Reversible solid oxide cell(RSOC)is a new energy conversion device with significant applications,especially for power grid peaking shaving.However,the reversible conversion process of power generation/energy storage p...Reversible solid oxide cell(RSOC)is a new energy conversion device with significant applications,especially for power grid peaking shaving.However,the reversible conversion process of power generation/energy storage poses challenges for the performance and stability of air electrodes.In this work,a novel high-entropy perovskite oxide La_(0.2)Pr_(0.2)Gd_(0.2)Sm_(0.2)Sr_(0.2)Co_(0.8)Fe_(0.2)O_(3−δ)(HE-LSCF)is proposed and investigated as an air electrode in RSOC.The electrochemical behavior of HE-LSCF was studied as an air electrode in both fuel cell and electrolysis modes.The polarization impedance(Rp)of the HE-LSCF electrode is only 0.25Ω·cm^(2) at 800℃ in an air atmosphere.Notably,at an electrolytic voltage of 2 V and a temperature of 800℃,the current density reaches up to 1.68 A/cm^(2).The HE-LSCF air electrode exhibited excellent reversibility and stability,and its electrochemical performance remains stable after 100 h of reversible operation.With these advantages,HE-LSCF is shown to be an excellent air electrode for RSOC.展开更多
Multicomponent Gd_(1−x)Sm_(x)Ba_(0.5)Sr_(0.5)CoCuO_(5+δ)double perovskites are optimized for application in terms of chemical composi-tion and morphology for the use as oxygen electrodes in solid oxide cells.Structur...Multicomponent Gd_(1−x)Sm_(x)Ba_(0.5)Sr_(0.5)CoCuO_(5+δ)double perovskites are optimized for application in terms of chemical composi-tion and morphology for the use as oxygen electrodes in solid oxide cells.Structural studies of other physicochemical properties are con-ducted on a series of materials obtained by the sol-gel method with different ratios of Gd and Sm cations.It is documented that changing the x value,and the resulting adjustment of the average ionic radius,have a significant impact on the crystal structure,stability,as well as on the total conductivity and thermomechanical properties of the materials,with the best results obtained for the Gd_(0.75)Sm_(0.2)5Ba_(0.5)Sr_(0.5)CoCuO_(5+δ)composition.Oxygen electrodes are prepared using the selected compound,allowing to obtain low polarization resistance values,such as 0.086Ω·cm^(2)at 800℃.Systematic studies of electrocatalytic activity are conducted using La_(0.8)Sr_(0.2)Ga_(0.8)Mg_(_(0.2))O_(3−δ)as the electrolyte for all electrodes,and Ce_(0.8)Gd_(0.2)O_(2−δ)electrolyte for the best performing Gd_(0.75)Sm_(0.2)5Ba_(0.5)Sr_(0.5)CoCuO_(5+δ)electrodes.The electrochemical data are analyzed using the distribution of relaxation times method.Also,the influence of the preparation method of the electrode material is in-ve`stigated using the electrospinning technique.Finally,the performance of the Gd_(0.75)Sm_(0.2)5Ba_(0.5)Sr_(0.5)CoCuO_(5+δ)electrodes is tested in a Ni-YSZ(yttria-stabilized zirconia)anode-supported cell with a Ce_(0.8)Gd_(0.2)O_(2−δ)buffer layer,in the fuel cell and electrolyzer operating modes.With the electrospun electrode,a power density of 462 mW·cm^(−2)is obtained at 700℃,with a current density of ca.0.2 A·cm^(−2)at 1.3 V for the electrolysis at the same temperature,indicating better performance compared to the sol-gel-based electrode.展开更多
Cation segregation on cathode surfaces plays a key role in determining the activity and operational stability of solid oxide fuel cells(SOFCs).The double perovskite oxide PrBa_(0.8)Ca_(0.2)Co_(2)O_(5+δ)(PBCC)has been...Cation segregation on cathode surfaces plays a key role in determining the activity and operational stability of solid oxide fuel cells(SOFCs).The double perovskite oxide PrBa_(0.8)Ca_(0.2)Co_(2)O_(5+δ)(PBCC)has been widely studied as an active cathode but still suffer from serious detrimental segregations.To enhance the cathode stability,a PBCC derived A-site medium-entropy Pr_(0.6)La_(0.1)Nd_(0.1)Sm_(0.1)Gd_(0.1)Ba_(0.8)Ca_(0.2)Co_(2)O_(5+δ)(ME-PBCC)oxide was prepared and its segregation behaviors were investigated under different conditions.Compared with initial PBCC oxide,the segregations of BaO and Co_(3)O_(4)on the surface of ME-PBCC material are significantly suppressed,especially for Co_(3)O_(4),which is attributed to its higher configuration entropy.Our results also confirm the improved electrochemical performance and structural stability of ME-PBCC material,enabling it as a promising cathode for SOFCs.展开更多
Introduction High-entropy oxides(HEOs)have attracted much attention in the field of electrochemistry due to their distinctive structural characteristics and unique properties.The multiple-principal elements in HEOs of...Introduction High-entropy oxides(HEOs)have attracted much attention in the field of electrochemistry due to their distinctive structural characteristics and unique properties.The multiple-principal elements in HEOs offer the multiple redox pairs and multiple possible active sites,which can enhance the energy storage capacity and the electrocatalytic performance.Although the notable progress is achieved in the development of HEOs electrodes,their electrochemical properties should be further improved to meet the requirements of high-performance supercapacitors and OER electrocatalysts.The abundant active sites for the Faradic redox reactions and short pathways for charge transportation could be constructed through the design of novel HEOs with advanced microstructures,thus improving the electrochemical properties.As advanced microstructures,a hollow structure has a great promise for energy storage and conversion because it can provide more accessible storage sites,more catalytic centers and a larger electrode/electrolyte contact area.It is thus expected that the construction of hollow structure is an alternative route to significantly promote the electrochemical properties of HEOs electrode materials.However,it is difficult to prepare the HEOs with a hollow structure due to the complexity of the high-entropy system.In this work,a hollow spherical high-entropy perovskite oxide of La(Cr_(0.2)Mn_(0.2)Fe_(0.2)Ni_(0.2)Cu_(0.2))O_(3)(HS-HEPs)was prepared by microwave solvothermal process and subsequent calcination treatment.The as-prepared HS-HEPs exhibited the excellent electrochemical performance when used as an electrode material for supercapacitors and OER electrocatalysts due to the advantages resulted from the combination of high-entropy perovskite and special hollow structure.Methods HS-HEPs were prepared by microwave solvothermal process and subsequent calcination treatment.Typically,0.134 mmol Cr(NO_(3))_(3)·6H_(2)O,0.134 mmol Mn(NO_(3))_(2)·4H_(2)O,0.134 mmol Fe(NO_(3))_(3)·9H_(2)O,0.134 mmol Ni(NO_(3))_(2)·6H_(2)O,0.134 mmol Cu(NO_(3))_(2)·3H_(2)O,and 0.5 mmol La(NO_(3))_(3)·6H_(2)O were dissolved in 30 mL ethanol under stirring for 1 h to obtain the homogeneous solution.Afterwards,60 mg of carbon spheres were added in the solution under ultrasonic treatment for 30 min.The resulting mixture was transferred to a 50 mL microwave digestion vessel.The vessel was heated in a microwave oven at a power of 210 W for 10 min.Subsequently,the obtained mixture was centrifuged,washed with deionized water,and dried in a vacuum drying oven at 70℃for 12 h.Finally,the obtained precursor powder was calcinated in a tube furnace with a heating rate of 3℃/min at 650℃for 2 h to acquire HS-HEPs.The crystalline structure of the sample was determined by X-ray diffraction(XRD,D8 Davinci,Bruker Co.,Germany).The morphology