Bi-based perovskite ferroelectric thin films have wide applications in electronic devices due to their excellent ferroelectric properties.New Bi-based perovskite thin films Bi(Cu_(1/2)Ti_(1/2))O_(3)–PbTiO_(3)(BCT–PT...Bi-based perovskite ferroelectric thin films have wide applications in electronic devices due to their excellent ferroelectric properties.New Bi-based perovskite thin films Bi(Cu_(1/2)Ti_(1/2))O_(3)–PbTiO_(3)(BCT–PT) are deposited on Pt(111)/Ti/SiO_(2)/Si substrates in the present study by the traditional sol–gel method.Their structures and related ferroelectric and fatigue characteristics are studied in-depth.The BCT–PT thin films exhibit good crystallization within the phase-pure perovskite structure,besides,they have a predominant(100) orientation together with a dense and homogeneous microstructure.The remnant polarization(2P_(r)) values at 30 μC/cm^(2) and 16 μC/cm^(2) are observed in 0.1BCT–0.9PT and 0.2BCT–0.8PT thin films,respectively.More intriguingly,although the polarization values are not so high,0.2BCT–0.8PT thin films show outstanding polarization fatigue properties,with a high switchable polarization of 93.6% of the starting values after 10^(8) cycles,indicating promising applications in ferroelectric memories.展开更多
Crystallization process determines the quality of perovskite films and the performances of resultant perovskite solar cells(PSCs).Dimethylamine oxalate has been proven as a multifunctional modulator,and is explored as...Crystallization process determines the quality of perovskite films and the performances of resultant perovskite solar cells(PSCs).Dimethylamine oxalate has been proven as a multifunctional modulator,and is explored as an efficient additive in manipulating the crystallization process of CsPbI_(3) perovskite films.On one hand,oxalate serves as the precipitator that facilitates the nucleation process of intermediate.The larger size of intermediate is conductive to the larger size and smaller grain boundaries of resultant perovskite.On the other hand,in subsequent annealing process,the phase conversion and growth process of transient perovskite can be decelerated due to the strong interactions of oxalate with both dimethylamine cation(DMA^(+))and Pb^(2+).Due to the optimized crystallization kinetics,the morphology and quality of CsPbI_(3) perovskite films are comprehensively improved with lower defect concentrations,and charge recombination loss is effectively suppressed.Benefiting from the optimized crystal quality of perovskite films,the carbon electrode-based CsPbI_(3) PSCs exhibit a champion efficiency of 18.48%.This represents one of the highest levels among all hole transport layer-free inorganic perovskite solar cells.展开更多
Perovskite type of PbTiO 3 fine powders which are homogeneous in physic chemical properties has been hydrothermally synthesized from the different precursors. The borderline reaction conditions, such as temperature...Perovskite type of PbTiO 3 fine powders which are homogeneous in physic chemical properties has been hydrothermally synthesized from the different precursors. The borderline reaction conditions, such as temperature and time, for the formation of PbTiO 3 were established and the effect of the precursor on the particle properties was investigated. As a precursor, Pb Ti alko carbonate xerogel dispersed in 2 methoxyethanol was found to be effective for the synthesis of the PbTiO 3 powders with a lower agglomeration and a simple mode of particle size.展开更多
Formamidine lead triiodide(FAPbI_(3))perovskites have become the most promising photovoltaic materials for perovskite solar cells with record power conversion efficiency(PCE).However,random nucleation,phase transition...Formamidine lead triiodide(FAPbI_(3))perovskites have become the most promising photovoltaic materials for perovskite solar cells with record power conversion efficiency(PCE).However,random nucleation,phase transition,and lattice defects are still the key challenges limiting the quality of FAPbI_(3) films.Previous studies show that the introduction or adding of seeds in the precursor is effective to promote the