The insurmountable charge transfer impedance at the Li metal/solid polymer electrolytes(SPEs)interface at room temperature as well as the ascending risk of short circuits at the operating temperature higher than the m...The insurmountable charge transfer impedance at the Li metal/solid polymer electrolytes(SPEs)interface at room temperature as well as the ascending risk of short circuits at the operating temperature higher than the melting point,dominantly limits their applications in solid-state batteries(SSBs).Although the inorganic filler such as CeO_(2)nanoparticle content of composite solid polymer electrolytes(CSPEs)can significantly reduce the enormous charge transfer impedance at the Li metal/SPEs interface,we found that the required content of CeO_(2)nanoparticles in SPEs varies for achieving a decent interfacial charge transfer impedance and the bulk ionic conductivity in CSPEs.In this regard,a sandwich-type composited solid polymer electrolyte with a 10%CeO_(2)CSPEs interlayer sandwiched between two 50%CeO_(2)CSPEs thin layers(sandwiched CSPEs)is constructed to simultaneously achieve low charge transfer impedance and superior ionic conductivity at 30℃.The sandwiched CSPEs allow for stable cycling of Li plating and stripping for 1000 h with 129 mV polarized voltage at 0.1 mA cm^(-2)and 30℃.In addition,the LiFePO_(4)/Sandwiched CSPEs/Li cell also exhibits exceptional cycle performance at 30℃and even elevated120℃without short circuits.Constructing multi-layered CSPEs with optimized contents of the inorganic fillers can be an efficient method for developing all solid-state PEO-based batteries with high performance at a wide range of temperatures.展开更多
Constructing heterojunction interface as an active catalyst is an effective strategy to boost electrocatalytic activity of oxygen evolution reaction(OER).Herein,we report an interfacial CoP/CeO_(2)heterostructure cata...Constructing heterojunction interface as an active catalyst is an effective strategy to boost electrocatalytic activity of oxygen evolution reaction(OER).Herein,we report an interfacial CoP/CeO_(2)heterostructure catalyst constructed by interface engineering and selective phosphorization procedure.X-ray photoelectron spectroscopy(XPS)suggests that coupling CeO_(2)nanoparticles on the surface of CoP will generate interfacial interaction at the two-phase interface,resulting in electron transfer between CoP and CeO_(2)components at the interface.Benefitting from the interfacial interaction,large exposed interface area,and luxuriant mesopores structure,CoP/CeO_(2)shows fascinating alkaline OER performance.At the current densities of 10 and 50 mA cm^(−2),the optimal CoP/CeO_(2)heterojunction exhibits lower overpotential(257 and 298 mV)than either CoP(288 and 354 mV)or RuO_(2)(305 and 409 mV).This work provides a facile synthetic protocol for constructing heterostructure interfaces to improve OER performance.展开更多
With the continuous tightening of automotive emission regulations and the increasing promotion of energy-efficient hybrid vehicles,new challenges have arisen for the low-temperature performance of three-way catalysts(...With the continuous tightening of automotive emission regulations and the increasing promotion of energy-efficient hybrid vehicles,new challenges have arisen for the low-temperature performance of three-way catalysts(TWCs).To guide the design of next-generation TWCs,it is essential to further develop our understanding of the relationships between microstructure and catalytic performance.Here,Rh/CeO_(2)–ZrO_(2) catalysts were synthesized with different Rh metal dispersion by using a combination of the wet impregnation method and reduction treatment.These catalysts included Rh single-atom catalysts,cluster catalysts,and nanoparticle catalysts.The results showed that the Rh nanoparticle catalyst,with an average size of 1.9 nm,exhibited superior three-way catalytic performance compared to the other catalysts.Based on the catalytic activity in a series of simple reaction atmospheres such as CO+O_(2),NO+CO,and hydrocarbons(HCs)+O_(2) and operando infrared spectroscopy,we found that metallic Rh sites on Rh nanoparticles are the key factor responsible for the low-temperature catalytic performance.展开更多
