Proton ceramic fuel cell efficiently converts chemical energy into electrical energy,representing a pivotal component of future energy systems.However,its current performance is hindered by limitations in cathode and ...Proton ceramic fuel cell efficiently converts chemical energy into electrical energy,representing a pivotal component of future energy systems.However,its current performance is hindered by limitations in cathode and electrolyte materials,thereby impeding commercialization.Anion doping emerges as a promising strategy to enhance the electrochemical efficiency of perovskite-based cathodes and electrolytes.However,integrating this approach within a single-cell structure still requires further research.In this study,F-doped perovskite oxides BaCo_(0.4)Fe_(0.4)Zr_(0.1)Y_(0.1)O_(2.9-δ)F_(0.1)(BCFZYF)and BaZr_(0.1)Ce_(0.7)Y_(0.1)Yb_(0.1)O_(2.9-δ)F_(0.1)(BZCYYbF)were synthesized for use as the cathode and electrolyte,respectively,in proton ceramic fuel cells.Our findings demonstrate that F-doped perovskite oxides exhibit superior electrochemical performance and enhanced structural stability.Furthermore,doping both electrodes and electrolytes with F ions improves their interfacial compatibility.The cell configuration BCFZYF|BZCYYbF|Ni-BZCYYbF achieved a peak power density of 998 mW·cm^(−2)at 650℃using H_(2)as fuel,and it maintained stable operation for over 400 h at 550℃with a current density of 400 mA·cm^(−2).This research underscores an effective strategy for enhancing the performance and durability of proton ceramic fuel cells.展开更多
The electrochemical nitrogen reduction reaction(NRR)under ambient conditions presents a promising approach for the eco-friendly and sustainable synthesis of ammonia,with a continuous emergence of potential electrocata...The electrochemical nitrogen reduction reaction(NRR)under ambient conditions presents a promising approach for the eco-friendly and sustainable synthesis of ammonia,with a continuous emergence of potential electrocatalysts.However,the low solubility and limited diffusion of N_(2)significantly hinder the achievement of satisfactory performance.In this context,we report an effective strategy to enhance NRR activity by introducing a metal-organic framework(MOF)membrane,specifically MIL-53(Al),onto a perovskite oxide(LiNbO_(3)),denoted as LN@MIL-X(X=0.2,0.4 and 0.6).The MIL-53(Al)membrane selectively recognizes and concentrates N_(2)at the catalyst interface while simultaneously repelling water molecules,thereby inhibiting the hydrogen evolution reaction(HER).This ultrathin nanostructure significantly improves the NRR performance of LN@MIL-X compared to pristine LiNbO_(3).Notably,LN@MIL-0.4 exhibits a maximum NH_(3)yield of 45.25 mg h^(-1)mg_(cat.)^(-1)with an impressive Faradaic efficiency(FE)of 86.41%at-0.45 V versus RHE in 0.1 mol L^(-1)Na_(2)SO_(4).This work provides a universal strategy for the design and synthesis of perovskite oxide electrocatalysts,facilitating high-efficiency ammonia synthesis.展开更多
Proton exchange membrane water electrolyzer(PEMWE)represents a highly promising technology for renewable hydrogen generation,urgently demanding low-cost,efficient,and robust anode oxygen evolution reaction(OER)electro...Proton exchange membrane water electrolyzer(PEMWE)represents a highly promising technology for renewable hydrogen generation,urgently demanding low-cost,efficient,and robust anode oxygen evolution reaction(OER)electrocatalysts in acidic media.Over the past decade(mainly from 2016 onwards),low-Ir/Ru perovskite oxides have emerged as promising candidate materials for acidic OER electrocatalysis owing to their flexible element compositions and crystal structures,which can evidently reduce the noble-metal content and meanwhile significantly promote electrocatalytic performance.In this review,the current research progress in low-Ir/Ru perovskite oxides for acidic OER electrocatalysis is comprehensively summarized.Initially,we present a brief introduction to general issues relevant to acidic OER catalyzed by low-Ir/Ru perovskite oxides,such as the actual active species,OER mechanisms,inverse activity-stability relationship,and performance evaluation metrics.Subsequently,we present a thorough overview of various low-Ir/Ru perovskite oxides for acidic OER electrocatalysis,including single perovskites,double perovskites,triple perovskites,quadruple perovskites,Ruddlesden-Popper perovskites,and other complex perovskite-derived oxides,with emphasis on the intrinsic factors contributing to their exceptional performance and structure-property-performance correlation.Finally,remaining challenges and some promising insights to inspire future studies in this exciting field are provided.展开更多
Crystalline perovskite oxides are regarded as promising electrocatalysts for water electrolysis,particularly for anodic oxygen evolution reactions,owing to their low cost and high intrinsic activity.Perovskite oxides ...Crystalline perovskite oxides are regarded as promising electrocatalysts for water electrolysis,particularly for anodic oxygen evolution reactions,owing to their low cost and high intrinsic activity.Perovskite oxides with noncrystalline or amorphous characteristics also exhibit promising electrocatalytic performance toward electrochemical water splitting.In this review,a fundamental understanding of the characteristics and advantages of crystalline,noncrystalline,and amorphous perovskite oxides is presented.Subsequently,recent progress in the development of advanced electrocatalysts for water electrolysis by engineering and breaking the crystallinity of perovskite oxides is reviewed,with a special focus on the underlying structure–activity relationships.Finally,the remaining challenges and unsolved issues are presented,and an outlook is briefly proposed for the future exploration of next-generation water-splitting electrocatalysts based on perovskite oxides.展开更多
Supported nanoparticles have attracted considerable attention as a promising catalyst for achieving unique properties in numerous applications,including fuel cells,chemical conversion,and batteries.Nanocatalysts demon...Supported nanoparticles have attracted considerable attention as a promising catalyst for achieving unique properties in numerous applications,including fuel cells,chemical conversion,and batteries.Nanocatalysts demonstrate high activity by expanding the number of active sites,but they also intensify deactivation issues,such as agglomeration and poisoning,simultaneously.Exsolution for bottomup synthesis of supported nanoparticles has emerged as a breakthrough technique to overcome limitations associated with conventional nanomaterials.Nanoparticles are uniformly exsolved from perovskite oxide supports and socketed into the oxide support by a one-step reduction process.Their uniformity and stability,resulting from the socketed structure,play a crucial role in the development of novel nanocatalysts.Recently,tremendous research efforts have been dedicated to further controlling exsolution particles.To effectively address exsolution at a more precise level,understanding the underlying mechanism is essential.This review presents a comprehensive overview of the exsolution mechanism,with a focus on its driving force,processes,properties,and synergetic strategies,as well as new pathways for optimizing nanocatalysts in diverse applications.展开更多