nucleation and crystallization of perovskite films.Nevertheless,the seed-assisted approach focuses on heterogeneous seeds or hetero-composites,which inevitably induce a lattice-mismatch,the genera-tion of strain or defects,and the phase segregation in the perovskite films.Herein,we first demonstrate that high-quality perovskite films are controllably prepared using α-and δ-phases mixed FAPbI_(3) micro-crystal as the homogeneous seeds with the one-step antisolvent method.The partially dissolved seeds with suitable sizes improve the crystallinity of the perovskite flm with preferable orientation,improved carrier lifetime,and increased carrier mobility.More importantly,the α-phase-containing seeds promote the formation of α-phase FAPbI_(3) films,leading to the reduction of residual lattice strain and the suppres-sion of I-ion migration.Besides,the adding of dimethyl 2,6-pyridine dicarboxylate(DPD)into the pre-cursor further suppresses the generation of defects,contributing to the PCE of devices prepared in air ambient being significantly improved to 23.75%,among the highest PCEs for fully air-processed FAPbI_(3) solar cells.The unpackaged target devices possess a high stability,maintaining 80%of the initial PCE under simulated solar illumination exceeding 800 h.展开更多
Hole transport material free carbon-based all-inorganic CsPbBr_(3)perovskite solar cells(PSCs)are promising for commercialization due to its low-cost,high open-circuit voltage(V_(oc))and superior stability.Due to the ...Hole transport material free carbon-based all-inorganic CsPbBr_(3)perovskite solar cells(PSCs)are promising for commercialization due to its low-cost,high open-circuit voltage(V_(oc))and superior stability.Due to the different solubility of PbBr_(2)and CsBr in conventional solvents,CsPbBr_(3)films are mainly obtained by multi-step spin-coating through the phase evolution from PbBr_(2)to CsPb_(2)Br_(5)and then to CsPbBr_(3).The scalable fabrication of high-quality CsPbBr_(3)films has been rarely studied.Herein,an inkjet-printing method is developed to prepare high-quality CsPbBr_(3)films.The formation of long-range crystalline CsPb_(2)Br_(5)phase can effectively improve phase purity and promote regular crystal stacking of CsPbBr_(3).Consequently,the inkjet-printed CsPbBr_(3)C-PSCs realized PCEs up to 9.09%,8.59%and 7.81%with active areas of 0.09,0.25,and 1 cm^(2),respectively,demonstrating the upscaling potential of our fabrication method and devices.This high performance is mainly ascribed to the high purity,strong crystal orientation,reduced surface roughness and lower trap states density of the as-printed CsPbBr_(3)films.This work provides insights into the relationship between the phase evolution mechanisms and crystal growth dynamics of cesium lead bromide halide films.展开更多
Advanced photovoltaics,such as ultra-flexible perovskite solar cells(UF-PSCs),which are known for their lightweight design and high power-to-mass ratio,have been a long-standing goal that we,as humans,have continuousl...Advanced photovoltaics,such as ultra-flexible perovskite solar cells(UF-PSCs),which are known for their lightweight design and high power-to-mass ratio,have been a long-standing goal that we,as humans,have continuously pursued.Unlike normal PSCs fabricated on rigid substrates,producing high-efficiency UF-PSCs remains a challenge due to the difficulty in achieving full coverage and minimizing defects of metal halide perovskite(MHP)films.In this study,we utilized Al_(2)O_(3) nanoparticles(NPs)as an inorganic surface modifier to enhance the wettability and reduce the roughness of poly-bis(4-phenyl)(2,4,6-trimethylphenyl)amine simultaneously.This approach proves essentials in fabricating UF-PSCs,enabling the deposition of uniform and dense MHP films with full coverage and fewer defects.We systematically investigated the effect of Al_(2)O_(3) NPs on film formation,combining simulation with experiments.Our strategy not only significantly increases the power conversion efficiency(PCE)from 11.96%to 16.33%,but also promotes reproducibility by effectively addressing the short circuit issue commonly encountered in UF-PSCs.Additionally,our UF-PSCs demonstrates good mechanical stability,maintaining 98.6%and 79.0%of their initial PCEs after 10,000 bending cycles with radii of 1.0 and 0.5 mm,respectively.展开更多
CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS acti...CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS activity for perovskite systems based on AFeO_(3)(where A=Ce,La,Y).These systems were synthesized by solution combustion synthesis(SCS)with diff erent ratios of fuel(glycine)and oxidizer(φ),diff erent amounts of NH 4 NO_(3),and the addition of alumina or silica as supports.Various techniques,including X-ray diff raction analysis,thermogravimetric analysis,Fourier transform infrared spectroscopy(FTIR),scanning electron microscopy,energy-dispersive X-ray spectroscopy,N 2-physisorption,H_(2) temper-ature-programmed reduction,temperature-programmed desorption of H_(2) and CO_(2),Raman spectroscopy,and in situ FTIR,were used to relate the physicochemical properties with the catalytic performance of the obtained composites.Each specifi c perovskite-containing system(either bulk or supported)has its own optimalφand NH_(4) NO_(3) amount to achieve the highest yield and dispersion of the perovskite phase.Among all synthesized systems,bulk SCS-derived La-Fe-O systems showed the highest resistance to reducing environments and the easiest hydrogen desorption,outperforming La-Fe-O produced by solgel combustion(SGC).CO_(2) conversion into CO at 600°C for bulk ferrite systems,depending on the A-cation type and preparation method,follows the order La(SGC)<Y<Ce<La(SCS).The diff erences in properties between La-Fe-O obtained by the SCS and SGC methods can be attributed to diff erent ratios of oxygen and lanthanum vacancy contributions,hydroxyl coverage,morphology,and free iron oxide presence.In situ FTIR data revealed that CO_(2) hydrogenation occurs through formates generated under reaction conditions on the bulk system based on La-Fe-O,obtained by the SCS method.γ-Al_(2)O_(3) improves the dispersion of CeFeO_(3) and LaFeO_(3) phases,the specifi c surface area,and the quantity of adsorbed H_(2) and CO_(2).This led to a signifi cant increase in CO_(2) conversion for supported CeFeO_(3) but not for the La-based system compared to bulk and SiO_(2)-supported perovskite catalysts.However,adding alumina increased the activity per mass for both Ce-and La-based perovskite systems,reducing the amount of rare-earth components in the catalyst and thereby lowering the cost without substantially compromising stability.展开更多
The utilization of perovskite oxide materials as catalysts for the photodegradation of organic pollutants in water is a promising and rapidly advancing field.In this study,a series of La_(1−x)Ba_(x)CoO_(3)(x=0.2,0.3,0...The utilization of perovskite oxide materials as catalysts for the photodegradation of organic pollutants in water is a promising and rapidly advancing field.In this study,a series of La_(1−x)Ba_(x)CoO_(3)(x=0.2,0.3,0.4,0.5,0.6)catalysts with varying Ba doping ratios were synthesized using the citric acid complexation-hydrothermal synthesis combined method for the degradation of phenol under visible light irradiation.Among the synthesized catalysts,La_(0.5)Ba_(0.5)CoO_(3) exhibited the highest photocatalytic activity.In addition,the photocatalytic mechanism for La_(0.5)Ba_(0.5)CoO_(3) perovskite degradation of phenol was also discussed.The synthesized catalysts were characterized using XRD,SEM,FT-IR,XPS,MPMS and other characterization techniques.The results revealed that the diffraction peak intensity of La_(1−x)Ba_(x)CoO_(3) increased with higher Ba doping ratios,and the La_(0.4)Ba_(0.6)CoO_(3) exhibited the strongest diffraction peaks.The catalyst particle sizes ranged from 10 to 50 nm,and the specific surface area decreased with increasing Ba content.Additionally,the paramagnetic properties of La_(0.5)Ba_(0.5)CoO_(3) were similar to that of La_(0.4)Ba_(0.6)CoO_(3).The experimental results suggested that the incorporation of Ba could significantly improve the catalytic performance of La_(1−x)Ba_(x)CoO_(3) perovskites,promote electron transfer and favor to the generation of hydroxyl radicals(•OH),leading to the efficiently degradation of phenol.展开更多
Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the...Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the use of Ca_(2)MnO_(4)-layered perovskites modified with NaNO_(3) dopants,serving as redox catalysts(also known as oxygen carriers),for the CL-ODH of ethane within a temperature range of 700-780℃.Our findings revealed that the incorporation of NaNO_(3) as a modifier significantly-nhanced the selectivity for-thylene generation from Ca_(2)MnO_(4).At 750℃and a gas hourly space velocity of 1300 h^(-1),we achieved an-thane conversion up to 68.17%,accompanied by a corresponding-thylene yield of 57.39%.X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO_(3) onto Ca_(2)MnO_(4) not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox catalyst.Furthermore,formation of NaNO_(3) shell on the surface of Ca_(2)MnO_(4) led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise manner.This modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO_(3)-doped Ca_(2)MnO_(4) catalyst.These findings provide compelling evidence for the potential of Ca_(2)MnO_(4)-layered perovskites as promising redox catalysts in the context of CL-ODH reactions.展开更多
基金Project supported by the National Key Research and Development Program of China(Grant No.2021YFA1400300)the National Natural Science Foundation of China(Grant Nos.22271309,21805215,11934017,12261131499,and 11921004)+1 种基金the Beijing Natural Science Foundation(Grant No.Z200007)the Fund from the Chinese Academy of Sciences(Grant No.XDB33000000)。
文摘Bi-based perovskite ferroelectric thin films have wide applications in electronic devices due to their excellent ferroelectric properties.New Bi-based perovskite thin films Bi(Cu_(1/2)Ti_(1/2))O_(3)–PbTiO_(3)(BCT–PT) are deposited on Pt(111)/Ti/SiO_(2)/Si substrates in the present study by the traditional sol–gel method.Their structures and related ferroelectric and fatigue characteristics are studied in-depth.The BCT–PT thin films exhibit good crystallization within the phase-pure perovskite structure,besides,they have a predominant(100) orientation together with a dense and homogeneous microstructure.The remnant polarization(2P_(r)) values at 30 μC/cm^(2) and 16 μC/cm^(2) are observed in 0.1BCT–0.9PT and 0.2BCT–0.8PT thin films,respectively.More intriguingly,although the polarization values are not so high,0.2BCT–0.8PT thin films show outstanding polarization fatigue properties,with a high switchable polarization of 93.6% of the starting values after 10^(8) cycles,indicating promising applications in ferroelectric memories.
基金supported by the National Natural Science Foundation of China(Nos.U21A20310,22278164,22122805,22308112)the Science and Technology Program of Guangzhou,China(No.2023A04J0665)China Postdoctoral Science Foundation(No.2023M741214)。
文摘Crystallization process determines the quality of perovskite films and the performances of resultant perovskite solar cells(PSCs).Dimethylamine oxalate has been proven as a multifunctional modulator,and is explored as an efficient additive in manipulating the crystallization process of CsPbI_(3) perovskite films.On one hand,oxalate serves as the precipitator that facilitates the nucleation process of intermediate.The larger size of intermediate is conductive to the larger size and smaller grain boundaries of resultant perovskite.On the other hand,in subsequent annealing process,the phase conversion and growth process of transient perovskite can be decelerated due to the strong interactions of oxalate with both dimethylamine cation(DMA^(+))and Pb^(2+).Due to the optimized crystallization kinetics,the morphology and quality of CsPbI_(3) perovskite films are comprehensively improved with lower defect concentrations,and charge recombination loss is effectively suppressed.Benefiting from the optimized crystal quality of perovskite films,the carbon electrode-based CsPbI_(3) PSCs exhibit a champion efficiency of 18.48%.This represents one of the highest levels among all hole transport layer-free inorganic perovskite solar cells.