Electrocatalytic nitrate reduction reaction(NO_(3)−RR)emerges as a highly efficient approach toward ammonia synthesis and degrading NO_(3)−contaminant.In our study,CeO_(2) nanoparticles with oxygen vacancies(VO)decora...Electrocatalytic nitrate reduction reaction(NO_(3)−RR)emerges as a highly efficient approach toward ammonia synthesis and degrading NO_(3)−contaminant.In our study,CeO_(2) nanoparticles with oxygen vacancies(VO)decorated N-doped carbon nanorods on graphite paper(CeO_(2)−x@NC/GP)were demonstrated as a highly efficient NO_(3)−RR electrocatalyst.The CeO_(2)−x@NC/GP catalyst manifests a significant NH_(3 )yield up to 712.75μmol·h^(−1)·cm^(−2) at−0.8 V vs.reversible hydrogen electrode(RHE)and remarkable Faradaic efficiency of 92.93%at−0.5 V vs.RHE under alkaline conditions,with excellent durability.Additionally,an assembled Zn-NO_(3)−battery with CeO_(2)−x@NC/GP as cathode accomplishes a high-power density of 3.44 mW·cm^(−2) and a large NH3 yield of 145.08μmol·h^(−1)·cm^(−2).Density functional theory results further expose the NO_(3)−reduction mechanism on CeO_(2)(111)surface with VO.展开更多
In current work,Ni-Ti-CeO_(2) nanocomposite coatings were achieved by co-adding Ti microparticles and CeO_(2) nanoparticles.Designed experiments and COMSOL computer simulation were applied to reveal the synergistic ro...In current work,Ni-Ti-CeO_(2) nanocomposite coatings were achieved by co-adding Ti microparticles and CeO_(2) nanoparticles.Designed experiments and COMSOL computer simulation were applied to reveal the synergistic role of Ti microparticles and CeO_(2) nanoparticles in tailoring the spatial microstructures and properties of Ni-Ti-CeO_(2) nanocomposite coating.Unilaterally,the conductive Ti microparticles conducted the growth behavior of Ni grains by current density concentration,distorting electronic feld lines and heterogeneous nucleation.Individual domains consisting of inner nanograins and outer radial columnar grains surrounded Ti microparticles,where Ti microparticles acted as seeds.Ti microparticles tended to be aggregated,leading to spatial heterogeneity of microstructures.Ni deposits buried the Ti microparticles in forms of“covering model”,contributing to the formation of inside voids and rough surface and aggregation of Ti microparticles;on the other hand,the non-conductive CeO_(2)microparticles hardly changed the distribution of current density and electronic feld lines on the cathode surface.Ni deposits buried the CeO_(2)microparticle in forms of“stacking model”,avoiding the inside voids and aggregation of particles.The incorporation of CeO_(2)microparticle brought in microstructure evolutions only on its top side without disturbing the growth behavior of Ni grains on its lateral side or bottom,suggesting the limited effects.This was correlated with the presence of current concentration above the CeO_(2) microparticle at the last stage of burying CeO_(2) microparticle.The co-addition of Ti microparticles and CeO_(2) nanoparticles into Ni deposits exploited the complementary action of the two particles,which gave birth to satisfed spatial microstructures and improved hardness.Ti microparticles took major responsibility for microstructure evolutions,while the CeO_(2) nanoparticles were mainly in charge of the microstructure homogeneity.展开更多
A series of transition metals(Fe,Co,Ni,Cu,Cr and Mn)-doped CeO_(2)-TiO_(2) catalysts were prepared by the sol-gel method and applied for the catalytic removal of 1,2-dichloroethane(DCE) as a model for chlorinated VOCs...A series of transition metals(Fe,Co,Ni,Cu,Cr and Mn)-doped CeO_(2)-TiO_(2) catalysts were prepared by the sol-gel method and applied for the catalytic removal of 1,2-dichloroethane(DCE) as a model for chlorinated VOCs(CVOCs).The various characterization methods including X-ray diffraction(XRD),N_(2) adsorption-desorption,UV-Raman,NH_(3) temperature-programmed desorption(NH_(3)-TPD) and H_(2) temperature-programmed reduction(H_(2)-TPR) were utilized to investigate the physicochemical properties of the catalysts.The results show that doping Fe,Co,Ni or Mn can obviously promote the activity of CeO_(2)-TiO_(2) mixed oxides for DCE degradation,which is related to their improved texture properties,acid sites(especially for strong acidity) and low-temperature reducibility.Particularly,CeTi-Fe doped with moderate Fe exhibits excellent activity for 1,2-dichloroethane(DCE) degradation,giving a T_(90%) value as low as 250℃.More importantly,only trace chlorinated byproducts were produced during the low-temperature degradation of various CVOCs(dichloromethane(DCM),trichloroethylene(TCE) and chlorobenzene(CB)) over CeTi-Fe1/9 catalyst with high durability.展开更多
