydrogen evolution reaction(HER)catalyst.Herein,a hybrid multiphase MoxC freestanding film coupled with Co3Mo(CM/MoxC@NC)is synthesized through the electrospinning method supplemented by the heteroatom incorporation.CM/MoxC@NC surpasses its pure phase counterparts and exhibits remarkable catalytic activity at 114mV to deliver a current density of 10mA cm^(−2) in acid,which is among the first-rate level performance reported for MoxC-based catalysts.The subsequent ex situ and in situ characterizations reveal a phase transition mechanism based on self-catalysis that CoOx depletes the coordinated C ofα-MoC via the interaction,which realizes the assembly of weak HBEα-MoC and strong HBEβ-Mo2C,and the enhanced utilization of active materials as well.The multiple structures with optimal HBE are in favor of the stepwise reactions of HER,as the study of the correlation between HBE and phase structure revealed.This study discloses the underlying phase transition mechanism and highlights the HBE–structure relationship that should be considered for catalyst design.
基金University of Macao,Grant/Award Numbers:MYRG2018-00192-IAPME,MYRG2020-00187-IAPMEScience and Technology Development Fund,Macao SAR,Grant/Award Numbers:0021/2019/AIR,0041/2019/A1,0046/2019/AFJ,0191/2017/A3UEA funding。
文摘Simultaneously enhancing the reaction kinetics,mass transport,and gas release during alkaline hydrogen evolution reaction(HER)is critical to minimizing the reaction polarization resistance,but remains a big challenge.Through rational design of a hierarchical multiheterogeneous three-dimensionally(3D)ordered macroporous Mo_(2)C-embedded nitrogen-doped carbon with ultrafine Ru nanoclusters anchored on its surface(OMS Mo_(2)C/NC-Ru),we realize both electronic and morphologic engineering of the catalyst to maximize the electrocatalysis performance.The formed Ru-NC heterostructure shows regulative electronic states and optimized adsorption energy with the intermediate H*,and the Mo_(2)C-NC heterostructure accelerates the Volmer reaction due to the strong water dissociation ability as confirmed by theoretical calculations.Consequently,superior HER activity in alkaline solution with an extremely low overpotential of 15.5 mV at 10 mAcm^(−2)with the mass activity more than 17 times higher than that of the benchmark Pt/C,an ultrasmall Tafel slope of 22.7 mV dec−1,and excellent electrocatalytic durability were achieved,attributing to the enhanced mass transport and favorable gas release process endowed from the unique OMS Mo_(2)C/NC-Ru structure.By oxidizing OMS Mo_(2)C/NC-Ru into OMS MoO_(3)-RuO_(2)catalyst,it can also be applied as efficient oxygen evolution electrocatalyst,enabling the construction of a quasi-symmetric electrolyzer for overall water splitting.Such a device's performance surpassed the state-of-the-art Pt/C||RuO2 electrolyzer.This study provides instructive guidance for designing 3D-ordered macroporous multicomponent catalysts for efficient catalytic applications.
基金financially supported by the National Natural Science Foundation of China(Nos.22108121,21908106 and21878158)Jiangsu Natural Science Foundation(No.BK20190682)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
文摘Fuel flexibility is one of the most distinguished advantages of solid oxide fuel cells(SOFCs)over other low-temperature fuel cells.Furthermore,the combination of ammonia fuel and SOFCs technology should be a promising clean energy system after considering the high energy density,easy transportation/storage,matured synthesis technology and carbon-free nature of NH_(3) as well as high efficiency of SOFCs.However,the large-scale applications of direct-ammonia SOFCs(DASOFCs)are strongly limited by the inferior anti-sintering capability and catalytic activity for ammonia decomposition reaction of conventional nickel-based cermet anode.Herein,a slightly ruthenium(Ru)doping in perovskite oxides is proposed to promote the alloy nanoparticle exsolution,enabling better DA-SOFCs with enhanced power outputs and operational stability.After treating Ru-doped Pr_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.75)Ru_(0.05)O_(3-δ) single-phase perovskite in a reducing atmosphere,in addition to the formation of two layered Ruddlesden-Popper perovskites and Pr_(2)O_(3) nanoparticles(the same as the Ru-free counterpart,Pr_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3-δ)),the exsolution of CoFeRu-based alloy nanoparticles is remarkably promoted.Such reduced Pr_(0.6)Sr0.4Co_(0.2)Fe_(0.75)Ru_(0.05)O_(3-δ) composite anode shows superior catalytic activity and stability for NH_(3) decomposition reaction as well as anti-sintering capability in DA-SOFCs to those of reduced Pr0.6Sr0.4Co0.2Fe0.8O_(3-δ)due to the facilitated nanoparticle exsolution and stronger nanoparticle/substrate interaction.This work provides a facile and effective strategy to design highly active and durable anodes for DA-SOFCs,promoting large-scale applications of this technology.