and microstructure of sample were characterized by field-emission scanning electron microscopy(FESEM,S-4800,Hitachi Co.Ltd.,Japan)equipped with energy dispersive X-ray spectroscopy(EDS)and transmission electron microscopy(TEM,2100F,JEOL Co.,Japan).The X-ray photoelectron spectra were obtained by a X-ray photoelectron spectrometry(XPS,ESCALab 250,Thermo VG Co.,USA).The supercapacitor and OER performance of the sample were measured on a CHI 660E electrochemical workstation(Shanghai Chenhua Instrument Co.,China).Results and discussion The as-prepared samples display a cubic perovskite crystalline structure and a hollow sphere morphology.According to the XPS analysis,the variable oxidation states of Cr,Fe and Mn present in the HS-HEPs,which benefits the Faradaic redox reactions and increases the capacitance.In addition,the existence of high concentration of oxygen vacancies in HS-HEPs is beneficial to enhancing the capacitance and OER activity.Based on the GCD curve,the specific capacitance of HS-HEPs is estimated to be 406 F/g at 1 A/g.After GCD cycles of 5000 at a current density of 5 A/g,65%capacitance is retained,implying a good long-term electrochemical stability.An asymmetric supercapacitor device(HS-HEPs//AC)with a two electrode configuration is assembled.A maximum energy density of 39.4 W·h/kg is achieved at power density of 746 W/kg.The OER activity of HS-HEPs is evaluated by a linear sweep voltammetry(LSV)polarization curve in 1 mol/L KOH aqueous solution using a standard three-electrode system.The overpotential of HS-HEPs is identified as 347 mV versus RHE for achieving a current density of 10 mA/cm^(2),which is smaller than that of commercial IrO2(372 mV).The HS-HEPs possess the excellent electrochemical performance,which can be ascribed to the high specific surface area,abundant active sites,and high oxygen vacancy content,resulting from the combination of high-entropy perovskite and special hollow structure.Conclusions High-entropy La(Cr_(0.2)Mn_(0.2)Fe_(0.2)Ni_(0.2)Cu_(0.2))O_(3)hollow spheres with a perovskite crystalline structure were prepared by microwave solvothermal process and subsequent calcination treatment.The HS-HEPs possessed the excellent electrochemical performance,which could be ascribed to the high specific surface area,abundant active sites,and high oxygen vacancy content,resulting from the combination of high-entropy perovskite and special hollow structure.Based on the electrochemical performance,HS-HEPs could be used as supercapacitor electrode material and OER electrocatalysts.This work could provide a strategy to design and prepare high-entropy oxides with a hollow sphere structure,having promising applications in energy storage and conversion.展开更多
Polycrystalline perovskite oxide particles are promising candidates for cathode materials in solid oxide fuel cells.However,their limited activity and stability pose significant challenges for practical applications.I...Polycrystalline perovskite oxide particles are promising candidates for cathode materials in solid oxide fuel cells.However,their limited activity and stability pose significant challenges for practical applications.In this study,we demonstrate a novel approach to achieve both high activity and durability in a PrBaCo_(2)O_(5+δ) catalyst through a simple epitaxial layer growth strategy.We found that an amorphous precursor of the highly durable catalyst SmBa_(0.5)Ca_(0.5)CoCuO_(5+δ) can spontaneously adhere to the surface of PrBaCo_(2)O_(5+δ) particles.Upon heat treatment,it grows along the perovskite lattice,forming a heteroepitaxial layer with just a few atomic layers thickness.This heterostructure enhances the operational stability of PrBaCo_(2)O_(5+δ) transforming a 78% decrease over 100 h into a 7% increase.After 100 h,the power output density of the cell with the modified sample is more than 500% higher than that of unmodified PrBaCo_(2)O_(5+δ.)This work presents a new strategy for fabricating heteroepitaxial layers on polycrystalline ceramic catalysts and introduces a pioneering approach for developing high-performance oxygen reduction catalysts and related materials.展开更多
Widely used spin-coated nickle oxide (NiOx) based perovskite solar cells often suffer from severe interfacial reactions between the NiOxand adjacent perovskite layers due to surface defect states,which inherently impa...Widely used spin-coated nickle oxide (NiOx) based perovskite solar cells often suffer from severe interfacial reactions between the NiOxand adjacent perovskite layers due to surface defect states,which inherently impair device performance in a long-term view,even with surface molecule passivation.In this study,we developed high-quality magnetron-sputtered NiOxthin films through detailed process optimization,and compared systematically sputtered and spin-coated NiOxthin film surfaces from materials to devices.These sputtered NiOxfilms exhibit improved crystallinity,smoother surfaces,and significantly reduced Ni3+or Ni vacancies compared to their spin-coated counterparts.Consequently,the interface between the perovskite and sputtered NiOxfilm shows a substantially reduced density of defect states.Perovskite solar cells (PSCs) fabricated with our optimally sputtered NiOxfilms achieved a high power conversion efficiency (PCE) of up to 19.93%and demonstrated enhanced stability,maintaining 86.2% efficiency during 500 h of maximum power point tracking under one standard sun illumination.Moreover,with the surface modification using (4-(2,7-dibromo-9,9-dimethylacridin-10(9H)-yl)butyl)p hosphonic acid (DMAcPA),the device PCE was further promoted to 23.07%,which is the highest value reported for sputtered NiOxbased PSCs so far.展开更多
Perovskite oxides(ABO_(3))are thought to be promising electrocatalysts for oxygen evolution reaction(OER),but their specific surface area(SSA)is too low(usually<10 m^(2) g^(−1)).Developing advanced ABO_(3) electroc...Perovskite oxides(ABO_(3))are thought to be promising electrocatalysts for oxygen evolution reaction(OER),but their specific surface area(SSA)is too low(usually<10 m^(2) g^(−1)).Developing advanced ABO_(3) electrocatalysts with high SSA and optimized structure is of great significance but remains a tremendous challenge.Herein,we propose a general strategy for fabrication of mesoporous perovskite oxide nanosheets(MPONs)with controllable atomic doping via self-sacrificial template-induced nanostructure modulation.A variety of MPONs including LaFeO_(3),A-site-doped LaFeO_(3)(A-LaFeO_(3),where A is Pr,Nd,Sm,Eu,or Gd)and B-site-doped LaFeO_(3)(B-LaFeO_(3),where B is Mn,Co,Ni,Cu,or Zn)have been achieved.Interestingly,it is discovered that the catalytic activities of A-LaFeO_(3) MPONs as OER catalysts are overall higher than those of B-LaFeO_(3) ones.Especially,the screened Eu-LaFeO_(3) MPONs only require a low overpotential of 267 mV at 10 mA cm^(−2),outperforming most reported perovskite oxides.The superior catalytic activity of Eu-LaFeO_(3) MPONs is attributed to their favorable porous structure,which increases the density of active sites,and enhanced lattice oxygen participation,which improves the intrinsic activity.This study provides guidance for the design and controlled synthesis of advanced rare-earth-doped MPONs with ultrahigh SSA for enhanced electrocatalysis.展开更多