In this paper, the partial oxidation of methane to synthesis gas using lattice oxygen of La1- SrxMO3-λ (M=Fe, x ...In this paper, the partial oxidation of methane to synthesis gas using lattice oxygen of La1- SrxMO3-λ (M=Fe, x Mn) perovskite oxides instead of molecular oxygen was investigated. The redox circulation between 11% O2/Ar flow and 11% CH4/He flow at 900℃ shows that methane can be oxidized to CO and H2 with a selectivity of over 90.7% using the lattice oxygen of La1- SrxFeO3-λ (x≤0.2) perovskite oxides in an appropriate reaction condition, while the lost lattice x oxygen can be supplemented by air re-oxidation. It is viable for the lattice oxygen of La1- SrxFeO3-λ (x≤0.2) perovskite x oxides instead of molecular oxygen to react with methane to synthesis gas in the redox mode.展开更多
Magnesia modified LaCoO3 was prepared by a facile one-step sol-gel method and used for removal of dilute methane.Compared with the conventional doping technique,the obtained LaCoO3@MgO-x exhibits pseudo core-shell str...Magnesia modified LaCoO3 was prepared by a facile one-step sol-gel method and used for removal of dilute methane.Compared with the conventional doping technique,the obtained LaCoO3@MgO-x exhibits pseudo core-shell structure and shows superior catalytic activity.The methane conversion exceeds90%at 532℃on LaCoO3@MgO-0.1,while only 60%of methane is conversed using the doped perovskite LaCo0.9Mg0.1O3.The high catalytic performance of LaCoO3@MgO-0.1 is mainly attributed to the adjustment of surface acid-base properties by the MgO shell structure.According to density functional theory(DFT)calculation,the methane is more likely to be adsorbed and cracked on LaCoO3@MgO-0.1.The in situ DRIFTS shows that CH3-O-CH3 intermediate specie is formed.The pseudo core-shell structure also enhances the stability and the LaCoO3@MgO-0.1 maintains high activity after working for 100 h.The above results demonstrate that surface modification by magnesia is an effective strategy for improving LaCoO3 catalytic performance.展开更多
Comparison of LaFeO3, La0.8Sr0.2FeO3, and La0.8Sr0.2Fe0.9CO0.1O3 perovskite oxides as oxygen carrier for partial oxidation of methane in the absence of gaseous oxygen was investigated by continuous flow reaction and s...Comparison of LaFeO3, La0.8Sr0.2FeO3, and La0.8Sr0.2Fe0.9CO0.1O3 perovskite oxides as oxygen carrier for partial oxidation of methane in the absence of gaseous oxygen was investigated by continuous flow reaction and sequential redox reaction, Methane was oxidized to syngas with high selectivity by oxygen species of perovskite oxides in the absence of gaseous oxygen. The sequential redox reaction revealed that the structural stability and continuous oxygen supply in redox reaction decreased over La0.8Sr0.2Fe0.9Co0. 1O3 oxide, while LaFeO3 and La0.8Sr0.2FeO3 exhibited excellent structural stability and continuous oxygen supply.展开更多
The oxygen evolution reaction (OER) dominates the efficiency of electrocatalytic water splitting owing to its sluggish kinetics.Perovskite oxides (ABO_(3)) have emerged as promising candidates to accelerate the OER pr...The oxygen evolution reaction (OER) dominates the efficiency of electrocatalytic water splitting owing to its sluggish kinetics.Perovskite oxides (ABO_(3)) have emerged as promising candidates to accelerate the OER process owing to their high intrinsic activities and tailorable properties.Fe ions in perovskite oxides have been proved to be a highly catalytic element for OER,while some Fe-based perovskites such as SrTi_(0.8)Fe_(0.2)O_(3-δ)(STF) and La_(0.66)Ti_(0.8)Fe_(0.2)O_(3-δ)(LTF) exhibit inferior OER activity.Yet the essential reason is still unclear and the effective method to promote the activity of such perovskite is also lacking.Herein,an in-situ exsolution strategy was proposed to boost the OER by migrating Fe from the bulk to the surface.Significantly enhanced OER activity was achieved on STF and LTF perovskites with surfacedecorated oxygen vacancies and Fe nanoparticles.In addition,theoretical calculation confirmed that the oxygen vacancies and Fe nanoparticle on surface could lower the overpotential of OER by facilitating the adsorption of OH^(-).From this study,migration of the active elements in perovskite is found to be an effective strategy to increase the quantity and activity of active sites,providing new insights and understanding for designing efficient OER catalysts.展开更多
Solid oxide electrolysis cell(SOEC) could be a potential technology to afford chemical storage of renewable electricity by converting water and carbon dioxide.In this work,we present the Ni-doped layered perovskite ox...Solid oxide electrolysis cell(SOEC) could be a potential technology to afford chemical storage of renewable electricity by converting water and carbon dioxide.In this work,we present the Ni-doped layered perovskite oxides,(La_(4)Sr_(n-4))_(0.9)Ti_(0.9n)Ni_(0.1n)O_(3n+2) with n=5,8,and 12(LSTNn) for application as catalysts of CO_(2) electrolysis with the exsolution of Ni nanoparticles through a simple in-situ growth method.It is found that the density,size,and distribution of exsolved Ni nanoparticles are determined by the number of n in LSTNn due to the different stack structures of TiO_6 octahedra along the c axis.The Ni doping in LSTNn significantly improved the electrochemical activity by increasing oxygen vacancies,and the Ni metallic nanoparticles afford much more active sites.The results show that LSTNn cathodes can successfully be manipulated the activity by controlling both the n number and Ni exsolution.Among these LSTNn(n=5,8,and 12),LSTN8 renders a higher activity for electrolysis of CO_(2) with a current density of 1.50A cm^(-2)@2.0 V at 800℃ It is clear from these results that the number of n in(La_(4)Sr_(n-4))_(0.9)Ti_(0.9n)Ni_(0.1n)O_(3n+2)with Ni-doping is a key factor in controlling the electrochemical performance and catalytic activity in SOEC.展开更多
Volatile organic compounds are a kind of important indoor and outdoor air pollutants.In recent years,more and more attention has been paid to the ways of volatile organic compound elimination because of its potential ...Volatile organic compounds are a kind of important indoor and outdoor air pollutants.In recent years,more and more attention has been paid to the ways of volatile organic compound elimination because of its potential long-term effects on human health.Among the various available methods for volatile organic compound elimination,the catalytic combustion is the most attractive method due to its high efficiency,low cost,simple operation,and easy scale-up.Perovskite oxides,as a large family of metal oxides with their A-site mainly of lanthanide element and/or alkaline earth metal element and B-site of transition metal element,have been extensively investigated as active and stable catalysts for volatile organic compound removal reactions due to their abundant compositional elements,high thermal/chemical stability,and compositional/structural flexibility.The catalytic performance of perovskite oxides is strongly depended on its material composition,morphology,and surface/bulk properties,while the doping,tailored synthesis route,and composite construction may have a significant effect on the bulk(oxygen vacancy concentration,lattice structure),surface(oxygen species,defect)properties,and particulate morphology,consequently the catalytic activity and stability for volatile organic compound removal.Herein,a comprehensive review about the recent advances in perovskite oxides for volatile organic compound elimination reactions based on catalytic combustion is presented from different aspects with a special emphasis on the material design strategies,such as compositional tuning,morphology control,nanostructure building,hybrid construction,and surface modification.At last,some perspectives are presented on the development and design of perovskite oxide-based catalysts for volatile organic compound removal applications by highlighgting the critical issues and challenges.展开更多