Herein,we prepared a bimetallic layered double hydroxide(FeCo LDH)featuring a dandelion-like structure.Anchoring of CeO_(2)onto FeCo LDH produced interfaces between the functionalizing CeO_(2)and the parent LDH.Compar...Herein,we prepared a bimetallic layered double hydroxide(FeCo LDH)featuring a dandelion-like structure.Anchoring of CeO_(2)onto FeCo LDH produced interfaces between the functionalizing CeO_(2)and the parent LDH.Comparative electrochemical studies were carried out.Onset potential,overpotential,and Tafel slope point to the superior oxygen-evolving performance of CeO_(2)-FeCo LDH with respect to FeCo LDH,therefore,demonstrating the merits of CeO_(2)functionalization.The electronic structures of Fe,Co,and Ce were analyzed by X-ray photoelectron spectroscopy(XPS)and electron energy loss spectroscopy(EELS)from which the increase of Co^(3+)and the concurrent lowering of Ce^(4+)were established.With the use of CeO_(2)-FeCo LDH,accelerated formation at a sizably reduced potential of Co-OOH,one of the key intermediates preceding the release of O_(2)was observed by in situ Raman spectroscopy.We now have the atomic-level and location-specific evidence,the increase of the active Co^(3+)across the interface to correlate the enhanced catalytic performance with CeO_(2)functionalization.展开更多
Natural enzymes as biological catalysts possess remarkable advantages,especially their highly efficient and selective catalysis under mild conditions.However,most natural enzymes are proteins,thus exhibiting an inhere...Natural enzymes as biological catalysts possess remarkable advantages,especially their highly efficient and selective catalysis under mild conditions.However,most natural enzymes are proteins,thus exhibiting an inherent low durability to harsh reaction conditions.Artificial enzyme mimetics have been pursued extensively to avoid this drawback.Quite recently,some inorganic nanoparticles(NPs) have been found to exhibit unique enzyme mimetics.In addition,their much higher stability overcomes the inherent disadvantage of natural enzymes.Furthermore,easy mass-production and low cost endow them more benefits.As a new member of artificial enzyme mimetics,they have received intense attention.In this review article,major progress in this field is summarized and future perspectives are highlighted.展开更多
Bone regeneration is a crucial part in the treatment of periodontal tissue regeneration,in which new attempts come out along with the development of nanomaterials.Herein,the effect of cerium oxide nanoparticles(CeO_(2...Bone regeneration is a crucial part in the treatment of periodontal tissue regeneration,in which new attempts come out along with the development of nanomaterials.Herein,the effect of cerium oxide nanoparticles(CeO_(2)NPs)on the cell behavior and function of human periodontal ligament stem cells(hPDLSCs)was investigated.Results of CCK-8 and cell cycle tests demonstrated that CeO_(2)NPs not only had good biocompatibility,but also promoted cell proliferation.Furthermore,the levels of alkaline phosphatase activity,mineralized nodule formation and expressions of osteogenic genes and proteins demonstrated CeO_(2)NPs could promote osteogenesis differentiation of hPDLSCs.Then we chose electrospinning to fabricate fibrous membranes containing CeO_(2)NPs.We showed that the composite membranes improved mechanical properties as well as realized release of CeO_(2)NPs.We then applied the composite membranes to in vivo study in rat cranial defect models.Micro-CT and histopathological evaluations revealed that nanofibrous membranes with CeO_(2)NPs further accelerated new bone formation.Those exciting results demonstrated that CeO_(2)NPs and porous membrane contributed to osteogenic ability,and CeO_(2)NPs contained electrospun membrane may be a promising candidate material for periodontal bone regeneration.展开更多