Premature perovskite films rapidly form at the FAI/PbI_(2)interface,inhibiting further reactions between FAI and PbI_(2)during the fabrication of perovskite films via the evaporating-spraying hybrid method according t...Premature perovskite films rapidly form at the FAI/PbI_(2)interface,inhibiting further reactions between FAI and PbI_(2)during the fabrication of perovskite films via the evaporating-spraying hybrid method according to our previous research.In this research,triphenylphosphine oxide(TPPO)was proved to be an effective coordinator that reduces the reaction rate between FAI and PbI_(2)at the initial stage,which can be attributed to the hydrogen(H)bonds between FA^(+)and TPPO,and coordinate bonds between TPPO and PbI_(2).Additionally,the quality of perovskite films improved significantly:the trap state density decreased from 1.6×10^(18)to 3.17×10^(17)cm^(-3),while the crystal size increased from 740 to 940 nm.The champion perovskite device achieved a remarkable efficiency of 20.93%(0.09 cm^(2))and 16.75%(63.7 cm^(2)),marking one of the highest reported results for the evaporating-spraying hybrid method.Moreover,the perovskite solar cells retained over 80%of their initial performances after 600 h of storage at 60℃in a nitrogen environment without encapsulation.It also maintained approximately 90%of its initial performance after continuous illumination at 25℃for 1400 h under the same conditions.展开更多
The increasing demand for solar energy,driven by the climate crisis and carbon neutrality goals,un-derscores the critical importance of aesthetics in solar panel integration across diverse environments,such as buildin...The increasing demand for solar energy,driven by the climate crisis and carbon neutrality goals,un-derscores the critical importance of aesthetics in solar panel integration across diverse environments,such as building-integrated photovoltaics.This study addresses this need by developing angle-insensitive coloration for translucent perovskite-colored solar cells(TPCSCs)to enhance both functionality and con-sumer appeal.By engineering oxide/metal/oxide(OMO)multilayer structures,we achieved consistent col-oration regardless of the viewing angle,overcoming a major challenge in colored solar cell technology.Specifically,ZnO:Al/Ag/ZnO:Al-based OMO layers were meticulously optimized to balance visual appeal with photovoltaic efficiency.Our results demonstrate exceptional angular stability,with negligible color shifts observed even at viewing angles exceeding 60°,significantly surpassing the limitations of previ-ous designs,which exhibited sensitivity at 40°.The OMO electrodes exploited distributed Bragg reflector(DBR)properties to amplify interference effects and utilized delocalized plasmonic modes and metal-dielectric-metal(MDM)cavity resonances to achieve vibrant colors.Advanced 3-pair OMO transparent conductive electrodes(TCEs)exhibited stable,angle-insensitive blue coloration,and the resulting translu-cent perovskite solar cell achieved a record-high power conversion efficiency(PCE)of 8.25%and an av-erage transmittance of 15.23%,maintaining consistent coloration up to a 60°viewing angle.Additionally,the optoelectronic control layer(OCL)thickness was fine-tuned to precisely target specific wavelengths,enabling a versatile spectrum of colors,including blue,green,yellowish-green,orange,and peach.This pioneering approach not only ensures color fidelity but also enhances the reflectance properties of TPC-SCs.By integrating aesthetic and functional advancements,our research makes a significant contribution to the development of sustainable energy solutions for future smart cities.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
The bifunctional oxygen evolution/reduction reaction(OER/ORR) performance of perovskite oxides in zinc-air batteries(ZABs) is fundamentally constrained by the unidirectional catalytic activity of B-site transition met...The bifunctional oxygen evolution/reduction reaction(OER/ORR) performance of perovskite oxides in zinc-air batteries(ZABs) is fundamentally constrained by the unidirectional catalytic activity of B-site transition metal elements.This work proposes a heterostructure engineering strategy through selective etching to construct crystalline perovskite@amorphous hydroxide composites with spatially segregated active sites,where crystalline cores are for ORR and amorphous shells are for OER.Our investigation reveals that the differential solubility of alkaline-earth and rare-earth elements in acidic media enables precise control over surface amorphous layer composition and thickness through A-site cation ratio modulation and tailored etching protocols.Ab initio molecular dynamics(AIMD) simulations reveal the coupled process of A-site cations dissolution,oxygen vacancy formation,and amorphous-layer growth during the dynamic restructuring of the core-shell structure.The optimized Pr_(0.25)Sr_(0.75)FeO_(3-δ)@NiFe LDH achieved a 212 mV improvement of OER/ORR potential gap(ΔE=E_(10 mA cm-2)-E_(1/2)) over pristine Pr_(0.25)Sr_(0.75)FeO_(3-δ).When deployed in ZABs,the catalyst demonstrates a peak power density of 92.9 mW cm~(-2) and exceptional cycling stability with only 6.3% energy efficiency decay after 300 h(vs.10.2% decay for Pt/C-RuO_(2)).This work establishes a universal "composition-guided reconstruction" paradigm,providing both theoretical insights and practical solutions for high-performance electrode design of ZABs.展开更多
The performance of the fuel electrode in a solid oxide electrolysis cell(SOEC)is crucial to facilitating fuel gas electrolysis and is the key determinant of overall electrolysis efficiency.Nevertheless,the commerciali...The performance of the fuel electrode in a solid oxide electrolysis cell(SOEC)is crucial to facilitating fuel gas electrolysis and is the key determinant of overall electrolysis efficiency.Nevertheless,the commercialization of integrated CO_(2)-H_(2)O electrolysis in SOEC remains constrained by suboptimal catalytic efficiency and long-term stability limitations inherent to conventional fuel electrode architec-tures.A novel high-entropy Sr_(2)FeTi_(0.2)Cr_(0.2)Mn_(0.2)Mo_(0.2)Co_(0.2)O_(6−δ)(SFTCMMC)was proposed as a prospective electrode material of co-elec-trolysis in this work.The physicochemical properties and electrochemical performance in the co-electrolysis reaction were investigated.Full cell is capable of electrolyzing H_(2)O and CO_(2)effectively with an applied voltage.The effects of temperature,H_(2)O and CO_(2)concentra-tions,and applied voltage on the electrochemical performance of Sc_(0.18)Zr_(0.82)O_(2−δ)(SSZ)-electrolyte supported SOEC were investigated by varying the operating conditions.The SOEC obtains a favorable electrolysis current density of 1.47 A·cm^(−2)under co-electrolysis condi-tion at 850℃ with 1.5 V.Furthermore,the cell maintains stable performance for 150 h at 1.3 V,and throughout this period,no carbon de-position is detected.The promising findings suggest that the high-entropy SFTCMMC perovskite is a viable fuel electrode candidate for efficient H_(2)O/CO_(2)co-electrolysis.展开更多
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
