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 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
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
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
Chemical looping oxidative dehydrogenation (CL-ODH) is an economically promising method for convertingethane into higher value-added ethylene utilizing lattice oxygen in redox catalysts, also known as oxygen carriers....Chemical looping oxidative dehydrogenation (CL-ODH) is an economically promising method for convertingethane into higher value-added ethylene utilizing lattice oxygen in redox catalysts, also known as oxygen carriers. Inthis study, perovskite-type oxide SrCoO_(3-δ) and B-site Mn ion-doped oxygen carriers (SrCo_(1-x)MnxO_(3-δ), x=0.1, 0.2, 0.3)were prepared and tested for the CL-ODH of ethane. The oxygen-deficient perovskite SrCoO_(3-δ) exhibited high ethyleneselectivity of up to 96.7% due to its unique oxygen vacancies and lattice oxygen migration rates. However, its low ethyleneyield limits its application in the CL-ODH of ethane. Mn doping promoted the reducibility of SrCoO_(3-δ) oxygen carriers,thereby improving ethane conversion and ethylene yield, as demonstrated by characterization and evaluation experiments.X-ray diffraction results confirmed the doping of Mn into the lattice of SrCoO_(3-δ), while X-ray photoelectron spectroscopy(XPS) indicated an increase in lattice oxygen ratio upon incorporation of Mn into the SrCoO_(3-δ) lattice. Additionally, H2temperature-programmed reduction (H2-TPR) tests revealed more peaks at lower temperature reduction zones and a declinein peak positions at higher temperatures. Among the four tested oxygen carriers, SrCo0.8Mn0.2O_(3-δ) exhibited satisfactoryperformance with an ethylene yield of 50% at 710 °C and good stability over 20 redox cycles. The synergistic effect of Mnplays a key role in increasing ethylene yields of SrCoO_(3-δ) oxygen carriers. Accordingly, SrCo0.8Mn0.2O_(3-δ) shows promisingpotential for the efficient production of ethylene from ethane via CL-ODH.展开更多
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
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
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
Tin-lead(Sn-Pb)mixed perovskites are extensively investigated in near-infrared(NIR)photodetectors(PDs)owing to their excellent photoelectric performance.However,achieving high-performance Sn-Pb mixed PDs remains chall...Tin-lead(Sn-Pb)mixed perovskites are extensively investigated in near-infrared(NIR)photodetectors(PDs)owing to their excellent photoelectric performance.However,achieving high-performance Sn-Pb mixed PDs remains challenging,primarily because of the rapid crystallization and the susceptibility of Sn^(2+) to oxidation.To ad⁃dress these issues,this study introduces the multifunctional molecules 2,3-difluorobenzenamine(DBM)to modulate the crystallization of Sn-Pb mixed perovskites and retard the oxidation of Sn^(2+),thereby significantly enhancing film quality.Compared with the pristine film,Sn-Pb mixed perovskite films modulated by DBM molecules exhibit a high⁃ly homogeneous morphology,reduced roughness and defect density.The self-powered NIR PDs fabricated with the improved films have a spectral response range from 300 nm to 1100 nm,a peak responsivity of 0.51 A·W^(-1),a spe⁃cific detectivity as high as 2.46×10^(11)Jones within the NIR region(780 nm to 1100 nm),a linear dynamic range ex⁃ceeding 152 dB,and ultrafast rise/fall time of 123/464 ns.Thanks to the outstanding performance of PDs,the fabri⁃cated 5×5 PDs array demonstrates superior imaging ability in the NIR region up to 980 nm.This work advances the development of Sn-Pb mixed perovskites for NIR detection and paves the way for their commercialization.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
Sustainable and clean hydrogen development has been considered a mainstream trend in contemporary energy research.Heterogenous photo(electro)catalysis is a promising approach to producing hydrogen in an environmentall...Sustainable and clean hydrogen development has been considered a mainstream trend in contemporary energy research.Heterogenous photo(electro)catalysis is a promising approach to producing hydrogen in an environmentally friendly manner.Perovskites have emerged as an inexpensive,earth-abundant,and easily fabricated semiconductor material for photo(electro)catalysis.However,some of their shortcomings have limited the wide range of applications.In this mini-review,we present the fundamentals and applications of various perovskites for photo(electro)catalytic water splitting.In addition,we summarize advanced strategies for photo(electro)catalytic water splitting based on perovskites,focusing on the following approaches:intrinsic modulation of perovskites,functionalization of perovskites,and design of perovskite tandem systems.In summary,we point out the challenges and potential applications for perovskite solar water splitting and systematically describe various strategies to improve the photo(electro)catalysis performance of perovskites,illustrating the potential of using perovskites as key materials for solar water splitting.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