The benefits of perovskite oxides include their low cost,customizable composition,ordered atomic structure,and extremely flexible electronic structure.They are the ideal substitute for precious metal catalysts in vari...The benefits of perovskite oxides include their low cost,customizable composition,ordered atomic structure,and extremely flexible electronic structure.They are the ideal substitute for precious metal catalysts in various electrocatalytic reactions.However,the initial activity of perovskite oxides is often quite limited,which is extremely related to their crystal structure and electronic structure.In this regard,component regulation is the simplest and most effective strategy to increase their stability and catalytic activity.In this review,we briefly outline the recent progress in the modulating component of perovskite oxides to enhance their catalytic properties.The outline was categorized according to the sites in the ABO3-type perovskite structure,including A-site,B-site,and O-site regulation.Finally,potential research directions aimed at modulating of perovskite oxide constituents are discussed.展开更多
Heterogeneous catalytic combustion provides a feasible technique for high efficient methane utilization.Perovskites ABO_3-type materials have received renewed attention as a potential alternative for noble metals supp...Heterogeneous catalytic combustion provides a feasible technique for high efficient methane utilization.Perovskites ABO_3-type materials have received renewed attention as a potential alternative for noble metals supported catalysts in catalytic methane combustion due to excellent hydrothermal stability and sulfur resistance. Recently, the emergence of nanostructured perovskite oxides（such as threedimensional ordered nanostructure, nano-array structure） with outstanding catalytic activity has further driven methane catalytic combustion research into spotlight. In this review, we summarize the recent development of nanostructured perovskite oxide catalysts for methane combustion, and shed some light on the rational design of high efficient nanostructured perovskite catalysts via lattice oxygen activation,lattice oxygen mobility and materials morphology engineering. The emergent issues needed to be addressed on perovskite catalysts were also proposed.展开更多
The magnetic functional materials play a particularly important role in our modern society and daily life.The magnetocaloric effect(MCE)is at the basis of a solid state magnetic refrigeration(MR)technology which may e...The magnetic functional materials play a particularly important role in our modern society and daily life.The magnetocaloric effect(MCE)is at the basis of a solid state magnetic refrigeration(MR)technology which may enhance the efficiency of cooling systems,both for room temperature and cryogenic appli-cations.Despite numerous experimental and theoretical MCE studies,commercial MR systems are still at developing stage.Designing magnetic solids with outstanding magnetocaloric performances remains therefore a most urgent task.Herein,recent progresses on characterizing the crystal structure,magnetic properties and cryogenic MCE of rare earths(RE)-based RE_(2)TMTM’O_(6)double perovskite(DP)oxides,where TM and TM’are different 3d transition metals,are summarized.Some Gd-based DP oxides are found to exhibit promising cryogenic magnetocaloric performances which make them attractive for active MR ap-plications.展开更多
CONSPECTUS:Ultraviolet(UV)light,spanning wavelengths from 10 to 400 nm,is ubiquitous in military,livelihood,and scientific domains.Accurate UV photodetection is therefore essential for monitoring environmental radiati...CONSPECTUS:Ultraviolet(UV)light,spanning wavelengths from 10 to 400 nm,is ubiquitous in military,livelihood,and scientific domains.Accurate UV photodetection is therefore essential for monitoring environmental radiation,safeguarding human health,and advancing technological applications in fields such as aerospace,medical science,and ecology.The fabrication of high-performance UV photodetection devices fundamentally depends on the development of high-sensitivity UV photosensitive materials.The evolution of UV photodetection materials has progressed from early wide-bandgap semiconductors like ZnS and ZnSe to third-generation semiconductors such as GaN and Ga_(2)O_(3),and most recently to two-dimensional(2D)wide-bandgap materials that combine exceptional optoelectronic properties with compelling physicochemical properties.Among these,2D perovskite oxides stand out due to their prominent advantages for UV detection.First,this large family of materials generally features wide bandgaps,strong UV absorption,and high spectral selectivity.Second,the tunable bandgaps of 2D perovskite oxides enable precise detection at specific wavelengths.Third,their excellent processability and flexibility facilitate feasible integration into devices,making them promising candidates for flexible photodetectors.Furthermore,2D perovskite oxides boast other properties such as high stability,dielectricity,ferroelectricity,and biocompatibility.These characteristics have promoted the blossoming of 2D perovskite oxides for highperformance UV photodetection and are poised to expand their applications in novel functional optoelectronics.In this Account,we systematically review the development of 2D perovskite oxides,with a focus on their application in the fabrication of high-performance UV photodetectors.First,we describe the top-down synthesis of these materials,highlighting key advances in synthesis techniques.Second,we specifically analyze the intrinsic advantages of 2D perovskite oxides which render them highly suitable for UV detection.Third,we discuss recent progress in the fabrication of UV photodetectors based on 2D perovskite oxides,emphasizing effective strategies for achieving high-performance devices.Next,we explore state-of-the-art optoelectronic applications leveraging these materials.Finally,we present our perspectives on the future development of this promising class of UVsensitive materials.Given their remarkable material diversity,we believe that this Account will provide valuable insights to guide future research and the application of 2D perovskite oxides in high-performance UV photodetectors and functional optoelectronics.展开更多
The interpretability of machine learning reveals associations between input features and predicted physical properties in models,which are essential for discovering new materials.However,previous works were mainly dev...The interpretability of machine learning reveals associations between input features and predicted physical properties in models,which are essential for discovering new materials.However,previous works were mainly devoted to algorithm improvement,while the essential multi-scale characteristics are not well addressed.This paper introduces distortion modes of oxygen octahedrons as cross-scale structural features to bridge chemical compositions and material properties.Combining modelagnostic interpretation methods,we are able to achieve interpretability even using simple machine learning schemes and develop a predictive model of effective mass for a widely used material type,namely perovskite oxides.With this framework,we reach the interpretability of the model,understanding the trend of the effective mass without any prior background information.Moreover,we obtained the knowledge only available to experts,i.e.,the interpretation of effective mass from the sep orbitals hybridization of B-site cations and O^(2-)in ABO_(3)perovskite oxides.展开更多
