Water electrolysis for energy-efficient H_(2)production coupled with hydrazine oxidation reaction(HzOR)is prevailing,while the sluggish electrocatalysts are strongly hindering its scalable application.Herein,we scheme...Water electrolysis for energy-efficient H_(2)production coupled with hydrazine oxidation reaction(HzOR)is prevailing,while the sluggish electrocatalysts are strongly hindering its scalable application.Herein,we schemed a novel porous Ce-doped Ni3N nanosheet arrays grown on nickel foam(Ce-Ni3N/NF)as a remarkable bifunctional catalyst for both hydrogen evolution reaction and HzOR.Significantly,the overall hydrazine splitting system can achieve low cell voltages of 0.156 and 0.671 V at 10 and 400 mA·cm^(−2),and the system is remarkably stable to operate over 100 h continuous test at the high-current-density of 400 mA·cm^(−2).Various characterizations prove that the porous nanosheet arrays expose more active sites,and more excellent diffusion kinetics and lower charge-transfer resistance,therefore boosting catalytic performance.Furthermore,density functional theory calculation reveals that the incorporation of Ce can effectively optimize the free energy of hydrogen adsorption and promote intrinsic catalytic activity of Ni_(3)N.展开更多
Pristine LiNi_（0.5）Mn_（1.5）O_4 and cerium doped LiCe_xNi_（0.5–x）Mn_（1.5）O_4（x=0.005, 0.01, 0.02） cathode materials were synthesized by solid-state method. The effect of Ce doping content on structure and el...Pristine LiNi_（0.5）Mn_（1.5）O_4 and cerium doped LiCe_xNi_（0.5–x）Mn_（1.5）O_4（x=0.005, 0.01, 0.02） cathode materials were synthesized by solid-state method. The effect of Ce doping content on structure and electrochemical properties of LiNi_（0.5）Mn_（1.5）O_4 cathode material was systematically investigated. The samples were characterized by X-ray diffraction（XRD）, Fourier transformation infrared spectrometer（FT-IR）, scanning electron microscopy（SEM）, electrochemical impedance spectroscopy（EIS）, cyclic voltammetry（CV） and constant-current charge/discharge tests. The results showed that Ce doping did not change the cubic spinel structure with Fd3m space group, but effectively restrained the formation of Li_xNi_（1–x）O impurity phase. Appropriate Ce doping（x=0.005） could decrease the extent of confusion between lithium ions and transition metal ions, increase the lattice parameter and Ni/Mn disordering degree（Mn^（3＋） content）. The synergic effects of the above factors led to the optimal electrochemical performance of LiCe_（0.005）Ni_（0.495）Mn_（1.5）O_4 sample. The discharge capacity at 10 C rate could reach 115.4 mAh/g, 94.82% of that at 0.2C rate, and the capacity retention rate after 100 cycles at 1C rate could reach 94.51%. However, heavier Ce doping had an adverse effect on the electrochemical properties, which might be due to the lower disordering degree and existence of more CeO_2 secondary phase.展开更多
A solid state reaction method was used to synthesize barium titanate （BT） and barium cerium titanate （BCT） ceramics at sintering temperature of 1473 K for 4 h. The effect of cerium （Ce） on the structure, microst...A solid state reaction method was used to synthesize barium titanate （BT） and barium cerium titanate （BCT） ceramics at sintering temperature of 1473 K for 4 h. The effect of cerium （Ce） on the structure, microstructure and dielectric properties of BCT was investigated. The scanning electron microscopy （SEM） investigations revealed that the grain size increases with increasing Ce content. The X-ray diffraction （XI^D） patterns showed mostly the BT phase, where the lattice parameter decreased with the addition of Ce. The temperature dependence of dielectric constant showed decrease in the phase transition temperature with higher Ce content. The dielectric constant decreased slightly with increasing frequency. The direct current （dc） density-voltage characteristics of the ceramics showed ohmic behavior for both the BT and BCT. As the temperature increased, the dc resistivity of the ceramics decreased. The activation energy increased with increasing Ce content.展开更多