基金This study was funded by the Science and Technology Development Fund,Macao SAR(File no.0191/2017/A3,0041/2019/A1,0046/2019/AFJ,0021/2019/AIR)the University of Macao(File no.MYRG2017-00216-FST and MYRG2018-00192-IAPME)+2 种基金the UEA funding,Science and Technology Program of Guangzhou(2019050001)the National Key Research and Development Program of China(2019YFE0198000)Fuming Chen acknowledges the Pearl River Talent Program(2019QN01L951).
文摘Aluminum-metal batteries show great potential as next-generation energy storage due to their abundant resources and intrinsic safety.However,the crucial limitations of metallic Al anodes,such as dendrite and corrosion problems in conventional aluminum-metal batteries,remain challenging and elusive.Here,we report a novel electrodeposition strategy to prepare an optimized 3D Al anode on carbon cloth with an uniform deposition morphology,low local current density,and mitigatory volume change.The symmetrical cells with the 3D Al anode show superior stable cycling(>450 h)and low-voltage hysteresis(~170 mV)at 0.5 mA cm^(−2).High reversibility(~99.7%)is achieved for the Al plating/stripping.The graphite||Al‐4/CC full batteries show a long lifespan of 800 cycles with 54 mAh g^(−1) capacity at a high current density of 1000 mA g^(−1),benefiting from the high capacitive-controlled distribution.This study proposes a novel strategy to design 3D Al anodes for metallic-Al-based batteries by eliminating the problems of planar Al anodes and realizing the potential applications of aluminum-graphite batteries.
基金the support provided by the“Australian Government Research Training Program(RTP)Scholarship”at Curtin University,Perth,Australia。
文摘The development of bi-functional electrocatalyst with high catalytic activity and stable performance for both oxygen evolution/reduction reactions(OER/ORR)in aqueous alkaline solution is key to realize practical application of zinc-air batteries(ZABs).In this study,we reported a new porous nano-micro-composite as a bifunctional electrocatalyst for ZABs,devised by the in situ growth of metal-organic framework(MOF)nanocrystals onto the micrometersized Ba0.5Sr0.5Co0.8Fe0.2O3(BSCF)perovskite oxide.Upon carbonization,MOF was converted to porous nitrogen-doped carbon nanocages and ultrafine cobalt oxides and CoN4 nanoparticles dispersing inside the carbon nanocages,which further anchored on the surface of BSCF oxide.We homogeneously dispersed BSCF perovskite particles in the surfactant;subsequently,ZIF-67 nanocrystals were grown onto the BSCF particles.In this way,leaching of metallic or organic species in MOFs and the aggregation of BSCF were effectively suppressed,thus maximizing the number of active sites for improving OER.The BSCF in turn acted as catalyst to promote the graphitization of carbon during pyrolysis,as well as to optimize the transition metal-tocarbon ratio,thus enhancing the ORR catalytic activity.A ZAB fabricated from such air electrode showed outstanding performance with a potential gap of only 0.83 V at 5 mA cm-2 for OER/ORR.Notably,no obvious performance degradation was observed for the continuous charge-discharge operation for 1800 cycles over an extended period of 300 h.
基金financially supported by the State Key Laboratory of Clean Energy Utilization(Open Fund Project No.ZJUCEU2021001)Natural Science Foundation of Jiangsu Province(No.BK20221312).
文摘Electrochemical conversion of CO_(2)to CO is an economically feasible method for mitigating greenhouse gas emissions.Among various electrochemical approaches,solid oxide electrolysis cells(SOECs)show high potential for CO_(2)reduction reaction(CO_(2)-RR)due to their ability to operate at high temperatures,resulting in fast reaction kinetics and increased efficiency.Considering their main energy loss is still associated with the large overpotential at the fuel electrode,the development of the highly efficient and durable cathode for SOECs has been extensively searched after.Here,we propose an A-site doping strategy to enhance the properties of Sr_(2)Fe_(1.5)Mo_(0.5)O_(6−δ)(SFM),which improve its performance as a cathode in SOECs for CO_(2)-RR,demonstrating favorable activity and durability.The structural and physiochemical characterizations,together with DFT calculations,show that the partial replacement of Sr by Bi in the SFM double perovskite not only improves CO_(2) adsorption capability at the catalyst surface but also enhances oxygen ionic conduction inside the bulk oxide,resulting in enhanced CO_(2)electrocatalysis performance in SOECs.Specifically,a La_(0.8)Sr_(0.2)Ga_(0.8)Mg_(0.2)O_(3−δ) (LSGM)electrolyte-supported single cell with the new Bi-doped SFM cathode demonstrates a large current density of 1620 mA cm^(−2) at a cell potential of 1.6 V at 850°C with good operational stability up to 200 h.Bi-doped SFM thus represents a highly promising cathode for ceramic CO_(2)electrolyzers and could accelerate our transition towards a carbon-neutral society.