文摘Perovskite type of PbTiO 3 fine powders which are homogeneous in physic chemical properties has been hydrothermally synthesized from the different precursors. The borderline reaction conditions, such as temperature and time, for the formation of PbTiO 3 were established and the effect of the precursor on the particle properties was investigated. As a precursor, Pb Ti alko carbonate xerogel dispersed in 2 methoxyethanol was found to be effective for the synthesis of the PbTiO 3 powders with a lower agglomeration and a simple mode of particle size.
基金supported by the National Natural Science Foundation of China (61604131,62025403)the Natural Science Foundation of Zhejiang Province (LY19F040009)+1 种基金the Fundamental Research Funds of Zhejiang SciTech University (23062120-Y)the Open Project of Key Laboratory of Solar Energy Utilization and Energy Saving Technology of Zhejiang Province (ZJS-OP-2020-07)
文摘Formamidine lead triiodide(FAPbI_(3))perovskites have become the most promising photovoltaic materials for perovskite solar cells with record power conversion efficiency(PCE).However,random nucleation,phase transition,and lattice defects are still the key challenges limiting the quality of FAPbI_(3) films.Previous studies show that the introduction or adding of seeds in the precursor is effective to promote the nucleation and crystallization of perovskite films.Nevertheless,the seed-assisted approach focuses on heterogeneous seeds or hetero-composites,which inevitably induce a lattice-mismatch,the genera-tion of strain or defects,and the phase segregation in the perovskite films.Herein,we first demonstrate that high-quality perovskite films are controllably prepared using α-and δ-phases mixed FAPbI_(3) micro-crystal as the homogeneous seeds with the one-step antisolvent method.The partially dissolved seeds with suitable sizes improve the crystallinity of the perovskite flm with preferable orientation,improved carrier lifetime,and increased carrier mobility.More importantly,the α-phase-containing seeds promote the formation of α-phase FAPbI_(3) films,leading to the reduction of residual lattice strain and the suppres-sion of I-ion migration.Besides,the adding of dimethyl 2,6-pyridine dicarboxylate(DPD)into the pre-cursor further suppresses the generation of defects,contributing to the PCE of devices prepared in air ambient being significantly improved to 23.75%,among the highest PCEs for fully air-processed FAPbI_(3) solar cells.The unpackaged target devices possess a high stability,maintaining 80%of the initial PCE under simulated solar illumination exceeding 800 h.
基金supported by the National Key Research and Development Program of China(Grant Nos.2021YFB3800100 and 2021YFB3800101)the National Natural Science Foundation of China(62004089,U2001217,and U19A2089)+6 种基金the Guangdong Basic and Applied Basic Research Foundation(2019A1515110439,2019B1515120083,and2022A1515011218)the Shenzhen Science and Technology Program(JCYJ20190809150811504 and KQTD2015033110182370)the HKRGC General Research Funds(16312216)the Shenzhen&Hong Kong Joint Research Program(SGLH20180622092406130)the Shenzhen Engineering Research and Development Center for Flexible Solar Cel s Project funding from Shenzhen Development and Reform Committee(2019-126)the Key Fundamental Research Project funding from the Shenzhen Science and Technology Innovation Committee(JCYJ20200109141014474)the Guangdong-Hong Kong-Macao Joint Laboratory(2019B121205001)
文摘Hole transport material free carbon-based all-inorganic CsPbBr_(3)perovskite solar cells(PSCs)are promising for commercialization due to its low-cost,high open-circuit voltage(V_(oc))and superior stability.Due to the different solubility of PbBr_(2)and CsBr in conventional solvents,CsPbBr_(3)films are mainly obtained by multi-step spin-coating through the phase evolution from PbBr_(2)to CsPb_(2)Br_(5)and then to CsPbBr_(3).The scalable fabrication of high-quality CsPbBr_(3)films has been rarely studied.Herein,an inkjet-printing method is developed to prepare high-quality CsPbBr_(3)films.The formation of long-range crystalline CsPb_(2)Br_(5)phase can effectively improve phase purity and promote regular crystal stacking of CsPbBr_(3).Consequently,the inkjet-printed CsPbBr_(3)C-PSCs realized PCEs up to 9.09%,8.59%and 7.81%with active areas of 0.09,0.25,and 1 cm^(2),respectively,demonstrating the upscaling potential of our fabrication method and devices.This high performance is mainly ascribed to the high purity,strong crystal orientation,reduced surface roughness and lower trap states density of the as-printed CsPbBr_(3)films.This work provides insights into the relationship between the phase evolution mechanisms and crystal growth dynamics of cesium lead bromide halide films.