Effect of doping cerium in the support on the catalytic activity and side product of the reaction in the oxidative carbonylation of phenol to diphenyl carbonate (DPC) over the catalyst Pd-Co/Cu-Co-Mn mixed oxides was ...Effect of doping cerium in the support on the catalytic activity and side product of the reaction in the oxidative carbonylation of phenol to diphenyl carbonate (DPC) over the catalyst Pd-Co/Cu-Co-Mn mixed oxides was studied. The specific surface areas, crystal phase, valency, and content of the element on the surface of the catalysts were determined, and the products were detected by gas chromatograph/mass spectrometry (GC-MS). It is found that the catalyst without Ce shows higher activity than that with Ce, and the yields of DPC for the two cata-lysts can reach 30% and 23%, respectively. However, doping cerium can prevent the formation of 2-hydroxyphenyl benzoate and p-bromophenyl phenyl carbonate.展开更多
The acid-proof anode Ti/SnO2+Mn2O3/PbO2 doped with Ce was prepared by thermal decomposition and electrodeposition combination technology, the effect of Ce on the morphology and structure of anode was also studied in t...The acid-proof anode Ti/SnO2+Mn2O3/PbO2 doped with Ce was prepared by thermal decomposition and electrodeposition combination technology, the effect of Ce on the morphology and structure of anode was also studied in this paper. The results obtained by cyclic voltammetry (CV), electrochemical impedance spectroscopic (EIS), X-ray Diffraction (XRD) and scanning electron microscopy (SEM) indicated that PbO2 crystal grains presented honeycomb structure were formed on the electrode surface by doping with Ce. The specific surface areas and catalytic active sites of the Ce-PbO2 doped electrode were increased and the catalytic activity was evidently greater than the undoped one. However, when Ce was doped into the intermediate layer (SnO2+Mn2O3), a more cracked surface structure formed, thus leading electrode deactivation by passivation of the Ti-substrate. So the anodic stability was decreased according to the accelerated life tests.展开更多
Cerium-doped titanium dioxide nano-powders were prepared through the sol-gel method and the compound sampies were characterized by X-ray diffraction （XRD）, transmission electron microscopy （TEM）, and UV/Vis diffus...Cerium-doped titanium dioxide nano-powders were prepared through the sol-gel method and the compound sampies were characterized by X-ray diffraction （XRD）, transmission electron microscopy （TEM）, and UV/Vis diffuse reflectance spectra （DRS）. The photocatalytic activity was evaluated by photocatalytic degradation of phenol in water. The results of XRD, TEM, and DRS show that pure TiO2 and Ce-doped TiO2 powder crystallines are a mixture of anatase and rutile ; the doping can retard the development of the grain size of TiO2 and decrease the diameter of TiO2 from more than 20 nm of pure TiO2 to about 10 nm; the doped TiO2 can improve the light absorption of TiO2 and suitable doping content tends to move the DRS spectrum of TiO2 towards visible light, but too much doping is not good for the light absorption ability. The results of the photocatalytic experiments show that doping with Ce content of 0.08% -0.4% can increase the photocatalytic activity of TiO2; however, doping with Ce content of 0.5% -2.5% can significantly decrease the photocatalytic activity of TiO2. The favorite doping content is 0.4% in the range of our experiments.展开更多
Metal-organic framework（MOF） material MIL-53（A1） with high thermal stability was prepared by a solvothermal method,serving as a support material of cerium doped copper catalyst（Ce-Cu）/MIL-53（A1） material for C...Metal-organic framework（MOF） material MIL-53（A1） with high thermal stability was prepared by a solvothermal method,serving as a support material of cerium doped copper catalyst（Ce-Cu）/MIL-53（A1） material for CO oxidation with high catalytic activity.The catalytic performance between the（CuCe）/MIL-53（A1） and the Cu/MIL-53（A1） catalytic material was compared to understand the catalytic behavior of the catalysts.The catalysts were characterized by thermogravimetric-differential scanning calorimetry（TGDSC）,N2 adsorption- desorption,X-ray diffraction（XRD）,and transmission electron microscopy（TEM）.The characterization results showed that MIL-53（A1） had good stability and high surface areas,the（Ce-Cu）nanoparticles on the MIL-53（A1） support was uniform.Therefore,the heterogeneous catalytic composite materials（Ce-Cu）/MIL-53（A1） catalyst exhibited much higher activity than that of the Cu/MIL- 53（A1） catalyst in CO oxidation test,with 100%conversion at 80 ℃.The results reveal that（Cu-Ce）/MIL-53（A1） is the suitable candidate for achieving low temperature and higher activity CO oxidation catalyst of MOFs.展开更多