基金financially supported by the Australian Research Council (Discovery Early Career Researcher Award No. DE190100005)the support of the Australian Research Council (Grant No. FT160100207)the ontinued support from the Queensland University of Technology (QUT) through the centre for Materials Science。
文摘The oxygen evolution reaction(OER) plays a crucial role in many electrochemical energy technologies,and creating multiple beneficial factors for OER catalysis is desirable for achieving high catalytic efficiency.Here,we highlight a new halogen-chlorine(Cl)-anion doping strategy to boost the OER activity of perovskite oxides.As a proof-of-concept,proper Cl doping at the oxygen site of LaFeO3(LFO) perovskite can induce multiple favorable characteristics for catalyzing the OER,including rich oxygen vacancies,increased electrical conductivity and enhanced Fe-O covalency.Benefiting from these factors,the LaFeO2.9-δCl0.1(LFOCl) perovskite displays significant intrinsic activity enhancement by a factor of around three relative to its parent LFO.This work uncovers the effect of Cl-anion doping in perovskites on promoting OER performance and paves a new way to design highly efficient electrocatalysts.
基金Natural Science Foundation of Jiangsu forthe Outstanding Youth Fund,Grant/Award Number:BK20211590National Natural Science Foundation ofChina,Grant/Award Number:51802152。
文摘Before the practical application of rechargeable Zn-air batteries(ZABs),a critical issue regarding the inherent slow reaction kinetics of the oxygen reduction(ORR)and oxygen evolution(OER)must be addressed.Here,we fabricate a cost-effective bifunctional oxygen electrocatalyst with a self-antistacking structure,where three-dimensional(3D)Fe-Co bimetallic oxide particles(FeCoO_(x))are directly grown on 2D N-doped graphene(NG).The in situ grown FeCoO_(x)particles can alleviate the NG interlaminar restacking,ensuring abundant channels for diffusion of O_(2)/OH−species,while the NG allows rapid electron flow.Benefiting from this self-antistacking 3D-on-2D structure and synergetic electrocatalysis,FeCoO_(x)@NG demonstrated excellent activity for both ORR and OER(ΔE=0.78 V),which is superior to that of the binary mixtures of Pt/C and RuO_(2)(ΔE=0.83 V).A homemade ZAB with 20%-FeCoO_(x)@NG delivers a specific capacity of 758.9 mAh g^(−1),a peak power density of 215 mW cm^(−2),and long-term cyclability for over 400 h.These research results suggest that designing a bimetallic oxide/N-doped carbon 3D-on-2D nanoarchitecture using an in situ growth strategy is an attractive and feasible solution to overcome electrocatalytic problems in ZABs.
基金financially supported by the National Natural Science Foundation of China(Nos.21576135 and 21706129)the Youth Fund of Jiangsu Province(No.BK20150945)+2 种基金Program for Jiangsu Specially-Appointed Professorsthe Funding from State Key Laboratory of Materials-Oriented Chemical Engineering(No.ZK201808)the financial support of the Australian Research Council.
文摘The requirement for a sustainable and renewable energy has inspired substantial interests in designing and developing earth-abundant and high-effectiveness electrocatalysts/electrodes for fuel cells and metal-air batteries,in which oxygen reduction reaction(ORR)plays a crucial role.Perovskite oxides have acquired rapid attention as ORR electrocatalysts to replace noble-metal-based catalysts owing to their intrinsic electrocatalytic activity,compositional and structural flexibility.Herein,we report a new Sc and P co-doped perovskite oxide(La0.8Sr0.2Mn0.95Sc0.025P0.025O3-δ,LSMSP)as an active and robust electrocatalyst for the ORR in an alkaline solution.LSMSP electrocatalyst shows superior ORR activity and stability than those of pristine La0.8Sr0.2MnO3-δ(LSM),Sc-doped LSM and P-doped LSM due to the optimized average valence of Mn ions,the large surface area,the smaller particle size and the synergetic effect introduced by the co-doping.Moreover,compared to the benchmark Pt/C electrocatalyst,LSMSP electrocatalyst displays comparable ORR activity and superior durability.These above results suggest that the co-doping strategy of Sc and P into perovskites is a useful method to design high-performance electrocatalysts for the ORR,which can be used in other electrocatalysis-based applications.