CO_(2)electrolysis using solid oxide electrolysis cells is a promising technology for CO_(2)utilization and conversion,which has attracted more and more attention in recent years because of its extremely high efficien...CO_(2)electrolysis using solid oxide electrolysis cells is a promising technology for CO_(2)utilization and conversion,which has attracted more and more attention in recent years because of its extremely high efficiency.However,traditional Ni-yttria-stabilized zirconia(Ni-YSZ)or Ni-Gd_(0.1)Ce_(0.9)O_(2-δ)(Ni-GDC)metal-ceramic cathode faces many problems such as Ni agglomeration and carbon deposition during long-time operation.Herein,a perovskite oxide La_(0.43-x)Ca_(0.37)Ti_(0.9)Ni_(0.1)O_(3-δ)(LCTN,x=0,0.05,0.1)with nanophase-LaVO_(4)exsolution was investigated as the novel cathode of solid oxide electrolysis cell(SOEC)for efficient CO_(2)electrolysis.The results confirm that the exsolution nanophase on LCTN surface can significantly improve the CO_(2)adsorption and conversion performance.For CO_(2)electrolysis at 1.8 V,an electrolysis current density of 1.24 A/cm2at 800℃can be obtained on SOEC with La_(0.43-x)Ca_(0.37)Ti_(0.9)Ni_(0.1)O_(3-δ)decorated with LaVO_(4)(LCTN-V0.05)cathode.Furthermore,the corresponding cell can maintain stable operation up to 100 h without apparent performance degradation.These results demonstrate that doping-induced second nanophase exsolution is a promising way to design high-performance SOEC cathodes for CO_(2)electrolysis.展开更多
Inverted perovskite solar cells(PSCs)have stood out in recent years for their great potential in offering low-temperature compatibility,long-term stability and tandem cell suitability.However,challenges persist,partic...Inverted perovskite solar cells(PSCs)have stood out in recent years for their great potential in offering low-temperature compatibility,long-term stability and tandem cell suitability.However,challenges persist,particularly concerning the use of nickel oxide nanoparticles(NiO_(x)NPs)as the hole transport material,where issues such as low conductivity,impurity-induced aggregation and interface redox reactions significantly hinder device performance.In response,this study presents a novel synthesis method for NiO_(x)NPs,leveraging the introduction of ammonium salt dopants(NH_(4)Cl and NH_(4)SCN),and the solar cell utilizing the doped NiO_(x)substrate exhibits much enhanced device performance.Furthermore,doped solar cells reach 23.27%power conversion efficiency(PCE)when a self-assembled monolayer(SAM)is further employed.This study provides critical insights into the synthesis and growth pathways of NiO_(x)NPs,propelling the development of efficient hole transport materials for high-performance PSCs.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
Co-based alloy coating was prepared on Zr alloy using laser melting and cladding technique to study the difference in the high-temperature oxidation behavior between pure metal Co coatings and Co-T800 alloy coatings,a...Co-based alloy coating was prepared on Zr alloy using laser melting and cladding technique to study the difference in the high-temperature oxidation behavior between pure metal Co coatings and Co-T800 alloy coatings,as well as the wear resistance of the coatings.Besides,the effect of changing the laser melting process on the coatings was also investigated.The oxidation mass gain at 800–1200℃and the high-temperature oxidation behavior during high-temperature treatment for 1 h of two coated Zr alloy samples were studied.Results show that the Co coating and the Co-T800 coating have better resistance against high-temperature oxidation.After oxidizing at 1000℃for 1 h,the thickness of the oxide layer of the uncoated sample was 241.0μm,whereas that of the sample with Co-based coating is only 11.8–35.5μm.The friction wear test shows that the depth of the abrasion mark of the coated sample is only 1/2 of that of the substrate,indicating that the hardness and wear resistance of the Zr substrate are greatly improved.The disadvantage of Co-based coatings is the inferior corrosion resistance in 3.5wt%NaCl solution.展开更多
All-perovskite tandem solar cells(ATSCs) have the potential to surpass the Shockley-Queisser efficiency limit of conventional single-junction devices. However, the performance and stability of mixed tin–lead(Sn–Pb) ...All-perovskite tandem solar cells(ATSCs) have the potential to surpass the Shockley-Queisser efficiency limit of conventional single-junction devices. However, the performance and stability of mixed tin–lead(Sn–Pb) perovskite solar cells(PSCs), which are crucial components of ATSCs, are much lower than those of lead-based perovskites. The primary challenges include the high crystallization rate of perovskite materials and the susceptibility of Sn^(2+) oxidation, which leads to rough morphology and unfavorable p-type self-doping. To address these issues, we introduced ethylhydrazine oxalate(EDO) at the perovskite interface, which effectively inhibits the oxidation of Sn^(2+) and simultaneously enhances the crystallinity of the perovskite. Consequently, the EDO-modified mixed tin-lead PSCs reached a power conversion efficiency(PCE) of 21.96% with high reproducibility. We further achieved a 27.58% efficient ATSCs by using EDO as interfacial passivator in the Sn-Pb PSCs.展开更多
As a hole transport layer, PEDOT:PSS usually limits the stability and efficiency of perovskite solar cells(PSCs) due to its hygroscopic nature and inability to block electrons. Here, a graphene-oxide(GO)-modified PEDO...As a hole transport layer, PEDOT:PSS usually limits the stability and efficiency of perovskite solar cells(PSCs) due to its hygroscopic nature and inability to block electrons. Here, a graphene-oxide(GO)-modified PEDOT:PSS hole transport layer was fabricated by spin-coating a GO solution onto the PEDOT:PSS surface. PSCs fabricated on a GO-modified PEDOT:PSS layer exhibited a power conversion efficiency(PCE) of 15.34%, which is higher than 11.90% of PSCs with the PEDOT:PSS layer.Furthermore, the stability of the PSCs was significantly improved, with the PCE remaining at 83.5% of the initial PCE values after aging for 39 days in air. The hygroscopic PSS material at the PEDOT:PSS surface was partlyremoved during spin-coating with the GO solution, which improves the moisture resistance and decreases the contact barrier between the hole transport layer and perovskite layer. The scattered distribution of the GO at the PEDOT:PSS surface exhibits superior wettability, which helps to form a high-quality perovskite layer with better crystallinity and fewer pin holes. Furthermore, the hole extraction selectivity of the GO further inhibits the carrier recombination at the interface between the perovskite and PEDOT:PSS layers. Therefore, the cooperative interactions of these factors greatly improve the light absorption of the perovskite layer, the carrier transport and collection abilities of the PSCs, and especially the stability of the cells.展开更多
Several compounds of rare earth complex oxides containing manganese and titanium were synthesized in Ar, and their crystal structures were analyzed by powder X-ray diffraction data and Rietveld method. Structures of A...Several compounds of rare earth complex oxides containing manganese and titanium were synthesized in Ar, and their crystal structures were analyzed by powder X-ray diffraction data and Rietveld method. Structures of A0.67Ln0.33 Mn0.33Ti0.6703（A = Ca or Sr and Ln = rare earth） were found to have orthorhombic symmetry with the space group Pnrna, and their interatomic distances and bond angles were obtained. This space group was also derived from electron microscopic study. Electrical conductivity of Cao.67Ln0.33Mn0.33Ti0.6703 for several rare earth elements showed a semiconducting property with the activation energy of 0.4 eV. Some of these compounds of the strontium system show the antiferromagnetic properties below 10 K.展开更多
基金supported by Fundamental Research Funds for the Central Universities(2023KYJD1008)the Science Research Projects of the Anhui Higher Education Institutions of China(2022AH051582).