Porous perovskite metal oxides(PPMOs)have emerged as promising candidates for efficient catalysts in fine chemical engineering due to their flexible crystal structures and tunable surface chemical properties.However,t...Porous perovskite metal oxides(PPMOs)have emerged as promising candidates for efficient catalysts in fine chemical engineering due to their flexible crystal structures and tunable surface chemical properties.However,the conventional high temperature calcination process required for crystallization frequently leads to collapse of pore structure,limiting the practical application of PPMOs.Herein,we propose a facile and general polymer derived bubble templates strategy to synthesize a series of PPMOs,including single-component PPMOs(e.g.,LaMnO_(3),LaFeO_(3),LaCoO_(3),PrMnO_(3),and NdMnO_(3))and multiple-component PPMOs(e.g.,LaCo_(x)Mn_(1-x)O_(3)(x=0.1,0.2,and 0.3))with tunable pore structure.The pore architectures(macropores,hierarchically meso/macropores,and mesopores),pore sizes,and specific surface areas(14-40 m^(2)·g^(-1))of the samples can be precisely tailored by adjusting the sizes of bubble templates.The hierarchically meso/macroporous LaMnO_(3)features multiple structural advantages,including well-defined hierarchical porous architecture,high specific surface area,and abundant oxygen vacancies,and exhibits a remarkable catalytic performance in oxidation of benzyl alcohol to benzaldehyde,with conversion and selectivity of 99%and 99%,respectively.This work not only provides a scalable and versatile pathway for fabricating advanced porous materials but also offers new perspectives for their application in diverse catalytic processes.展开更多
It is urgent to develop novel energy storage and conversion systems to address the pressing issues of the energy crisis and environmental pollution,including alkaline water electrolysis,alkaline fuel cells and metal-a...It is urgent to develop novel energy storage and conversion systems to address the pressing issues of the energy crisis and environmental pollution,including alkaline water electrolysis,alkaline fuel cells and metal-air batteries.However,these systems are hampered by the sluggish kinetics of the oxygen evolution reaction(OER)or oxygen reduction reaction(ORR).One of the most effective strategies to overcome this challenge is the development of efficient and stable catalysts for both ORR and OER,which typically consist of Pt,Ir,or other precious metals.Unfortunately,most precious metal catalysts are limited to single catalytic activity(either ORR or OER)and are constrained by the high cost and scarcity of noble metals.Perovskite oxides offer significant promise as efficient bifunctional ORR/OER catalysts due to their high catalytic activity,versatile composition,low cost,and high stability in alkaline environments.The general preparation methods of perovskite-type oxides are summarized in this work.Then recent mechanistic studies on the ORR and OER of perovskite oxides are also discussed,particularly highlighting the theoretical and experimental methods employed to facilitate these studies.Further strategies for improving the catalytic performance of perovskite oxides are discussed from five perspectives.The perspective of challenges and future directions for the development of perovskite oxides in ORR and OER applications are finally presented.展开更多
All-solid-state batteries equipped with solid-state electrolytes(SSEs)havegained significant interest due to their enhanced safety,energy density,andlongevity in comparison to traditional liquid organic electrolyte-ba...All-solid-state batteries equipped with solid-state electrolytes(SSEs)havegained significant interest due to their enhanced safety,energy density,andlongevity in comparison to traditional liquid organic electrolyte-based batteries.However,many SSEs,such as sulfides and hydrides,are highly sensitiveto water,limiting their practical use.As one class of important perovskites,theRuddlesden–Popper perovskite oxides(RPPOs),show great promise as SSEsdue to their exceptional stability,particularly in terms of water resistance.Inthis review,the crystal structure and synthesis methods of RPPOs SSEs are firstintroduced in brief.Subsequently,the mechanisms of ion transportation,including oxygen anions and lithium-ions,and the relevant strategies forenhancing their ionic conductivity are described in detail.Additionally,theprogress made in developing flexible RPPOs SSEs,which are critical for flexibleand wearable electronic devices,has also been summarized.Furthermore,thekey challenges and prospects for exploring and developing RPPOs SSEs in allsolid-state batteries are suggested.This review presents in detail the synthesismethods,the ion transportation mechanism,and strategies to enhance theroom temperature ionic conductivity of RPPOs SSEs,providing valuableinsights on enhancing their ionic conductivity and thus for their practicalapplication in solid-state batteries.展开更多
Developing electrochemical energy storage and conversion devices(e.g.,water splitting,regenerative fuel cells and rechargeable metal-air batteries)driven by intermittent renewable energy sources holds a great potentia...Developing electrochemical energy storage and conversion devices(e.g.,water splitting,regenerative fuel cells and rechargeable metal-air batteries)driven by intermittent renewable energy sources holds a great potential to facilitate global energy transition and alleviate the associated environmental issues.However,the involved kinetically sluggish oxygen evolution reaction(OER)severely limits the entire reaction efficiency,thus designing high-performance materials toward efficient OER is of prime significance to remove this obstacle.Among various materials,cost-effective perovskite oxides have drawn particular attention due to their desirable catalytic activity,excellent stability and large reserves.To date,substantial efforts have been dedicated with varying degrees of success to promoting OER on perovskite oxides,which have generated multiple reviews from various perspectives,e.g.,electronic structure modulation and heteroatom doping and various applications.Nonetheless,the reviews that comprehensively and systematically focus on the latest intellectual design strategies of perovskite oxides toward efficient OER are quite limited.To bridge the gap,this review thus emphatically concentrates on this very topic with broader coverages,more comparative discussions and deeper insights into the synthetic modulation,doping,surface engineering,structure mutation and hybrids.More specifically,this review elucidates,in details,the underlying causality between the being-tuned physiochemical properties[e.g.,electronic structure,metal-oxygen(M-O)bonding configuration,adsorption capacity of oxygenated species and electrical conductivity]of the intellectually designed perovskite oxides and the resulting OER performances,coupled with perspectives and potential challenges on future research.It is our sincere hope for this review to provide the scientific community with more insights for developing advanced perovskite oxides with high OER catalytic efficiency and further stimulate more exciting applications.展开更多
基金supported by the National Natural Science Foundation of China(No.22278203)The authors appreciate the support of Zhejiang Zheneng Technology and Environment Group Co.,Ltd’s project(No.TD-KJ-23-005:Methanation of carbon monoxide coupled with in-situ formed hydrogen in a low-temperature SOEC reactor).