A new magnetic mesoporous As(Ⅲ)adsorbent of Fe_(3)O_(4)@SiO_(2)@Ce-ZrO_(2)was prepared by solvothermal and sol^(-)gel method.The core-shell adsorbent presented a high specific surface area(168.2 m^(2)/g)and fast magn...A new magnetic mesoporous As(Ⅲ)adsorbent of Fe_(3)O_(4)@SiO_(2)@Ce-ZrO_(2)was prepared by solvothermal and sol^(-)gel method.The core-shell adsorbent presented a high specific surface area(168.2 m^(2)/g)and fast magnetic separation performance(5.37 A·m^(2)/kg).Compared with Fe_(3)O_(4)@SiO_(2)@ZrO_(2),the Ce-doped sample exhibited 12%-23%increase in As(Ⅲ)uptake over p H 3-11,which was mainly attributed to the formation of bimetal M—O—As complexes.The coexisted SO^_(4)(2-)and PO^_(4)(3-)weakened As(Ⅲ)adsorption,Ca^(2+)worked oppositely,but the impact of Cl^(-)and NO_(3)^(-)was negligible.The As(Ⅲ)maximum adsorption capacity was 24.52 mg/g at 313 K with an initial As(Ⅲ)concentration of 5 mg/L at pH 7,and its kinetics was well fitted by the pseudo-second-order model.Moreover,the adsorbent exhibited remarkable recyclability.It is suggested that Fe_(3)O_(4)@SiO_(2)@Ce-ZrO_(2)is a promising adsorbent for the advanced treatment of As(Ⅲ)contaminated wastewater.展开更多
Al2O3 powders with different morphologies,namely fibrous,sheet-like,and spherical,were prepared by the hydrothermal-thermolysis method.Subsequently,polycrystalline,transparent cerium doped lutetium aluminum garnet（Lu...Al2O3 powders with different morphologies,namely fibrous,sheet-like,and spherical,were prepared by the hydrothermal-thermolysis method.Subsequently,polycrystalline,transparent cerium doped lutetium aluminum garnet（Lu3Al5O（12）：Ce^3＋）green phosphors were synthesized by high temperature solidstate method using commercial lutetium（III）oxide,cerium（III）oxide,and as-prepared Al2O3 powders with different morphologies.The phases,morphologies,and photoluminescent properties of the prepared phosphors were investigated by X-ray diffraction（XRD）,scanning electron microscopy（SEM）,and photoluminescence spectroscopy（PL）.Moreover,the influences of the morphologies ofα-Al2O3 on the types of crystal structure,morphologies,and photoluminescent properties of LuAG：Ce^3＋green phosphors were investigated.The results indicated that the morphologies and particle sizes of theα-Al2O3 powders could be controlled by the additives and parameters.Notably,the sphericalα-Al2O3 powders with good dispersibility were found to be the excellent base materials of LuAG：Ce^3＋green phosphors for white light emitting diodes.展开更多
Lithium(Li)metal is regarded as the holy grail anode material for high-energy-density batteries owing to its ultrahigh theoretical specific capacity.However,its practical application is severely hindered by the high r...Lithium(Li)metal is regarded as the holy grail anode material for high-energy-density batteries owing to its ultrahigh theoretical specific capacity.However,its practical application is severely hindered by the high reactivity of metallic Li against the commonly used electrolytes and uncontrolled growth of mossy/dendritic Li.Different from widely-used approaches of optimization of the electrolyte and/or interfacial engineering,here,we report a strategy of in-situ cerium(Ce)doping of Li metal to promote the preferential plating along the[200]direction and remarkably decreased surface energy of metallic Li.The in-situ Ce-doped Li shows a significantly reduced reactivity towards a standard electrolyte and,uniform and dendrite-free morphology after plating/stripping,as demonstrated by spectroscopic,morphological and electrochemical characterizations.In symmetric half cells,the in-situ Ce-doped Li shows a low corrosion current density against the electrolyte and drastically improved cycling even at a lean electrolyte condition.Furthermore,we show that the stable Li|LiCoO2 full cells with improved coulombic efficiency and cycle life are also achieved using the Ce-doped Li metal anode.This work provides an inspiring approach to bring Li metal towards practical application in high energy-density batteries.展开更多