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 double perovskite Cs_(2)SnI_(6)has notable optical and electrical characteristics,rendering it a highly prospective candidate for deployment as the absorber layer in perovskite solar cells(PSCs).We simulated the p...The double perovskite Cs_(2)SnI_(6)has notable optical and electrical characteristics,rendering it a highly prospective candidate for deployment as the absorber layer in perovskite solar cells(PSCs).We simulated the performance of PSCs using lead-free Cs_(2)SnI_(6)double perovskite absorber layer and graphene derivatives,namely graphene oxide(GO)and reduced graphene oxide(rGO),as hole transport layers(HTLs).Our findings show that r GO offers an excellent hole extraction property with minimal interfacial recombination compared to GO.展开更多
Despite the rapid efficiency increase,tin halide perovskite solar cells are significantly behind their lead-based counterpart,with the highest reported efficiency of 15.38%.The main reason for this large difference is...Despite the rapid efficiency increase,tin halide perovskite solar cells are significantly behind their lead-based counterpart,with the highest reported efficiency of 15.38%.The main reason for this large difference is attributed to the instability of Sn^(2+),which easily oxidizes to Sn^(4+),creating Sn vacancies and increasing the open-circuit voltage loss.In this work,we implemented tin thiocyanate(Sn(SCN)_(2))as an additive for passivating the bulk defects of a germanium-doped tin halide perovskite film.Adding Sn^(2+)and SCN-ions reduces the Sn and iodine vacancies,limiting non-radiative recombination and favoring longer charge-carrier dynamics.Moreover,the addition of Sn(SCN)_(2) induces a higher film crystallinity and preferential orientation of the(l00)planes parallel to the substrate.The passivated devices showed improved photovoltaic parameters with the best open-circuit voltage of 0.716 V and the best efficiency of 12.22%,compared to 0.647 V and 10.2%for the reference device.In addition,the passivated solar cell retains 88.7%of its initial efficiency after 80 min of illumination under 100 mW cm^(-2) and is substantially better than the control device,which reaches 82.6%of its initial power conversion efficiency only after 30 min.This work demonstrates the passivation potential of tin-based additives,which combined with different counterions give a relatively large space of choices for passivation of Sn-based perovskites.展开更多
Surface regulation is a crucial technique for improving catalytic performance in heterogeneous catalysis.Although perovskite oxides containing noble metals show good performance and excellent thermal stability,the enc...Surface regulation is a crucial technique for improving catalytic performance in heterogeneous catalysis.Although perovskite oxides containing noble metals show good performance and excellent thermal stability,the encapsulation of noble metals in perovskite lattice restricts the exposure/usage of active sites.Herein,a method of high-temperature calcination coupling with selective dissolution was adopted to tune the physicochemical environment on the LaPd_(0.1)Mn_(0.9)O_(3)catalyst surface.The X-ray diffraction(XRD)and Raman results reveal that more Pd species emerge on the surface by elevating the calcination temperature,resulting in improved catalytic toluene oxidation activity.A further acid-etching of the LPMO-900 catalyst can also boost catalytic performance,being attributed to the enhanced redox ability and abundant surface oxygen vacancies.In addition,the optimized catalyst also exhibits excellent resistance to sintering and water vapor.This study provides new avenues for the rational design of highly efficient perovskite-based catalysts.展开更多