基金supported by the National Key R&D Program of China(2021YFB2400400)the National Natural Science Foundation of China(Grant No.22379120,22179085)+5 种基金the Key Research and Development Plan of Shanxi Province(China,Grant No.2018ZDXM-GY-135,2021JLM-36)the National Natural Science Foundation of China(Grant No.22108218)the“Young Talent Support Plan”of Xi’an Jiaotong University(71211201010723)the Qinchuangyuan Innovative Talent Project(QCYRCXM-2022-137)the“Young Talent Support Plan”of Xi’an Jiaotong University(HG6J003)the“1000-Plan program”of Shaanxi Province。
文摘The insurmountable charge transfer impedance at the Li metal/solid polymer electrolytes(SPEs)interface at room temperature as well as the ascending risk of short circuits at the operating temperature higher than the melting point,dominantly limits their applications in solid-state batteries(SSBs).Although the inorganic filler such as CeO_(2)nanoparticle content of composite solid polymer electrolytes(CSPEs)can significantly reduce the enormous charge transfer impedance at the Li metal/SPEs interface,we found that the required content of CeO_(2)nanoparticles in SPEs varies for achieving a decent interfacial charge transfer impedance and the bulk ionic conductivity in CSPEs.In this regard,a sandwich-type composited solid polymer electrolyte with a 10%CeO_(2)CSPEs interlayer sandwiched between two 50%CeO_(2)CSPEs thin layers(sandwiched CSPEs)is constructed to simultaneously achieve low charge transfer impedance and superior ionic conductivity at 30℃.The sandwiched CSPEs allow for stable cycling of Li plating and stripping for 1000 h with 129 mV polarized voltage at 0.1 mA cm^(-2)and 30℃.In addition,the LiFePO_(4)/Sandwiched CSPEs/Li cell also exhibits exceptional cycle performance at 30℃and even elevated120℃without short circuits.Constructing multi-layered CSPEs with optimized contents of the inorganic fillers can be an efficient method for developing all solid-state PEO-based batteries with high performance at a wide range of temperatures.
基金supported by the National Natural Science Foundation of China(grant No.22072018)the Natural Science Foundation of Fujian Province of China(grant No.2021J06010).
文摘Constructing heterojunction interface as an active catalyst is an effective strategy to boost electrocatalytic activity of oxygen evolution reaction(OER).Herein,we report an interfacial CoP/CeO_(2)heterostructure catalyst constructed by interface engineering and selective phosphorization procedure.X-ray photoelectron spectroscopy(XPS)suggests that coupling CeO_(2)nanoparticles on the surface of CoP will generate interfacial interaction at the two-phase interface,resulting in electron transfer between CoP and CeO_(2)components at the interface.Benefitting from the interfacial interaction,large exposed interface area,and luxuriant mesopores structure,CoP/CeO_(2)shows fascinating alkaline OER performance.At the current densities of 10 and 50 mA cm^(−2),the optimal CoP/CeO_(2)heterojunction exhibits lower overpotential(257 and 298 mV)than either CoP(288 and 354 mV)or RuO_(2)(305 and 409 mV).This work provides a facile synthetic protocol for constructing heterostructure interfaces to improve OER performance.
基金supported by the National Key Research and Development Program of China(No.2022YFB3504202)the National Natural Science Foundation of China(No.52204376)Youth Foundation of Hebei Province(No.E2022103007).
文摘With the continuous tightening of automotive emission regulations and the increasing promotion of energy-efficient hybrid vehicles,new challenges have arisen for the low-temperature performance of three-way catalysts(TWCs).To guide the design of next-generation TWCs,it is essential to further develop our understanding of the relationships between microstructure and catalytic performance.Here,Rh/CeO_(2)–ZrO_(2) catalysts were synthesized with different Rh metal dispersion by using a combination of the wet impregnation method and reduction treatment.These catalysts included Rh single-atom catalysts,cluster catalysts,and nanoparticle catalysts.The results showed that the Rh nanoparticle catalyst,with an average size of 1.9 nm,exhibited superior three-way catalytic performance compared to the other catalysts.Based on the catalytic activity in a series of simple reaction atmospheres such as CO+O_(2),NO+CO,and hydrocarbons(HCs)+O_(2) and operando infrared spectroscopy,we found that metallic Rh sites on Rh nanoparticles are the key factor responsible for the low-temperature catalytic performance.
基金supported by the National Natural Science Foundation of China(No.22072015).