文摘Proton ceramic fuel cell efficiently converts chemical energy into electrical energy,representing a pivotal component of future energy systems.However,its current performance is hindered by limitations in cathode and electrolyte materials,thereby impeding commercialization.Anion doping emerges as a promising strategy to enhance the electrochemical efficiency of perovskite-based cathodes and electrolytes.However,integrating this approach within a single-cell structure still requires further research.In this study,F-doped perovskite oxides BaCo_(0.4)Fe_(0.4)Zr_(0.1)Y_(0.1)O_(2.9-δ)F_(0.1)(BCFZYF)and BaZr_(0.1)Ce_(0.7)Y_(0.1)Yb_(0.1)O_(2.9-δ)F_(0.1)(BZCYYbF)were synthesized for use as the cathode and electrolyte,respectively,in proton ceramic fuel cells.Our findings demonstrate that F-doped perovskite oxides exhibit superior electrochemical performance and enhanced structural stability.Furthermore,doping both electrodes and electrolytes with F ions improves their interfacial compatibility.The cell configuration BCFZYF|BZCYYbF|Ni-BZCYYbF achieved a peak power density of 998 mW·cm^(−2)at 650℃using H_(2)as fuel,and it maintained stable operation for over 400 h at 550℃with a current density of 400 mA·cm^(−2).This research underscores an effective strategy for enhancing the performance and durability of proton ceramic fuel cells.
基金supported by the National Natural Science Foundation of China(No.U22A20418,22075196)the Research Project Supported by Shanxi Scholarship Council of China(2022–050).
文摘The electrochemical nitrogen reduction reaction(NRR)under ambient conditions presents a promising approach for the eco-friendly and sustainable synthesis of ammonia,with a continuous emergence of potential electrocatalysts.However,the low solubility and limited diffusion of N_(2)significantly hinder the achievement of satisfactory performance.In this context,we report an effective strategy to enhance NRR activity by introducing a metal-organic framework(MOF)membrane,specifically MIL-53(Al),onto a perovskite oxide(LiNbO_(3)),denoted as LN@MIL-X(X=0.2,0.4 and 0.6).The MIL-53(Al)membrane selectively recognizes and concentrates N_(2)at the catalyst interface while simultaneously repelling water molecules,thereby inhibiting the hydrogen evolution reaction(HER).This ultrathin nanostructure significantly improves the NRR performance of LN@MIL-X compared to pristine LiNbO_(3).Notably,LN@MIL-0.4 exhibits a maximum NH_(3)yield of 45.25 mg h^(-1)mg_(cat.)^(-1)with an impressive Faradaic efficiency(FE)of 86.41%at-0.45 V versus RHE in 0.1 mol L^(-1)Na_(2)SO_(4).This work provides a universal strategy for the design and synthesis of perovskite oxide electrocatalysts,facilitating high-efficiency ammonia synthesis.
基金supported by the Natural Science Foundation for Young Scholars of Jiangsu Province(No.BK20220879)the National Natural Science Foundation of China(No.22209072 and No.22479075)+1 种基金the Open Research Fund of Guangdong Advanced Carbon Materials Co.,Ltd(No.Kargen-2024B0801)the Jiangsu Specially-Appointed Professors and National Natural Science Fund of China for Excellent Young Scientists Fund Program(Overseas)。
文摘Proton exchange membrane water electrolyzer(PEMWE)represents a highly promising technology for renewable hydrogen generation,urgently demanding low-cost,efficient,and robust anode oxygen evolution reaction(OER)electrocatalysts in acidic media.Over the past decade(mainly from 2016 onwards),low-Ir/Ru perovskite oxides have emerged as promising candidate materials for acidic OER electrocatalysis owing to their flexible element compositions and crystal structures,which can evidently reduce the noble-metal content and meanwhile significantly promote electrocatalytic performance.In this review,the current research progress in low-Ir/Ru perovskite oxides for acidic OER electrocatalysis is comprehensively summarized.Initially,we present a brief introduction to general issues relevant to acidic OER catalyzed by low-Ir/Ru perovskite oxides,such as the actual active species,OER mechanisms,inverse activity-stability relationship,and performance evaluation metrics.Subsequently,we present a thorough overview of various low-Ir/Ru perovskite oxides for acidic OER electrocatalysis,including single perovskites,double perovskites,triple perovskites,quadruple perovskites,Ruddlesden-Popper perovskites,and other complex perovskite-derived oxides,with emphasis on the intrinsic factors contributing to their exceptional performance and structure-property-performance correlation.Finally,remaining challenges and some promising insights to inspire future studies in this exciting field are provided.
基金Program for Jiangsu Specially-AppointedProfessors。
文摘Crystalline perovskite oxides are regarded as promising electrocatalysts for water electrolysis,particularly for anodic oxygen evolution reactions,owing to their low cost and high intrinsic activity.Perovskite oxides with noncrystalline or amorphous characteristics also exhibit promising electrocatalytic performance toward electrochemical water splitting.In this review,a fundamental understanding of the characteristics and advantages of crystalline,noncrystalline,and amorphous perovskite oxides is presented.Subsequently,recent progress in the development of advanced electrocatalysts for water electrolysis by engineering and breaking the crystallinity of perovskite oxides is reviewed,with a special focus on the underlying structure–activity relationships.Finally,the remaining challenges and unsolved issues are presented,and an outlook is briefly proposed for the future exploration of next-generation water-splitting electrocatalysts based on perovskite oxides.
基金This study was supported by the National Research Foundation of Korea(NRF-2021R1C1C1010233)funded by the Korean government(MSIT)+1 种基金This research was also supported by the Korea Institute of Energy Technology Evaluation and Planning(KETEP)Grant(No.G032542411)funded by the Korea Ministry of Trade,Industry,and Energy(MOTIE).
文摘Supported nanoparticles have attracted considerable attention as a promising catalyst for achieving unique properties in numerous applications,including fuel cells,chemical conversion,and batteries.Nanocatalysts demonstrate high activity by expanding the number of active sites,but they also intensify deactivation issues,such as agglomeration and poisoning,simultaneously.Exsolution for bottomup synthesis of supported nanoparticles has emerged as a breakthrough technique to overcome limitations associated with conventional nanomaterials.Nanoparticles are uniformly exsolved from perovskite oxide supports and socketed into the oxide support by a one-step reduction process.Their uniformity and stability,resulting from the socketed structure,play a crucial role in the development of novel nanocatalysts.Recently,tremendous research efforts have been dedicated to further controlling exsolution particles.To effectively address exsolution at a more precise level,understanding the underlying mechanism is essential.This review presents a comprehensive overview of the exsolution mechanism,with a focus on its driving force,processes,properties,and synergetic strategies,as well as new pathways for optimizing nanocatalysts in diverse applications.