Tin oxide has emerged as a promising electron transport material in perovskite solar cells due to its high conductivity and photostability.However,the inherent defects in SnO_(2)nanoparticles and their imperfect bondi...Tin oxide has emerged as a promising electron transport material in perovskite solar cells due to its high conductivity and photostability.However,the inherent defects in SnO_(2)nanoparticles and their imperfect bonding with perovskite at the interface lead to additional energy loss.To achieve bifacial passivation on the SnO_(2)electron transport layer and the SnO_(2)/perovskite interface synchronously,a multifunctional surface modulation strategy has been developed by incorporating O-phospho-L-serine monolithium salt(PSLi)to regulate the SnO_(2)nanoparticles.PS-Li coordinates with SnO_(2)through the phosphate/carboxyl groups,with the exposed amino group passivating the uncoordinated lead ions at the interface.The introduction of a lithium ion further regulates the energy band of SnO_(2),accelerating electron extraction and transport.This multifunctional modulation strategy reduces trap states from tin dangling bonds and oxygen vacancies,enhancing film conductivity.It also regulates the growth of the perovskite crystal and reduces nonradiative recombination at the interface.Consequently,the optimized perovskite solar cells achieve power conversion efficiencies(PCEs)of 24.91% for small-area devices and 23.14% for minimodules(aperture area of 30 cm^(2)).The unencapsulated device retains 91% and 89% of its initial PCE after enduring 1000 h under ambient conditions,and 500 h under 1 sun illumination in N2atmosphere,respectively.展开更多
Inverted perovskite solar cells,which nickel oxide(NiOx)has been widely employed as a hole transport layer,have shown promise for perovskite-silicon tandem solar cells.However,the deficient quality of perovskite/NiOx ...Inverted perovskite solar cells,which nickel oxide(NiOx)has been widely employed as a hole transport layer,have shown promise for perovskite-silicon tandem solar cells.However,the deficient quality of perovskite/NiOx interface has constrained the performance and stability of the solar cells.In this paper,low-temperature atomic layer deposition(ALD)was employed to prepare a nanometer aluminum oxide(Al_(2)O_(3))layer that effectively blocks carriers recombination,facilitates carriers transport by improving the valence band maximum(VBM)alignment between HTL and perovskite and enhances the morphology of self-assembled monolayer(SAM).The interface between NiO_(x)and perovskite was modified by the embedded Al_(2)O_(3)layer,achieving an open current voltage(Voc)of 1.19 V and a short-circuit current density(J_(sc))of 22.98 mA cm^(-2).The efficiency of the champion cell was 22.22%at 1.5 AM(0.2 cm^(2)),which was a notable enhancement compared to solar cells of average power conversion efficiency(PCE)20.33%without Al_(2)O_(3)passivation layer.The passivated perovskite solar cell exhibits enhanced stability in degradation tests,retaining 85.70%of the initial PCE after storage in ambient air(40%-60%relative humidity(R.H.))at 25℃for 100 h.The results show the potential of low-temperature ALD-Al_(2)O_(3)in inverted perovskite solar cells as well as perovskite-silicon tandem solar cells.展开更多
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 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 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.
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.
基金the SINOPEC Research and Development Project(No.JR22094).
文摘Chemical looping oxidative dehydrogenation (CL-ODH) is an economically promising method for convertingethane into higher value-added ethylene utilizing lattice oxygen in redox catalysts, also known as oxygen carriers. Inthis study, perovskite-type oxide SrCoO_(3-δ) and B-site Mn ion-doped oxygen carriers (SrCo_(1-x)MnxO_(3-δ), x=0.1, 0.2, 0.3)were prepared and tested for the CL-ODH of ethane. The oxygen-deficient perovskite SrCoO_(3-δ) exhibited high ethyleneselectivity of up to 96.7% due to its unique oxygen vacancies and lattice oxygen migration rates. However, its low ethyleneyield limits its application in the CL-ODH of ethane. Mn doping promoted the reducibility of SrCoO_(3-δ) oxygen carriers,thereby improving ethane conversion and ethylene yield, as demonstrated by characterization and evaluation experiments.X-ray diffraction results confirmed the doping of Mn into the lattice of SrCoO_(3-δ), while X-ray photoelectron spectroscopy(XPS) indicated an increase in lattice oxygen ratio upon incorporation of Mn into the SrCoO_(3-δ) lattice. Additionally, H2temperature-programmed reduction (H2-TPR) tests revealed more peaks at lower temperature reduction zones and a declinein peak positions at higher temperatures. Among the four tested oxygen carriers, SrCo0.8Mn0.2O_(3-δ) exhibited satisfactoryperformance with an ethylene yield of 50% at 710 °C and good stability over 20 redox cycles. The synergistic effect of Mnplays a key role in increasing ethylene yields of SrCoO_(3-δ) oxygen carriers. Accordingly, SrCo0.8Mn0.2O_(3-δ) shows promisingpotential for the efficient production of ethylene from ethane via CL-ODH.
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.