文摘Reversible solid oxide cell(RSOC)is a new energy conversion device with significant applications,especially for power grid peaking shaving.However,the reversible conversion process of power generation/energy storage poses challenges for the performance and stability of air electrodes.In this work,a novel high-entropy perovskite oxide La_(0.2)Pr_(0.2)Gd_(0.2)Sm_(0.2)Sr_(0.2)Co_(0.8)Fe_(0.2)O_(3−δ)(HE-LSCF)is proposed and investigated as an air electrode in RSOC.The electrochemical behavior of HE-LSCF was studied as an air electrode in both fuel cell and electrolysis modes.The polarization impedance(Rp)of the HE-LSCF electrode is only 0.25Ω·cm^(2) at 800℃ in an air atmosphere.Notably,at an electrolytic voltage of 2 V and a temperature of 800℃,the current density reaches up to 1.68 A/cm^(2).The HE-LSCF air electrode exhibited excellent reversibility and stability,and its electrochemical performance remains stable after 100 h of reversible operation.With these advantages,HE-LSCF is shown to be an excellent air electrode for RSOC.
基金funded by the National Science Centre,Poland,on the basis of the decision number UMO-2020/37/B/ST8/02097supported by the program“Excellence Initiative-Research University”for the AGH University of Krakow(IDUB AGH,No.501.696.7996,Action 4,ID 9880).
文摘Multicomponent Gd_(1−x)Sm_(x)Ba_(0.5)Sr_(0.5)CoCuO_(5+δ)double perovskites are optimized for application in terms of chemical composi-tion and morphology for the use as oxygen electrodes in solid oxide cells.Structural studies of other physicochemical properties are con-ducted on a series of materials obtained by the sol-gel method with different ratios of Gd and Sm cations.It is documented that changing the x value,and the resulting adjustment of the average ionic radius,have a significant impact on the crystal structure,stability,as well as on the total conductivity and thermomechanical properties of the materials,with the best results obtained for the Gd_(0.75)Sm_(0.2)5Ba_(0.5)Sr_(0.5)CoCuO_(5+δ)composition.Oxygen electrodes are prepared using the selected compound,allowing to obtain low polarization resistance values,such as 0.086Ω·cm^(2)at 800℃.Systematic studies of electrocatalytic activity are conducted using La_(0.8)Sr_(0.2)Ga_(0.8)Mg_(_(0.2))O_(3−δ)as the electrolyte for all electrodes,and Ce_(0.8)Gd_(0.2)O_(2−δ)electrolyte for the best performing Gd_(0.75)Sm_(0.2)5Ba_(0.5)Sr_(0.5)CoCuO_(5+δ)electrodes.The electrochemical data are analyzed using the distribution of relaxation times method.Also,the influence of the preparation method of the electrode material is in-ve`stigated using the electrospinning technique.Finally,the performance of the Gd_(0.75)Sm_(0.2)5Ba_(0.5)Sr_(0.5)CoCuO_(5+δ)electrodes is tested in a Ni-YSZ(yttria-stabilized zirconia)anode-supported cell with a Ce_(0.8)Gd_(0.2)O_(2−δ)buffer layer,in the fuel cell and electrolyzer operating modes.With the electrospun electrode,a power density of 462 mW·cm^(−2)is obtained at 700℃,with a current density of ca.0.2 A·cm^(−2)at 1.3 V for the electrolysis at the same temperature,indicating better performance compared to the sol-gel-based electrode.
基金Project supported by the National Natural Science Foundation of China(22279025,21773048,52302119)the Fundamental Research Funds for the Central Universities(2023FRFK06005,HIT.NSRIF202204)。
文摘Cation segregation on cathode surfaces plays a key role in determining the activity and operational stability of solid oxide fuel cells(SOFCs).The double perovskite oxide PrBa_(0.8)Ca_(0.2)Co_(2)O_(5+δ)(PBCC)has been widely studied as an active cathode but still suffer from serious detrimental segregations.To enhance the cathode stability,a PBCC derived A-site medium-entropy Pr_(0.6)La_(0.1)Nd_(0.1)Sm_(0.1)Gd_(0.1)Ba_(0.8)Ca_(0.2)Co_(2)O_(5+δ)(ME-PBCC)oxide was prepared and its segregation behaviors were investigated under different conditions.Compared with initial PBCC oxide,the segregations of BaO and Co_(3)O_(4)on the surface of ME-PBCC material are significantly suppressed,especially for Co_(3)O_(4),which is attributed to its higher configuration entropy.Our results also confirm the improved electrochemical performance and structural stability of ME-PBCC material,enabling it as a promising cathode for SOFCs.
文摘Introduction High-entropy oxides(HEOs)have attracted much attention in the field of electrochemistry due to their distinctive structural characteristics and unique properties.The multiple-principal elements in HEOs offer the multiple redox pairs and multiple possible active sites,which can enhance the energy storage capacity and the electrocatalytic performance.Although the notable progress is achieved in the development of HEOs electrodes,their electrochemical properties should be further improved to meet the requirements of high-performance supercapacitors and OER electrocatalysts.The abundant active sites for the Faradic redox reactions and short pathways for charge transportation could be constructed through the design of novel HEOs with advanced microstructures,thus improving the electrochemical properties.As advanced microstructures,a hollow structure has a great promise for energy storage and conversion because it can provide more accessible storage sites,more catalytic centers and a larger electrode/electrolyte contact area.It is thus expected that the construction of hollow structure is an alternative route to significantly promote the electrochemical properties of HEOs electrode materials.However,it is difficult to prepare the HEOs with a hollow structure due to the complexity of the high-entropy system.In this work,a hollow spherical high-entropy perovskite oxide of La(Cr_(0.2)Mn_(0.2)Fe_(0.2)Ni_(0.2)Cu_(0.2))O_(3)(HS-HEPs)was prepared by microwave solvothermal process and subsequent calcination treatment.The as-prepared HS-HEPs exhibited the excellent electrochemical performance when used as an electrode material for supercapacitors and OER electrocatalysts due to the advantages resulted from the combination of high-entropy perovskite and special hollow structure.Methods HS-HEPs were prepared by microwave solvothermal process and subsequent calcination treatment.Typically,0.134 mmol Cr(NO_(3))_(3)·6H_(2)O,0.134 mmol Mn(NO_(3))_(2)·4H_(2)O,0.134 mmol Fe(NO_(3))_(3)·9H_(2)O,0.134 mmol Ni(NO_(3))_(2)·6H_(2)O,0.134 mmol Cu(NO_(3))_(2)·3H_(2)O,and 0.5 mmol La(NO_(3))_(3)·6H_(2)O were dissolved in 30 mL ethanol under stirring for 1 h to obtain the homogeneous solution.Afterwards,60 mg of carbon spheres were added in the solution under ultrasonic treatment for 30 min.The resulting mixture was transferred to a 50 mL microwave digestion vessel.The vessel was heated in a microwave oven at a power of 210 W for 10 min.Subsequently,the obtained mixture was centrifuged,washed with deionized water,and dried in a vacuum drying oven at 70℃for 12 h.Finally,the obtained precursor powder was calcinated in a tube furnace with a heating rate of 3℃/min at 650℃for 2 h to acquire HS-HEPs.The crystalline structure of the sample was determined by X-ray diffraction(XRD,D8 Davinci,Bruker Co.,Germany).The morphology and microstructure of sample were characterized by field-emission scanning electron microscopy(FESEM,S-4800,Hitachi Co.Ltd.,Japan)equipped with energy dispersive X-ray spectroscopy(EDS)and transmission electron microscopy(TEM,2100F,JEOL Co.,Japan).The X-ray photoelectron spectra were obtained by a X-ray photoelectron spectrometry(XPS,ESCALab 250,Thermo VG Co.,USA).The supercapacitor and OER performance of the sample were measured on a CHI 660E electrochemical workstation(Shanghai Chenhua Instrument Co.,China).Results and discussion The as-prepared samples display a cubic perovskite crystalline structure and a hollow sphere morphology.According to the XPS analysis,the variable oxidation states of Cr,Fe and Mn present in the HS-HEPs,which benefits the Faradaic redox reactions and increases the capacitance.In addition,the existence of high concentration of oxygen vacancies in HS-HEPs is beneficial to enhancing the capacitance and OER activity.Based on the GCD curve,the specific capacitance of HS-HEPs is estimated to be 406 F/g at 1 A/g.After GCD cycles of 5000 at a current density of 5 A/g,65%capacitance is retained,implying a good long-term electrochemical stability.An asymmetric supercapacitor device(HS-HEPs//AC)with a two electrode configuration is assembled.A maximum energy density of 39.4 W·h/kg is achieved at power density of 746 W/kg.The OER activity of HS-HEPs is evaluated by a linear sweep voltammetry(LSV)polarization curve in 1 mol/L KOH aqueous solution using a standard three-electrode system.The overpotential of HS-HEPs is identified as 347 mV versus RHE for achieving a current density of 10 mA/cm^(2),which is smaller than that of commercial IrO2(372 mV).The HS-HEPs possess the excellent electrochemical performance,which can be ascribed to the high specific surface area,abundant active sites,and high oxygen vacancy content,resulting from the combination of high-entropy perovskite and special hollow structure.Conclusions High-entropy La(Cr_(0.2)Mn_(0.2)Fe_(0.2)Ni_(0.2)Cu_(0.2))O_(3)hollow spheres with a perovskite crystalline structure were prepared by microwave solvothermal process and subsequent calcination treatment.The HS-HEPs possessed the excellent electrochemical performance,which could be ascribed to the high specific surface area,abundant active sites,and high oxygen vacancy content,resulting from the combination of high-entropy perovskite and special hollow structure.Based on the electrochemical performance,HS-HEPs could be used as supercapacitor electrode material and OER electrocatalysts.This work could provide a strategy to design and prepare high-entropy oxides with a hollow sphere structure,having promising applications in energy storage and conversion.