文摘In this paper, the partial oxidation of methane to synthesis gas using lattice oxygen of La1- SrxMO3-λ (M=Fe, x Mn) perovskite oxides instead of molecular oxygen was investigated. The redox circulation between 11% O2/Ar flow and 11% CH4/He flow at 900℃ shows that methane can be oxidized to CO and H2 with a selectivity of over 90.7% using the lattice oxygen of La1- SrxFeO3-λ (x≤0.2) perovskite oxides in an appropriate reaction condition, while the lost lattice x oxygen can be supplemented by air re-oxidation. It is viable for the lattice oxygen of La1- SrxFeO3-λ (x≤0.2) perovskite x oxides instead of molecular oxygen to react with methane to synthesis gas in the redox mode.
基金Project supported by the Ministry of Education Blue Fire Program(XZJH201717)。
文摘Magnesia modified LaCoO3 was prepared by a facile one-step sol-gel method and used for removal of dilute methane.Compared with the conventional doping technique,the obtained LaCoO3@MgO-x exhibits pseudo core-shell structure and shows superior catalytic activity.The methane conversion exceeds90%at 532℃on LaCoO3@MgO-0.1,while only 60%of methane is conversed using the doped perovskite LaCo0.9Mg0.1O3.The high catalytic performance of LaCoO3@MgO-0.1 is mainly attributed to the adjustment of surface acid-base properties by the MgO shell structure.According to density functional theory(DFT)calculation,the methane is more likely to be adsorbed and cracked on LaCoO3@MgO-0.1.The in situ DRIFTS shows that CH3-O-CH3 intermediate specie is formed.The pseudo core-shell structure also enhances the stability and the LaCoO3@MgO-0.1 maintains high activity after working for 100 h.The above results demonstrate that surface modification by magnesia is an effective strategy for improving LaCoO3 catalytic performance.
基金the Chinese Natural Science Foundation(Project No.20306016)
文摘Comparison of LaFeO3, La0.8Sr0.2FeO3, and La0.8Sr0.2Fe0.9CO0.1O3 perovskite oxides as oxygen carrier for partial oxidation of methane in the absence of gaseous oxygen was investigated by continuous flow reaction and sequential redox reaction, Methane was oxidized to syngas with high selectivity by oxygen species of perovskite oxides in the absence of gaseous oxygen. The sequential redox reaction revealed that the structural stability and continuous oxygen supply in redox reaction decreased over La0.8Sr0.2Fe0.9Co0. 1O3 oxide, while LaFeO3 and La0.8Sr0.2FeO3 exhibited excellent structural stability and continuous oxygen supply.
基金financial supports from the Youth Innovation Fund of Dalian Institute of Chemical Physics (DICP I202126)the Strategic Priority Research Program of Chinese Academy of Sciences (XDB17020400)。
文摘The oxygen evolution reaction (OER) dominates the efficiency of electrocatalytic water splitting owing to its sluggish kinetics.Perovskite oxides (ABO_(3)) have emerged as promising candidates to accelerate the OER process owing to their high intrinsic activities and tailorable properties.Fe ions in perovskite oxides have been proved to be a highly catalytic element for OER,while some Fe-based perovskites such as SrTi_(0.8)Fe_(0.2)O_(3-δ)(STF) and La_(0.66)Ti_(0.8)Fe_(0.2)O_(3-δ)(LTF) exhibit inferior OER activity.Yet the essential reason is still unclear and the effective method to promote the activity of such perovskite is also lacking.Herein,an in-situ exsolution strategy was proposed to boost the OER by migrating Fe from the bulk to the surface.Significantly enhanced OER activity was achieved on STF and LTF perovskites with surfacedecorated oxygen vacancies and Fe nanoparticles.In addition,theoretical calculation confirmed that the oxygen vacancies and Fe nanoparticle on surface could lower the overpotential of OER by facilitating the adsorption of OH^(-).From this study,migration of the active elements in perovskite is found to be an effective strategy to increase the quantity and activity of active sites,providing new insights and understanding for designing efficient OER catalysts.
基金supported by the National Natural Science Foundation of China (51877173)the Key R&D Project of Shaanxi Province (2023-YBGY-057)+1 种基金the State Key Laboratory of Electrical Insulation and Power Equipment (EIPE22314, EIPE22306)the Natural Science Basic Research Program of Shaanxi (2023-JC-QN-0483)。
文摘Solid oxide electrolysis cell(SOEC) could be a potential technology to afford chemical storage of renewable electricity by converting water and carbon dioxide.In this work,we present the Ni-doped layered perovskite oxides,(La_(4)Sr_(n-4))_(0.9)Ti_(0.9n)Ni_(0.1n)O_(3n+2) with n=5,8,and 12(LSTNn) for application as catalysts of CO_(2) electrolysis with the exsolution of Ni nanoparticles through a simple in-situ growth method.It is found that the density,size,and distribution of exsolved Ni nanoparticles are determined by the number of n in LSTNn due to the different stack structures of TiO_6 octahedra along the c axis.The Ni doping in LSTNn significantly improved the electrochemical activity by increasing oxygen vacancies,and the Ni metallic nanoparticles afford much more active sites.The results show that LSTNn cathodes can successfully be manipulated the activity by controlling both the n number and Ni exsolution.Among these LSTNn(n=5,8,and 12),LSTN8 renders a higher activity for electrolysis of CO_(2) with a current density of 1.50A cm^(-2)@2.0 V at 800℃ It is clear from these results that the number of n in(La_(4)Sr_(n-4))_(0.9)Ti_(0.9n)Ni_(0.1n)O_(3n+2)with Ni-doping is a key factor in controlling the electrochemical performance and catalytic activity in SOEC.
基金supported by the National Natural Science Foundation of China(Project No.21908106 and 21878158)the Jiangsu Natural Science Foundation(Project No.BK20190682)+2 种基金the Program for Jiangsu Specially Appointed Professorsthe Funding from State Key Laboratory of Materials-Oriented Chemical Engineering(Project No.ZK201808)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
文摘Volatile organic compounds are a kind of important indoor and outdoor air pollutants.In recent years,more and more attention has been paid to the ways of volatile organic compound elimination because of its potential long-term effects on human health.Among the various available methods for volatile organic compound elimination,the catalytic combustion is the most attractive method due to its high efficiency,low cost,simple operation,and easy scale-up.Perovskite oxides,as a large family of metal oxides with their A-site mainly of lanthanide element and/or alkaline earth metal element and B-site of transition metal element,have been extensively investigated as active and stable catalysts for volatile organic compound removal reactions due to their abundant compositional elements,high thermal/chemical stability,and compositional/structural flexibility.The catalytic performance of perovskite oxides is strongly depended on its material composition,morphology,and surface/bulk properties,while the doping,tailored synthesis route,and composite construction may have a significant effect on the bulk(oxygen vacancy concentration,lattice structure),surface(oxygen species,defect)properties,and particulate morphology,consequently the catalytic activity and stability for volatile organic compound removal.Herein,a comprehensive review about the recent advances in perovskite oxides for volatile organic compound elimination reactions based on catalytic combustion is presented from different aspects with a special emphasis on the material design strategies,such as compositional tuning,morphology control,nanostructure building,hybrid construction,and surface modification.At last,some perspectives are presented on the development and design of perovskite oxide-based catalysts for volatile organic compound removal applications by highlighgting the critical issues and challenges.