文摘Electrocatalytic nitrate reduction reaction(NO_(3)−RR)emerges as a highly efficient approach toward ammonia synthesis and degrading NO_(3)−contaminant.In our study,CeO_(2) nanoparticles with oxygen vacancies(VO)decorated N-doped carbon nanorods on graphite paper(CeO_(2)−x@NC/GP)were demonstrated as a highly efficient NO_(3)−RR electrocatalyst.The CeO_(2)−x@NC/GP catalyst manifests a significant NH_(3 )yield up to 712.75μmol·h^(−1)·cm^(−2) at−0.8 V vs.reversible hydrogen electrode(RHE)and remarkable Faradaic efficiency of 92.93%at−0.5 V vs.RHE under alkaline conditions,with excellent durability.Additionally,an assembled Zn-NO_(3)−battery with CeO_(2)−x@NC/GP as cathode accomplishes a high-power density of 3.44 mW·cm^(−2) and a large NH3 yield of 145.08μmol·h^(−1)·cm^(−2).Density functional theory results further expose the NO_(3)−reduction mechanism on CeO_(2)(111)surface with VO.
文摘In current work,Ni-Ti-CeO_(2) nanocomposite coatings were achieved by co-adding Ti microparticles and CeO_(2) nanoparticles.Designed experiments and COMSOL computer simulation were applied to reveal the synergistic role of Ti microparticles and CeO_(2) nanoparticles in tailoring the spatial microstructures and properties of Ni-Ti-CeO_(2) nanocomposite coating.Unilaterally,the conductive Ti microparticles conducted the growth behavior of Ni grains by current density concentration,distorting electronic feld lines and heterogeneous nucleation.Individual domains consisting of inner nanograins and outer radial columnar grains surrounded Ti microparticles,where Ti microparticles acted as seeds.Ti microparticles tended to be aggregated,leading to spatial heterogeneity of microstructures.Ni deposits buried the Ti microparticles in forms of“covering model”,contributing to the formation of inside voids and rough surface and aggregation of Ti microparticles;on the other hand,the non-conductive CeO_(2)microparticles hardly changed the distribution of current density and electronic feld lines on the cathode surface.Ni deposits buried the CeO_(2)microparticle in forms of“stacking model”,avoiding the inside voids and aggregation of particles.The incorporation of CeO_(2)microparticle brought in microstructure evolutions only on its top side without disturbing the growth behavior of Ni grains on its lateral side or bottom,suggesting the limited effects.This was correlated with the presence of current concentration above the CeO_(2) microparticle at the last stage of burying CeO_(2) microparticle.The co-addition of Ti microparticles and CeO_(2) nanoparticles into Ni deposits exploited the complementary action of the two particles,which gave birth to satisfed spatial microstructures and improved hardness.Ti microparticles took major responsibility for microstructure evolutions,while the CeO_(2) nanoparticles were mainly in charge of the microstructure homogeneity.
基金Project supported by the National Key Research and Development Program of China(2016YFC0204300)the National Natural Science Foundation of China(21477109)。
文摘A series of transition metals(Fe,Co,Ni,Cu,Cr and Mn)-doped CeO_(2)-TiO_(2) catalysts were prepared by the sol-gel method and applied for the catalytic removal of 1,2-dichloroethane(DCE) as a model for chlorinated VOCs(CVOCs).The various characterization methods including X-ray diffraction(XRD),N_(2) adsorption-desorption,UV-Raman,NH_(3) temperature-programmed desorption(NH_(3)-TPD) and H_(2) temperature-programmed reduction(H_(2)-TPR) were utilized to investigate the physicochemical properties of the catalysts.The results show that doping Fe,Co,Ni or Mn can obviously promote the activity of CeO_(2)-TiO_(2) mixed oxides for DCE degradation,which is related to their improved texture properties,acid sites(especially for strong acidity) and low-temperature reducibility.Particularly,CeTi-Fe doped with moderate Fe exhibits excellent activity for 1,2-dichloroethane(DCE) degradation,giving a T_(90%) value as low as 250℃.More importantly,only trace chlorinated byproducts were produced during the low-temperature degradation of various CVOCs(dichloromethane(DCM),trichloroethylene(TCE) and chlorobenzene(CB)) over CeTi-Fe1/9 catalyst with high durability.