基金financially supported by the National Natural Science Foundation of China (U2032157, 22209061)the Natural Science Foundation of Jiangsu Province (BK20201425)the Start-up Fund for Senior Talents in Jiangsu University(21JDG060)。
文摘Polycrystalline perovskite oxide particles are promising candidates for cathode materials in solid oxide fuel cells.However,their limited activity and stability pose significant challenges for practical applications.In this study,we demonstrate a novel approach to achieve both high activity and durability in a PrBaCo_(2)O_(5+δ) catalyst through a simple epitaxial layer growth strategy.We found that an amorphous precursor of the highly durable catalyst SmBa_(0.5)Ca_(0.5)CoCuO_(5+δ) can spontaneously adhere to the surface of PrBaCo_(2)O_(5+δ) particles.Upon heat treatment,it grows along the perovskite lattice,forming a heteroepitaxial layer with just a few atomic layers thickness.This heterostructure enhances the operational stability of PrBaCo_(2)O_(5+δ) transforming a 78% decrease over 100 h into a 7% increase.After 100 h,the power output density of the cell with the modified sample is more than 500% higher than that of unmodified PrBaCo_(2)O_(5+δ.)This work presents a new strategy for fabricating heteroepitaxial layers on polycrystalline ceramic catalysts and introduces a pioneering approach for developing high-performance oxygen reduction catalysts and related materials.
基金National Natural Science Foundation of China (NSFC)(52273266, U2001216)Shenzhen Science and Technology Innovation Committee (20231121102401001)+2 种基金Shenzhen Key Laboratory Project (ZDSYS201602261933302)GuangdongHong Kong-Macao Joint Laboratory on Micro-Nano Manufacturing Technology (2021LSYS004)SUSTech high level special funds (G03050K002)。
文摘Widely used spin-coated nickle oxide (NiOx) based perovskite solar cells often suffer from severe interfacial reactions between the NiOxand adjacent perovskite layers due to surface defect states,which inherently impair device performance in a long-term view,even with surface molecule passivation.In this study,we developed high-quality magnetron-sputtered NiOxthin films through detailed process optimization,and compared systematically sputtered and spin-coated NiOxthin film surfaces from materials to devices.These sputtered NiOxfilms exhibit improved crystallinity,smoother surfaces,and significantly reduced Ni3+or Ni vacancies compared to their spin-coated counterparts.Consequently,the interface between the perovskite and sputtered NiOxfilm shows a substantially reduced density of defect states.Perovskite solar cells (PSCs) fabricated with our optimally sputtered NiOxfilms achieved a high power conversion efficiency (PCE) of up to 19.93%and demonstrated enhanced stability,maintaining 86.2% efficiency during 500 h of maximum power point tracking under one standard sun illumination.Moreover,with the surface modification using (4-(2,7-dibromo-9,9-dimethylacridin-10(9H)-yl)butyl)p hosphonic acid (DMAcPA),the device PCE was further promoted to 23.07%,which is the highest value reported for sputtered NiOxbased PSCs so far.
基金financially supported by the National Key Research and Development Program(Nos.2022YFB2502104 and 2022YFA1602700)the Key Research and Development Program of Jiangsu Provincial Department of Science and Technology of China(No.BE2022332)+4 种基金the Jiangsu Carbon Peak Carbon Neutralization Science and Technology Innovation Special Fund(No.BE2022605)the National Natural Science Foundation of China(Nos.22109073,22379071)the DECRA program of Australian Research Council(No.DE230100357)the JSPS KAKENHI(No.JP23K13703)the Center for Computational Materials Science,Institute for Materials Research,Tohoku University for the use of MASAMUNE-IMR(202312-SCKXX-0203)。
文摘Perovskite oxides(ABO_(3))are thought to be promising electrocatalysts for oxygen evolution reaction(OER),but their specific surface area(SSA)is too low(usually<10 m^(2) g^(−1)).Developing advanced ABO_(3) electrocatalysts with high SSA and optimized structure is of great significance but remains a tremendous challenge.Herein,we propose a general strategy for fabrication of mesoporous perovskite oxide nanosheets(MPONs)with controllable atomic doping via self-sacrificial template-induced nanostructure modulation.A variety of MPONs including LaFeO_(3),A-site-doped LaFeO_(3)(A-LaFeO_(3),where A is Pr,Nd,Sm,Eu,or Gd)and B-site-doped LaFeO_(3)(B-LaFeO_(3),where B is Mn,Co,Ni,Cu,or Zn)have been achieved.Interestingly,it is discovered that the catalytic activities of A-LaFeO_(3) MPONs as OER catalysts are overall higher than those of B-LaFeO_(3) ones.Especially,the screened Eu-LaFeO_(3) MPONs only require a low overpotential of 267 mV at 10 mA cm^(−2),outperforming most reported perovskite oxides.The superior catalytic activity of Eu-LaFeO_(3) MPONs is attributed to their favorable porous structure,which increases the density of active sites,and enhanced lattice oxygen participation,which improves the intrinsic activity.This study provides guidance for the design and controlled synthesis of advanced rare-earth-doped MPONs with ultrahigh SSA for enhanced electrocatalysis.