基金acknowledge support from the National Natural Science Foundation of China(Nos.21922105,21931001,22201111,and 22271124)the National Key R&D Program of China(2021YFA1501101)+4 种基金the National Natural Science Foundation of Gansu Province(22JR5RA470)the Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province(2019ZX-04)the 111 Project(B20027).We also acknowledge support from the Fundamental Research Funds for the Central Universities(lzujbky-2021-sp62)the support of the Natural Science Foundation of China(NSFC)(No.21771156)the Early Career Scheme(ECS)fund(Grant PolyU253026/16P)from the Research Grant Council(RGC)in Hong Kong.
文摘The benefits of perovskite oxides include their low cost,customizable composition,ordered atomic structure,and extremely flexible electronic structure.They are the ideal substitute for precious metal catalysts in various electrocatalytic reactions.However,the initial activity of perovskite oxides is often quite limited,which is extremely related to their crystal structure and electronic structure.In this regard,component regulation is the simplest and most effective strategy to increase their stability and catalytic activity.In this review,we briefly outline the recent progress in the modulating component of perovskite oxides to enhance their catalytic properties.The outline was categorized according to the sites in the ABO3-type perovskite structure,including A-site,B-site,and O-site regulation.Finally,potential research directions aimed at modulating of perovskite oxide constituents are discussed.
基金the financial support from the Recruitment Program of Global Young Experts Start-up Fundthe Program of Introducing Talents of Discipline to Universities of China(111 Program, No. B17019)
文摘Heterogeneous catalytic combustion provides a feasible technique for high efficient methane utilization.Perovskites ABO_3-type materials have received renewed attention as a potential alternative for noble metals supported catalysts in catalytic methane combustion due to excellent hydrothermal stability and sulfur resistance. Recently, the emergence of nanostructured perovskite oxides（such as threedimensional ordered nanostructure, nano-array structure） with outstanding catalytic activity has further driven methane catalytic combustion research into spotlight. In this review, we summarize the recent development of nanostructured perovskite oxide catalysts for methane combustion, and shed some light on the rational design of high efficient nanostructured perovskite catalysts via lattice oxygen activation,lattice oxygen mobility and materials morphology engineering. The emergent issues needed to be addressed on perovskite catalysts were also proposed.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.52171174 and 91963123)the Ten Thousand Talents Plan of Zhejiang Province(No.2018R52003)the Fundamental Research Funds for the Provincial University of Zhejiang(No.GK199900299012-022).
文摘The magnetic functional materials play a particularly important role in our modern society and daily life.The magnetocaloric effect(MCE)is at the basis of a solid state magnetic refrigeration(MR)technology which may enhance the efficiency of cooling systems,both for room temperature and cryogenic appli-cations.Despite numerous experimental and theoretical MCE studies,commercial MR systems are still at developing stage.Designing magnetic solids with outstanding magnetocaloric performances remains therefore a most urgent task.Herein,recent progresses on characterizing the crystal structure,magnetic properties and cryogenic MCE of rare earths(RE)-based RE_(2)TMTM’O_(6)double perovskite(DP)oxides,where TM and TM’are different 3d transition metals,are summarized.Some Gd-based DP oxides are found to exhibit promising cryogenic magnetocaloric performances which make them attractive for active MR ap-plications.
基金support from the National Natural Science Foundation of China(Grant Nos.52425308,62374035 and 92263106).
文摘CONSPECTUS:Ultraviolet(UV)light,spanning wavelengths from 10 to 400 nm,is ubiquitous in military,livelihood,and scientific domains.Accurate UV photodetection is therefore essential for monitoring environmental radiation,safeguarding human health,and advancing technological applications in fields such as aerospace,medical science,and ecology.The fabrication of high-performance UV photodetection devices fundamentally depends on the development of high-sensitivity UV photosensitive materials.The evolution of UV photodetection materials has progressed from early wide-bandgap semiconductors like ZnS and ZnSe to third-generation semiconductors such as GaN and Ga_(2)O_(3),and most recently to two-dimensional(2D)wide-bandgap materials that combine exceptional optoelectronic properties with compelling physicochemical properties.Among these,2D perovskite oxides stand out due to their prominent advantages for UV detection.First,this large family of materials generally features wide bandgaps,strong UV absorption,and high spectral selectivity.Second,the tunable bandgaps of 2D perovskite oxides enable precise detection at specific wavelengths.Third,their excellent processability and flexibility facilitate feasible integration into devices,making them promising candidates for flexible photodetectors.Furthermore,2D perovskite oxides boast other properties such as high stability,dielectricity,ferroelectricity,and biocompatibility.These characteristics have promoted the blossoming of 2D perovskite oxides for highperformance UV photodetection and are poised to expand their applications in novel functional optoelectronics.In this Account,we systematically review the development of 2D perovskite oxides,with a focus on their application in the fabrication of high-performance UV photodetectors.First,we describe the top-down synthesis of these materials,highlighting key advances in synthesis techniques.Second,we specifically analyze the intrinsic advantages of 2D perovskite oxides which render them highly suitable for UV detection.Third,we discuss recent progress in the fabrication of UV photodetectors based on 2D perovskite oxides,emphasizing effective strategies for achieving high-performance devices.Next,we explore state-of-the-art optoelectronic applications leveraging these materials.Finally,we present our perspectives on the future development of this promising class of UVsensitive materials.Given their remarkable material diversity,we believe that this Account will provide valuable insights to guide future research and the application of 2D perovskite oxides in high-performance UV photodetectors and functional optoelectronics.
基金supported by the National Key Research and Development Program of China(No.2023YFB3812200)Major Program of the Natural Science Foundation of China(51790490)+2 种基金NSFC-Guangdong Joint Funds of the Natural Science Foundation of China(No.U1601209)the National Key Basic Research Program of China(973 Program)(No.2015CB654601)Technical Innovation Special Program of Hubei Province(2017AHB055).
文摘The interpretability of machine learning reveals associations between input features and predicted physical properties in models,which are essential for discovering new materials.However,previous works were mainly devoted to algorithm improvement,while the essential multi-scale characteristics are not well addressed.This paper introduces distortion modes of oxygen octahedrons as cross-scale structural features to bridge chemical compositions and material properties.Combining modelagnostic interpretation methods,we are able to achieve interpretability even using simple machine learning schemes and develop a predictive model of effective mass for a widely used material type,namely perovskite oxides.With this framework,we reach the interpretability of the model,understanding the trend of the effective mass without any prior background information.Moreover,we obtained the knowledge only available to experts,i.e.,the interpretation of effective mass from the sep orbitals hybridization of B-site cations and O^(2-)in ABO_(3)perovskite oxides.