基金This work was financially supported by Shenzhen Nobel Prize Scientists Laboratory Project(No.C17213101)Guangdong Provincial Key Laboratory of Catalysis(No.2020B121201002)+6 种基金Guangdong Provincial Key Laboratory of Energy Materials for Electric Power(No.2018B030322001)China Postdoctoral Science Foundation(No.2018M642133,X.Y.Z.)Post-doctorate Scientific Research Fund for staying(coming to)Shenzhen(No.K21217502,X.Y.Z.)the National Natural Science Foundation of China(No.21671096,Z.G.L.)Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials(No.ZDSYS20200421111401738,Z.G.L.)The authors also acknowledge the assistance of Southern University of Science and Technology Core Research Facilities(SUSTech CRF)Key Laboratory of Energy Conversion and Storage Technologies(Southern University of Science and Technology).
文摘Herein,we prepared a bimetallic layered double hydroxide(FeCo LDH)featuring a dandelion-like structure.Anchoring of CeO_(2)onto FeCo LDH produced interfaces between the functionalizing CeO_(2)and the parent LDH.Comparative electrochemical studies were carried out.Onset potential,overpotential,and Tafel slope point to the superior oxygen-evolving performance of CeO_(2)-FeCo LDH with respect to FeCo LDH,therefore,demonstrating the merits of CeO_(2)functionalization.The electronic structures of Fe,Co,and Ce were analyzed by X-ray photoelectron spectroscopy(XPS)and electron energy loss spectroscopy(EELS)from which the increase of Co^(3+)and the concurrent lowering of Ce^(4+)were established.With the use of CeO_(2)-FeCo LDH,accelerated formation at a sizably reduced potential of Co-OOH,one of the key intermediates preceding the release of O_(2)was observed by in situ Raman spectroscopy.We now have the atomic-level and location-specific evidence,the increase of the active Co^(3+)across the interface to correlate the enhanced catalytic performance with CeO_(2)functionalization.
基金supported by the National Natural Science Foundation of China (Grant No. 20773032)the National Basic Research Program of China (Grant No. 2011CB932802)
文摘Natural enzymes as biological catalysts possess remarkable advantages,especially their highly efficient and selective catalysis under mild conditions.However,most natural enzymes are proteins,thus exhibiting an inherent low durability to harsh reaction conditions.Artificial enzyme mimetics have been pursued extensively to avoid this drawback.Quite recently,some inorganic nanoparticles(NPs) have been found to exhibit unique enzyme mimetics.In addition,their much higher stability overcomes the inherent disadvantage of natural enzymes.Furthermore,easy mass-production and low cost endow them more benefits.As a new member of artificial enzyme mimetics,they have received intense attention.In this review article,major progress in this field is summarized and future perspectives are highlighted.
基金This work was supported by the National Natural Science Foundation of China(No.82001049,81771074)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD,2018-87)+1 种基金the Natural Science Foundation of Jiangsu Province(BK.20200665)The authors are grateful to Professor Yong Hu(Nanjing University)for his critical support on electrospinning technology and valuable discussion of the project.
文摘Bone regeneration is a crucial part in the treatment of periodontal tissue regeneration,in which new attempts come out along with the development of nanomaterials.Herein,the effect of cerium oxide nanoparticles(CeO_(2)NPs)on the cell behavior and function of human periodontal ligament stem cells(hPDLSCs)was investigated.Results of CCK-8 and cell cycle tests demonstrated that CeO_(2)NPs not only had good biocompatibility,but also promoted cell proliferation.Furthermore,the levels of alkaline phosphatase activity,mineralized nodule formation and expressions of osteogenic genes and proteins demonstrated CeO_(2)NPs could promote osteogenesis differentiation of hPDLSCs.Then we chose electrospinning to fabricate fibrous membranes containing CeO_(2)NPs.We showed that the composite membranes improved mechanical properties as well as realized release of CeO_(2)NPs.We then applied the composite membranes to in vivo study in rat cranial defect models.Micro-CT and histopathological evaluations revealed that nanofibrous membranes with CeO_(2)NPs further accelerated new bone formation.Those exciting results demonstrated that CeO_(2)NPs and porous membrane contributed to osteogenic ability,and CeO_(2)NPs contained electrospun membrane may be a promising candidate material for periodontal bone regeneration.