基金supported by the National Natural Science Foundation of China(22005043,52272193)the National Key Research and Development Program of China(2019YFA0709102 and 2020YFA0714502)+1 种基金the Liaoning Revitalization Talents Program(XLYC2007038,XLYC2008032)the Fundamental Research Funds for the Central Universities(DUT22LAB602,DUT22GJ201).
文摘Advanced photovoltaics,such as ultra-flexible perovskite solar cells(UF-PSCs),which are known for their lightweight design and high power-to-mass ratio,have been a long-standing goal that we,as humans,have continuously pursued.Unlike normal PSCs fabricated on rigid substrates,producing high-efficiency UF-PSCs remains a challenge due to the difficulty in achieving full coverage and minimizing defects of metal halide perovskite(MHP)films.In this study,we utilized Al_(2)O_(3) nanoparticles(NPs)as an inorganic surface modifier to enhance the wettability and reduce the roughness of poly-bis(4-phenyl)(2,4,6-trimethylphenyl)amine simultaneously.This approach proves essentials in fabricating UF-PSCs,enabling the deposition of uniform and dense MHP films with full coverage and fewer defects.We systematically investigated the effect of Al_(2)O_(3) NPs on film formation,combining simulation with experiments.Our strategy not only significantly increases the power conversion efficiency(PCE)from 11.96%to 16.33%,but also promotes reproducibility by effectively addressing the short circuit issue commonly encountered in UF-PSCs.Additionally,our UF-PSCs demonstrates good mechanical stability,maintaining 98.6%and 79.0%of their initial PCEs after 10,000 bending cycles with radii of 1.0 and 0.5 mm,respectively.
基金The research was carried out within the State Assignment of the Ministry of Science and Higher Education of the Russian Federation(project No.FFUG-2024-0036)。
文摘CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS activity for perovskite systems based on AFeO_(3)(where A=Ce,La,Y).These systems were synthesized by solution combustion synthesis(SCS)with diff erent ratios of fuel(glycine)and oxidizer(φ),diff erent amounts of NH 4 NO_(3),and the addition of alumina or silica as supports.Various techniques,including X-ray diff raction analysis,thermogravimetric analysis,Fourier transform infrared spectroscopy(FTIR),scanning electron microscopy,energy-dispersive X-ray spectroscopy,N 2-physisorption,H_(2) temper-ature-programmed reduction,temperature-programmed desorption of H_(2) and CO_(2),Raman spectroscopy,and in situ FTIR,were used to relate the physicochemical properties with the catalytic performance of the obtained composites.Each specifi c perovskite-containing system(either bulk or supported)has its own optimalφand NH_(4) NO_(3) amount to achieve the highest yield and dispersion of the perovskite phase.Among all synthesized systems,bulk SCS-derived La-Fe-O systems showed the highest resistance to reducing environments and the easiest hydrogen desorption,outperforming La-Fe-O produced by solgel combustion(SGC).CO_(2) conversion into CO at 600°C for bulk ferrite systems,depending on the A-cation type and preparation method,follows the order La(SGC)<Y<Ce<La(SCS).The diff erences in properties between La-Fe-O obtained by the SCS and SGC methods can be attributed to diff erent ratios of oxygen and lanthanum vacancy contributions,hydroxyl coverage,morphology,and free iron oxide presence.In situ FTIR data revealed that CO_(2) hydrogenation occurs through formates generated under reaction conditions on the bulk system based on La-Fe-O,obtained by the SCS method.γ-Al_(2)O_(3) improves the dispersion of CeFeO_(3) and LaFeO_(3) phases,the specifi c surface area,and the quantity of adsorbed H_(2) and CO_(2).This led to a signifi cant increase in CO_(2) conversion for supported CeFeO_(3) but not for the La-based system compared to bulk and SiO_(2)-supported perovskite catalysts.However,adding alumina increased the activity per mass for both Ce-and La-based perovskite systems,reducing the amount of rare-earth components in the catalyst and thereby lowering the cost without substantially compromising stability.