基金supported by the National Natural Science Foundation of China(Nos.22175071 and 22425104)National Key R&D Program of China(No.2023YFA1506300)+1 种基金the“111”Project of the Ministry of Education of China(No.B17020)the Jilin Province Science and Technology Development Plan(No.YDZJ202101ZYTS137).
文摘Porous perovskite metal oxides(PPMOs)have emerged as promising candidates for efficient catalysts in fine chemical engineering due to their flexible crystal structures and tunable surface chemical properties.However,the conventional high temperature calcination process required for crystallization frequently leads to collapse of pore structure,limiting the practical application of PPMOs.Herein,we propose a facile and general polymer derived bubble templates strategy to synthesize a series of PPMOs,including single-component PPMOs(e.g.,LaMnO_(3),LaFeO_(3),LaCoO_(3),PrMnO_(3),and NdMnO_(3))and multiple-component PPMOs(e.g.,LaCo_(x)Mn_(1-x)O_(3)(x=0.1,0.2,and 0.3))with tunable pore structure.The pore architectures(macropores,hierarchically meso/macropores,and mesopores),pore sizes,and specific surface areas(14-40 m^(2)·g^(-1))of the samples can be precisely tailored by adjusting the sizes of bubble templates.The hierarchically meso/macroporous LaMnO_(3)features multiple structural advantages,including well-defined hierarchical porous architecture,high specific surface area,and abundant oxygen vacancies,and exhibits a remarkable catalytic performance in oxidation of benzyl alcohol to benzaldehyde,with conversion and selectivity of 99%and 99%,respectively.This work not only provides a scalable and versatile pathway for fabricating advanced porous materials but also offers new perspectives for their application in diverse catalytic processes.
基金the Natural Science Foundation of Shanghai Municipality General Project(No.24ZR1430400).
文摘It is urgent to develop novel energy storage and conversion systems to address the pressing issues of the energy crisis and environmental pollution,including alkaline water electrolysis,alkaline fuel cells and metal-air batteries.However,these systems are hampered by the sluggish kinetics of the oxygen evolution reaction(OER)or oxygen reduction reaction(ORR).One of the most effective strategies to overcome this challenge is the development of efficient and stable catalysts for both ORR and OER,which typically consist of Pt,Ir,or other precious metals.Unfortunately,most precious metal catalysts are limited to single catalytic activity(either ORR or OER)and are constrained by the high cost and scarcity of noble metals.Perovskite oxides offer significant promise as efficient bifunctional ORR/OER catalysts due to their high catalytic activity,versatile composition,low cost,and high stability in alkaline environments.The general preparation methods of perovskite-type oxides are summarized in this work.Then recent mechanistic studies on the ORR and OER of perovskite oxides are also discussed,particularly highlighting the theoretical and experimental methods employed to facilitate these studies.Further strategies for improving the catalytic performance of perovskite oxides are discussed from five perspectives.The perspective of challenges and future directions for the development of perovskite oxides in ORR and OER applications are finally presented.
基金National Natural Science Foundation of China,Grant/Award Numbers:21671106,22371043,62288102Priority Academic Program Development of Jiangsu Higher Education Institutions+1 种基金Minjiang Scholars Award Program(2023),Fujian ProvinceStart-Up Fund for High-Leveled Talents from Fujian Normal University,Grant/Award Numbers:Y0720316K13,Y0720320K13。
文摘All-solid-state batteries equipped with solid-state electrolytes(SSEs)havegained significant interest due to their enhanced safety,energy density,andlongevity in comparison to traditional liquid organic electrolyte-based batteries.However,many SSEs,such as sulfides and hydrides,are highly sensitiveto water,limiting their practical use.As one class of important perovskites,theRuddlesden–Popper perovskite oxides(RPPOs),show great promise as SSEsdue to their exceptional stability,particularly in terms of water resistance.Inthis review,the crystal structure and synthesis methods of RPPOs SSEs are firstintroduced in brief.Subsequently,the mechanisms of ion transportation,including oxygen anions and lithium-ions,and the relevant strategies forenhancing their ionic conductivity are described in detail.Additionally,theprogress made in developing flexible RPPOs SSEs,which are critical for flexibleand wearable electronic devices,has also been summarized.Furthermore,thekey challenges and prospects for exploring and developing RPPOs SSEs in allsolid-state batteries are suggested.This review presents in detail the synthesismethods,the ion transportation mechanism,and strategies to enhance theroom temperature ionic conductivity of RPPOs SSEs,providing valuableinsights on enhancing their ionic conductivity and thus for their practicalapplication in solid-state batteries.
基金supported by the National Natural Science Foundation of China(NSFC,Grant No.22109182)the Natural Science Foundation of Hunan Province,China(2022JJ30684)+1 种基金the Start-up Funding of Central South University(No.206030104)the Natural Sciences and Engineering Research Council(NSERC)of Canada Discovery Grant(GRPIN−2016−05494).
文摘Developing electrochemical energy storage and conversion devices(e.g.,water splitting,regenerative fuel cells and rechargeable metal-air batteries)driven by intermittent renewable energy sources holds a great potential to facilitate global energy transition and alleviate the associated environmental issues.However,the involved kinetically sluggish oxygen evolution reaction(OER)severely limits the entire reaction efficiency,thus designing high-performance materials toward efficient OER is of prime significance to remove this obstacle.Among various materials,cost-effective perovskite oxides have drawn particular attention due to their desirable catalytic activity,excellent stability and large reserves.To date,substantial efforts have been dedicated with varying degrees of success to promoting OER on perovskite oxides,which have generated multiple reviews from various perspectives,e.g.,electronic structure modulation and heteroatom doping and various applications.Nonetheless,the reviews that comprehensively and systematically focus on the latest intellectual design strategies of perovskite oxides toward efficient OER are quite limited.To bridge the gap,this review thus emphatically concentrates on this very topic with broader coverages,more comparative discussions and deeper insights into the synthetic modulation,doping,surface engineering,structure mutation and hybrids.More specifically,this review elucidates,in details,the underlying causality between the being-tuned physiochemical properties[e.g.,electronic structure,metal-oxygen(M-O)bonding configuration,adsorption capacity of oxygenated species and electrical conductivity]of the intellectually designed perovskite oxides and the resulting OER performances,coupled with perspectives and potential challenges on future research.It is our sincere hope for this review to provide the scientific community with more insights for developing advanced perovskite oxides with high OER catalytic efficiency and further stimulate more exciting applications.