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Supported by National Key Research and Development Program of China(2022YFA1404201)National Natural Science Foundation of China(62205187,U23A20380,U22A2091,62222509,62127817,62075120)+3 种基金Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China(IRT_17R70)Fundamental Research Program of Shanxi Province(202103021223032,202303021222031)Project Funded by China Postdoctoral Science Foundation(2022M722006)Fund for Shanxi“1331 Project”Key Subjects Construction。
文摘Tin-lead(Sn-Pb)mixed perovskites are extensively investigated in near-infrared(NIR)photodetectors(PDs)owing to their excellent photoelectric performance.However,achieving high-performance Sn-Pb mixed PDs remains challenging,primarily because of the rapid crystallization and the susceptibility of Sn^(2+) to oxidation.To ad⁃dress these issues,this study introduces the multifunctional molecules 2,3-difluorobenzenamine(DBM)to modulate the crystallization of Sn-Pb mixed perovskites and retard the oxidation of Sn^(2+),thereby significantly enhancing film quality.Compared with the pristine film,Sn-Pb mixed perovskite films modulated by DBM molecules exhibit a high⁃ly homogeneous morphology,reduced roughness and defect density.The self-powered NIR PDs fabricated with the improved films have a spectral response range from 300 nm to 1100 nm,a peak responsivity of 0.51 A·W^(-1),a spe⁃cific detectivity as high as 2.46×10^(11)Jones within the NIR region(780 nm to 1100 nm),a linear dynamic range ex⁃ceeding 152 dB,and ultrafast rise/fall time of 123/464 ns.Thanks to the outstanding performance of PDs,the fabri⁃cated 5×5 PDs array demonstrates superior imaging ability in the NIR region up to 980 nm.This work advances the development of Sn-Pb mixed perovskites for NIR detection and paves the way for their commercialization.
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supported by the National Natural Science Foundation of China (No.62204067)Young Talent Support Project of Guangzhou Association for Science and Technology (No.QT-2023-051)+2 种基金industry support from Shenzhen Jinjia jituan Co.,Ltd with funding No.R00043the financial support from the Science and Technology Development Fund,Macao SAR (File no.FDCT-0125/2022/A and FDCT-0006/2023/RIB1)the National Natural Science Foundation of China (No.22305009)
文摘Sustainable and clean hydrogen development has been considered a mainstream trend in contemporary energy research.Heterogenous photo(electro)catalysis is a promising approach to producing hydrogen in an environmentally friendly manner.Perovskites have emerged as an inexpensive,earth-abundant,and easily fabricated semiconductor material for photo(electro)catalysis.However,some of their shortcomings have limited the wide range of applications.In this mini-review,we present the fundamentals and applications of various perovskites for photo(electro)catalytic water splitting.In addition,we summarize advanced strategies for photo(electro)catalytic water splitting based on perovskites,focusing on the following approaches:intrinsic modulation of perovskites,functionalization of perovskites,and design of perovskite tandem systems.In summary,we point out the challenges and potential applications for perovskite solar water splitting and systematically describe various strategies to improve the photo(electro)catalysis performance of perovskites,illustrating the potential of using perovskites as key materials for solar water splitting.
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.
文摘The double perovskite Cs_(2)SnI_(6)has notable optical and electrical characteristics,rendering it a highly prospective candidate for deployment as the absorber layer in perovskite solar cells(PSCs).We simulated the performance of PSCs using lead-free Cs_(2)SnI_(6)double perovskite absorber layer and graphene derivatives,namely graphene oxide(GO)and reduced graphene oxide(rGO),as hole transport layers(HTLs).Our findings show that r GO offers an excellent hole extraction property with minimal interfacial recombination compared to GO.
基金support from the Focus Group‘Next Generation Organic Photovoltaics’participating with the Dutch Institute for Fundamental Energy Research(DIFFER)(FOM130)Advanced Materials research program of the Zernike National Research Centre under the Bonus Incentive Scheme(BIS)of the Dutch Ministry for Education,Culture and Science.
文摘Despite the rapid efficiency increase,tin halide perovskite solar cells are significantly behind their lead-based counterpart,with the highest reported efficiency of 15.38%.The main reason for this large difference is attributed to the instability of Sn^(2+),which easily oxidizes to Sn^(4+),creating Sn vacancies and increasing the open-circuit voltage loss.In this work,we implemented tin thiocyanate(Sn(SCN)_(2))as an additive for passivating the bulk defects of a germanium-doped tin halide perovskite film.Adding Sn^(2+)and SCN-ions reduces the Sn and iodine vacancies,limiting non-radiative recombination and favoring longer charge-carrier dynamics.Moreover,the addition of Sn(SCN)_(2) induces a higher film crystallinity and preferential orientation of the(l00)planes parallel to the substrate.The passivated devices showed improved photovoltaic parameters with the best open-circuit voltage of 0.716 V and the best efficiency of 12.22%,compared to 0.647 V and 10.2%for the reference device.In addition,the passivated solar cell retains 88.7%of its initial efficiency after 80 min of illumination under 100 mW cm^(-2) and is substantially better than the control device,which reaches 82.6%of its initial power conversion efficiency only after 30 min.This work demonstrates the passivation potential of tin-based additives,which combined with different counterions give a relatively large space of choices for passivation of Sn-based perovskites.