基金The Fundamental Research Program for Young Scientists of Shanxi Province(Project No.202103021223294)The Fundamental Research Program of Shanxi Province(Project No.202203021211203)+1 种基金The Start-up Fund for Doctorate Scientific Research Project of Taiyuan University of Science and Technology(Project No.20232124)The Innovation and Entrepreneurship Training Program for Undergraduate,Taiyuan University of Science and Technology(Project No.DCX2024162).
文摘The utilization of perovskite oxide materials as catalysts for the photodegradation of organic pollutants in water is a promising and rapidly advancing field.In this study,a series of La_(1−x)Ba_(x)CoO_(3)(x=0.2,0.3,0.4,0.5,0.6)catalysts with varying Ba doping ratios were synthesized using the citric acid complexation-hydrothermal synthesis combined method for the degradation of phenol under visible light irradiation.Among the synthesized catalysts,La_(0.5)Ba_(0.5)CoO_(3) exhibited the highest photocatalytic activity.In addition,the photocatalytic mechanism for La_(0.5)Ba_(0.5)CoO_(3) perovskite degradation of phenol was also discussed.The synthesized catalysts were characterized using XRD,SEM,FT-IR,XPS,MPMS and other characterization techniques.The results revealed that the diffraction peak intensity of La_(1−x)Ba_(x)CoO_(3) increased with higher Ba doping ratios,and the La_(0.4)Ba_(0.6)CoO_(3) exhibited the strongest diffraction peaks.The catalyst particle sizes ranged from 10 to 50 nm,and the specific surface area decreased with increasing Ba content.Additionally,the paramagnetic properties of La_(0.5)Ba_(0.5)CoO_(3) were similar to that of La_(0.4)Ba_(0.6)CoO_(3).The experimental results suggested that the incorporation of Ba could significantly improve the catalytic performance of La_(1−x)Ba_(x)CoO_(3) perovskites,promote electron transfer and favor to the generation of hydroxyl radicals(•OH),leading to the efficiently degradation of phenol.
基金support of National Natural Science Foundation of China(22179027)gratefully acknowledged.This work was also supported by the Natural Science Foundation of Guangxi Province(2021GXNSFAA075063,2018GXNSFDA281005)+1 种基金the National Key Research and Development Program of China(2017YFE0105500)Science&Technology Research Project of Guangdong Province(2017A020216009).
文摘Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the use of Ca_(2)MnO_(4)-layered perovskites modified with NaNO_(3) dopants,serving as redox catalysts(also known as oxygen carriers),for the CL-ODH of ethane within a temperature range of 700-780℃.Our findings revealed that the incorporation of NaNO_(3) as a modifier significantly-nhanced the selectivity for-thylene generation from Ca_(2)MnO_(4).At 750℃and a gas hourly space velocity of 1300 h^(-1),we achieved an-thane conversion up to 68.17%,accompanied by a corresponding-thylene yield of 57.39%.X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO_(3) onto Ca_(2)MnO_(4) not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox catalyst.Furthermore,formation of NaNO_(3) shell on the surface of Ca_(2)MnO_(4) led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise manner.This modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO_(3)-doped Ca_(2)MnO_(4) catalyst.These findings provide compelling evidence for the potential of Ca_(2)MnO_(4)-layered perovskites as promising redox catalysts in the context of CL-ODH reactions.