基金supported by the National Natural Science Foundation of China(22279031)the Key Research and Development Plan of Hubei Province(2023BAB 109)+3 种基金the Longzhong Talent Planthe Joint Foundation for Innovation and Development of Hubei Natural Science Foundation(2022CFD079,2023AFD034 and 2023AFD032)Graduate Quality Engineering Funding Project of Hubei University of Arts and Sciences(YZ3202304)Independent Innovation Projects of the Hubei Longzhong Laboratory(2024KF-07 and 2024KF-33)。
文摘Premature perovskite films rapidly form at the FAI/PbI_(2)interface,inhibiting further reactions between FAI and PbI_(2)during the fabrication of perovskite films via the evaporating-spraying hybrid method according to our previous research.In this research,triphenylphosphine oxide(TPPO)was proved to be an effective coordinator that reduces the reaction rate between FAI and PbI_(2)at the initial stage,which can be attributed to the hydrogen(H)bonds between FA^(+)and TPPO,and coordinate bonds between TPPO and PbI_(2).Additionally,the quality of perovskite films improved significantly:the trap state density decreased from 1.6×10^(18)to 3.17×10^(17)cm^(-3),while the crystal size increased from 740 to 940 nm.The champion perovskite device achieved a remarkable efficiency of 20.93%(0.09 cm^(2))and 16.75%(63.7 cm^(2)),marking one of the highest reported results for the evaporating-spraying hybrid method.Moreover,the perovskite solar cells retained over 80%of their initial performances after 600 h of storage at 60℃in a nitrogen environment without encapsulation.It also maintained approximately 90%of its initial performance after continuous illumination at 25℃for 1400 h under the same conditions.
基金supported by the National Research Foundation of Korea(NRF)funded by the Korea government(MSIT)(NRF-RS-2023-00217270,RS-2023-00212744,and RS-2024-00436187)the Fundamental Research Program(PNKA390)of the Korean Institute of Materials Science(KIMS)+1 种基金the National Research Council of Science&Technology(NST)grant by the Korea govern-ment(MSIT)(No.GTL24041-000)the Energy Technology De-velopment Program of the Korean Institute of Energy Technology Evaluation and Planning(KETEP)(Grant No.RS-2023-00301944).
文摘The increasing demand for solar energy,driven by the climate crisis and carbon neutrality goals,un-derscores the critical importance of aesthetics in solar panel integration across diverse environments,such as building-integrated photovoltaics.This study addresses this need by developing angle-insensitive coloration for translucent perovskite-colored solar cells(TPCSCs)to enhance both functionality and con-sumer appeal.By engineering oxide/metal/oxide(OMO)multilayer structures,we achieved consistent col-oration regardless of the viewing angle,overcoming a major challenge in colored solar cell technology.Specifically,ZnO:Al/Ag/ZnO:Al-based OMO layers were meticulously optimized to balance visual appeal with photovoltaic efficiency.Our results demonstrate exceptional angular stability,with negligible color shifts observed even at viewing angles exceeding 60°,significantly surpassing the limitations of previ-ous designs,which exhibited sensitivity at 40°.The OMO electrodes exploited distributed Bragg reflector(DBR)properties to amplify interference effects and utilized delocalized plasmonic modes and metal-dielectric-metal(MDM)cavity resonances to achieve vibrant colors.Advanced 3-pair OMO transparent conductive electrodes(TCEs)exhibited stable,angle-insensitive blue coloration,and the resulting translu-cent perovskite solar cell achieved a record-high power conversion efficiency(PCE)of 8.25%and an av-erage transmittance of 15.23%,maintaining consistent coloration up to a 60°viewing angle.Additionally,the optoelectronic control layer(OCL)thickness was fine-tuned to precisely target specific wavelengths,enabling a versatile spectrum of colors,including blue,green,yellowish-green,orange,and peach.This pioneering approach not only ensures color fidelity but also enhances the reflectance properties of TPC-SCs.By integrating aesthetic and functional advancements,our research makes a significant contribution to the development of sustainable energy solutions for future smart cities.
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financial support from the National Natural Science Foundation of China (51872067 and 52472195)。
文摘The bifunctional oxygen evolution/reduction reaction(OER/ORR) performance of perovskite oxides in zinc-air batteries(ZABs) is fundamentally constrained by the unidirectional catalytic activity of B-site transition metal elements.This work proposes a heterostructure engineering strategy through selective etching to construct crystalline perovskite@amorphous hydroxide composites with spatially segregated active sites,where crystalline cores are for ORR and amorphous shells are for OER.Our investigation reveals that the differential solubility of alkaline-earth and rare-earth elements in acidic media enables precise control over surface amorphous layer composition and thickness through A-site cation ratio modulation and tailored etching protocols.Ab initio molecular dynamics(AIMD) simulations reveal the coupled process of A-site cations dissolution,oxygen vacancy formation,and amorphous-layer growth during the dynamic restructuring of the core-shell structure.The optimized Pr_(0.25)Sr_(0.75)FeO_(3-δ)@NiFe LDH achieved a 212 mV improvement of OER/ORR potential gap(ΔE=E_(10 mA cm-2)-E_(1/2)) over pristine Pr_(0.25)Sr_(0.75)FeO_(3-δ).When deployed in ZABs,the catalyst demonstrates a peak power density of 92.9 mW cm~(-2) and exceptional cycling stability with only 6.3% energy efficiency decay after 300 h(vs.10.2% decay for Pt/C-RuO_(2)).This work establishes a universal "composition-guided reconstruction" paradigm,providing both theoretical insights and practical solutions for high-performance electrode design of ZABs.
基金supported by the National Natural Science Foundation of China(No.52472270)the Basic Research Program of Jiangsu(No.BK20243049)the Fundamental Research Funds for the Central Universities(No.2023KYJD1010).
文摘The performance of the fuel electrode in a solid oxide electrolysis cell(SOEC)is crucial to facilitating fuel gas electrolysis and is the key determinant of overall electrolysis efficiency.Nevertheless,the commercialization of integrated CO_(2)-H_(2)O electrolysis in SOEC remains constrained by suboptimal catalytic efficiency and long-term stability limitations inherent to conventional fuel electrode architec-tures.A novel high-entropy Sr_(2)FeTi_(0.2)Cr_(0.2)Mn_(0.2)Mo_(0.2)Co_(0.2)O_(6−δ)(SFTCMMC)was proposed as a prospective electrode material of co-elec-trolysis in this work.The physicochemical properties and electrochemical performance in the co-electrolysis reaction were investigated.Full cell is capable of electrolyzing H_(2)O and CO_(2)effectively with an applied voltage.The effects of temperature,H_(2)O and CO_(2)concentra-tions,and applied voltage on the electrochemical performance of Sc_(0.18)Zr_(0.82)O_(2−δ)(SSZ)-electrolyte supported SOEC were investigated by varying the operating conditions.The SOEC obtains a favorable electrolysis current density of 1.47 A·cm^(−2)under co-electrolysis condi-tion at 850℃ with 1.5 V.Furthermore,the cell maintains stable performance for 150 h at 1.3 V,and throughout this period,no carbon de-position is detected.The promising findings suggest that the high-entropy SFTCMMC perovskite is a viable fuel electrode candidate for efficient H_(2)O/CO_(2)co-electrolysis.