基金Project supported by the National Key R&D Program of China(2023YFC3710300)the National Natural Science Foundation of China(U23A2099,22276111)+1 种基金the Taishan Scholar Project of Shandong Province(202306031)the Natural Science Foundation of Shandong Province(2023HWYQ-024)。
文摘Surface regulation is a crucial technique for improving catalytic performance in heterogeneous catalysis.Although perovskite oxides containing noble metals show good performance and excellent thermal stability,the encapsulation of noble metals in perovskite lattice restricts the exposure/usage of active sites.Herein,a method of high-temperature calcination coupling with selective dissolution was adopted to tune the physicochemical environment on the LaPd_(0.1)Mn_(0.9)O_(3)catalyst surface.The X-ray diffraction(XRD)and Raman results reveal that more Pd species emerge on the surface by elevating the calcination temperature,resulting in improved catalytic toluene oxidation activity.A further acid-etching of the LPMO-900 catalyst can also boost catalytic performance,being attributed to the enhanced redox ability and abundant surface oxygen vacancies.In addition,the optimized catalyst also exhibits excellent resistance to sintering and water vapor.This study provides new avenues for the rational design of highly efficient perovskite-based catalysts.
基金financially supported by the Science Foundation of the Chinese Academy of Sciences。
文摘Tin oxide has emerged as a promising electron transport material in perovskite solar cells due to its high conductivity and photostability.However,the inherent defects in SnO_(2)nanoparticles and their imperfect bonding with perovskite at the interface lead to additional energy loss.To achieve bifacial passivation on the SnO_(2)electron transport layer and the SnO_(2)/perovskite interface synchronously,a multifunctional surface modulation strategy has been developed by incorporating O-phospho-L-serine monolithium salt(PSLi)to regulate the SnO_(2)nanoparticles.PS-Li coordinates with SnO_(2)through the phosphate/carboxyl groups,with the exposed amino group passivating the uncoordinated lead ions at the interface.The introduction of a lithium ion further regulates the energy band of SnO_(2),accelerating electron extraction and transport.This multifunctional modulation strategy reduces trap states from tin dangling bonds and oxygen vacancies,enhancing film conductivity.It also regulates the growth of the perovskite crystal and reduces nonradiative recombination at the interface.Consequently,the optimized perovskite solar cells achieve power conversion efficiencies(PCEs)of 24.91% for small-area devices and 23.14% for minimodules(aperture area of 30 cm^(2)).The unencapsulated device retains 91% and 89% of its initial PCE after enduring 1000 h under ambient conditions,and 500 h under 1 sun illumination in N2atmosphere,respectively.
基金supported by the Special Fund for Science and Technology Innovation of Jiangsu Province(No.BE2022022-1)the Natural Science Foundation of Guangdong Province(No.2022A1515011722).
文摘Inverted perovskite solar cells,which nickel oxide(NiOx)has been widely employed as a hole transport layer,have shown promise for perovskite-silicon tandem solar cells.However,the deficient quality of perovskite/NiOx interface has constrained the performance and stability of the solar cells.In this paper,low-temperature atomic layer deposition(ALD)was employed to prepare a nanometer aluminum oxide(Al_(2)O_(3))layer that effectively blocks carriers recombination,facilitates carriers transport by improving the valence band maximum(VBM)alignment between HTL and perovskite and enhances the morphology of self-assembled monolayer(SAM).The interface between NiO_(x)and perovskite was modified by the embedded Al_(2)O_(3)layer,achieving an open current voltage(Voc)of 1.19 V and a short-circuit current density(J_(sc))of 22.98 mA cm^(-2).The efficiency of the champion cell was 22.22%at 1.5 AM(0.2 cm^(2)),which was a notable enhancement compared to solar cells of average power conversion efficiency(PCE)20.33%without Al_(2)O_(3)passivation layer.The passivated perovskite solar cell exhibits enhanced stability in degradation tests,retaining 85.70%of the initial PCE after storage in ambient air(40%-60%relative humidity(R.H.))at 25℃for 100 h.The results show the potential of low-temperature ALD-Al_(2)O_(3)in inverted perovskite solar cells as well as perovskite-silicon tandem solar cells.