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Project supported by the National Key Research&Development Project(2023YFB4006001)National Natural Science Foundation of China(52172199)。
文摘CO_(2)electrolysis using solid oxide electrolysis cells is a promising technology for CO_(2)utilization and conversion,which has attracted more and more attention in recent years because of its extremely high efficiency.However,traditional Ni-yttria-stabilized zirconia(Ni-YSZ)or Ni-Gd_(0.1)Ce_(0.9)O_(2-δ)(Ni-GDC)metal-ceramic cathode faces many problems such as Ni agglomeration and carbon deposition during long-time operation.Herein,a perovskite oxide La_(0.43-x)Ca_(0.37)Ti_(0.9)Ni_(0.1)O_(3-δ)(LCTN,x=0,0.05,0.1)with nanophase-LaVO_(4)exsolution was investigated as the novel cathode of solid oxide electrolysis cell(SOEC)for efficient CO_(2)electrolysis.The results confirm that the exsolution nanophase on LCTN surface can significantly improve the CO_(2)adsorption and conversion performance.For CO_(2)electrolysis at 1.8 V,an electrolysis current density of 1.24 A/cm2at 800℃can be obtained on SOEC with La_(0.43-x)Ca_(0.37)Ti_(0.9)Ni_(0.1)O_(3-δ)decorated with LaVO_(4)(LCTN-V0.05)cathode.Furthermore,the corresponding cell can maintain stable operation up to 100 h without apparent performance degradation.These results demonstrate that doping-induced second nanophase exsolution is a promising way to design high-performance SOEC cathodes for CO_(2)electrolysis.
基金supported by the Open Research Fund of Songshan Lake Materials Laboratory(No.2021SLABFK09)the National Natural Science Foundation of China(No.22109093)+1 种基金the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning and the Shanghai Rising-Star Program(No.19QA1403800)the Project of Innovative Development Agency of Republic of Uzbekistan(No.FZ-20200929177)and Shanghai Technical Service Computing Center of Science and Engineering,Shanghai University.
文摘Inverted perovskite solar cells(PSCs)have stood out in recent years for their great potential in offering low-temperature compatibility,long-term stability and tandem cell suitability.However,challenges persist,particularly concerning the use of nickel oxide nanoparticles(NiO_(x)NPs)as the hole transport material,where issues such as low conductivity,impurity-induced aggregation and interface redox reactions significantly hinder device performance.In response,this study presents a novel synthesis method for NiO_(x)NPs,leveraging the introduction of ammonium salt dopants(NH_(4)Cl and NH_(4)SCN),and the solar cell utilizing the doped NiO_(x)substrate exhibits much enhanced device performance.Furthermore,doped solar cells reach 23.27%power conversion efficiency(PCE)when a self-assembled monolayer(SAM)is further employed.This study provides critical insights into the synthesis and growth pathways of NiO_(x)NPs,propelling the development of efficient hole transport materials for high-performance PSCs.
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National Natural Science Foundation of China(52071126)Natural Science Foundation of Tianjin City,China(22JCQNJC01240)+2 种基金Central Guidance on Local Science and Technology Development Fund of Hebei Province(226Z1009G)Special Funds for Science and Technology Innovation in Hebei(2022X19)Anhui Provincial Natural Science Foundation(2308085ME135)。
文摘Co-based alloy coating was prepared on Zr alloy using laser melting and cladding technique to study the difference in the high-temperature oxidation behavior between pure metal Co coatings and Co-T800 alloy coatings,as well as the wear resistance of the coatings.Besides,the effect of changing the laser melting process on the coatings was also investigated.The oxidation mass gain at 800–1200℃and the high-temperature oxidation behavior during high-temperature treatment for 1 h of two coated Zr alloy samples were studied.Results show that the Co coating and the Co-T800 coating have better resistance against high-temperature oxidation.After oxidizing at 1000℃for 1 h,the thickness of the oxide layer of the uncoated sample was 241.0μm,whereas that of the sample with Co-based coating is only 11.8–35.5μm.The friction wear test shows that the depth of the abrasion mark of the coated sample is only 1/2 of that of the substrate,indicating that the hardness and wear resistance of the Zr substrate are greatly improved.The disadvantage of Co-based coatings is the inferior corrosion resistance in 3.5wt%NaCl solution.
基金financially supported by National Key R&D Program of China (2025YFE0100300)the National Natural Science Foundation of China (52202293 and 52330004)the Fundamental Research Funds for the Central Universities (WUT: 2023IVA075 and 2023IVB009)。
文摘All-perovskite tandem solar cells(ATSCs) have the potential to surpass the Shockley-Queisser efficiency limit of conventional single-junction devices. However, the performance and stability of mixed tin–lead(Sn–Pb) perovskite solar cells(PSCs), which are crucial components of ATSCs, are much lower than those of lead-based perovskites. The primary challenges include the high crystallization rate of perovskite materials and the susceptibility of Sn^(2+) oxidation, which leads to rough morphology and unfavorable p-type self-doping. To address these issues, we introduced ethylhydrazine oxalate(EDO) at the perovskite interface, which effectively inhibits the oxidation of Sn^(2+) and simultaneously enhances the crystallinity of the perovskite. Consequently, the EDO-modified mixed tin-lead PSCs reached a power conversion efficiency(PCE) of 21.96% with high reproducibility. We further achieved a 27.58% efficient ATSCs by using EDO as interfacial passivator in the Sn-Pb PSCs.
基金supported by National Natural Science Foundation of China(Grant Nos.61275038 and 11274119)
文摘As a hole transport layer, PEDOT:PSS usually limits the stability and efficiency of perovskite solar cells(PSCs) due to its hygroscopic nature and inability to block electrons. Here, a graphene-oxide(GO)-modified PEDOT:PSS hole transport layer was fabricated by spin-coating a GO solution onto the PEDOT:PSS surface. PSCs fabricated on a GO-modified PEDOT:PSS layer exhibited a power conversion efficiency(PCE) of 15.34%, which is higher than 11.90% of PSCs with the PEDOT:PSS layer.Furthermore, the stability of the PSCs was significantly improved, with the PCE remaining at 83.5% of the initial PCE values after aging for 39 days in air. The hygroscopic PSS material at the PEDOT:PSS surface was partlyremoved during spin-coating with the GO solution, which improves the moisture resistance and decreases the contact barrier between the hole transport layer and perovskite layer. The scattered distribution of the GO at the PEDOT:PSS surface exhibits superior wettability, which helps to form a high-quality perovskite layer with better crystallinity and fewer pin holes. Furthermore, the hole extraction selectivity of the GO further inhibits the carrier recombination at the interface between the perovskite and PEDOT:PSS layers. Therefore, the cooperative interactions of these factors greatly improve the light absorption of the perovskite layer, the carrier transport and collection abilities of the PSCs, and especially the stability of the cells.
基金Foundation ite ms:Project supported bythe Grant-in-Aidfor Scientific Research (C) (18560662) bythe Japan Societyfor the Promotion of Science
文摘Several compounds of rare earth complex oxides containing manganese and titanium were synthesized in Ar, and their crystal structures were analyzed by powder X-ray diffraction data and Rietveld method. Structures of A0.67Ln0.33 Mn0.33Ti0.6703（A = Ca or Sr and Ln = rare earth） were found to have orthorhombic symmetry with the space group Pnrna, and their interatomic distances and bond angles were obtained. This space group was also derived from electron microscopic study. Electrical conductivity of Cao.67Ln0.33Mn0.33Ti0.6703 for several rare earth elements showed a semiconducting property with the activation energy of 0.4 eV. Some of these compounds of the strontium system show the antiferromagnetic properties below 10 K.