In this paper,factors influencing themineralization of dimethyl phthalate(DMP)during catalytic ozonation with a cerium-doped Ru/Al_(2)O_(3) catalyst were studied.The catalytic contribution was calculated through the r...In this paper,factors influencing themineralization of dimethyl phthalate(DMP)during catalytic ozonation with a cerium-doped Ru/Al_(2)O_(3) catalyst were studied.The catalytic contribution was calculated through the results of a comparison experiment.It showed that doping cerium significantly enhanced catalytic activity.The total organic carbon(TOC)removal over the doped catalyst at 100 min reached 75.1%,61.3% using Ru/Al_(2)O_(3) catalyst and only 14.0% using ozone alone.Catalytic activity reached the maximum when 0.2% of ruthenium and 1.0% of cerium were simultaneously loaded onto Al_(2)O_(3) support.Results of experiments on oxidation by ozone alone,adsorption of the catalyst,Ce ion’s and heterogeneous catalytic ozonation confirmed that the contribution of heterogeneous catalytic ozonation was about 50%,which showed the obvious effect of Ru-Ce/Al_(2)O_(3) on catalytic activity.展开更多
Understanding how defect chemistry of oxide material influences the thermal stability of noble metal dopant ions plays an important role in designing high-performance heterogeneous catalytic systems.Here we use in-sit...Understanding how defect chemistry of oxide material influences the thermal stability of noble metal dopant ions plays an important role in designing high-performance heterogeneous catalytic systems.Here we use in-situ ambient-pressure X-ray photoemission spectroscopy(APXPS)to experimentally determine the role of grain boundary in the thermal stability of platinum doped cerium oxide(Pt/CeO_(2)).The grain boundaries were introduced in Pt/CeO_(2)thin films by pulsed laser deposition without significantly change of the surface microstructure.The defect level was tuned by the strain field obtained using a highly/low mismatched substrate.The Pt/CeO_(2)thin film models having well defined crystallographic properties but different grain boundary structural defect levels provide an ideal platform for exploring the evolution of Pt–O–Ce bond with changing the temperature in reducing conditions.We have direct demonstration and explanation of the role of Ce^(3+)induced by grain boundaries in enhancing Pt2+stability.We observe that the Pt^(2+)–O–Ce^(3+)bond provides an ideal coordinated site for anchoring of Pt^(2+)ions and limits the further formation of oxygen vacancies during the reduction with H_(2).Our findings demonstrate the importance of grain boundary in the atomic-scale design of thermally stable catalytic active sites.展开更多
基金supported by Nantong University Analysis&Testing Center。
文摘Water electrolysis for energy-efficient H_(2)production coupled with hydrazine oxidation reaction(HzOR)is prevailing,while the sluggish electrocatalysts are strongly hindering its scalable application.Herein,we schemed a novel porous Ce-doped Ni3N nanosheet arrays grown on nickel foam(Ce-Ni3N/NF)as a remarkable bifunctional catalyst for both hydrogen evolution reaction and HzOR.Significantly,the overall hydrazine splitting system can achieve low cell voltages of 0.156 and 0.671 V at 10 and 400 mA·cm^(−2),and the system is remarkably stable to operate over 100 h continuous test at the high-current-density of 400 mA·cm^(−2).Various characterizations prove that the porous nanosheet arrays expose more active sites,and more excellent diffusion kinetics and lower charge-transfer resistance,therefore boosting catalytic performance.Furthermore,density functional theory calculation reveals that the incorporation of Ce can effectively optimize the free energy of hydrogen adsorption and promote intrinsic catalytic activity of Ni_(3)N.
基金supported by the Natural Science Foundation of Hebei Province(E2015202356)Key R&D Plan Self-raised Project of Hebei Province(16214406)Technology Innovation Foundation Project for Outstanding Youth of Hebei University of Technology(2013009)
文摘Pristine LiNi_（0.5）Mn_（1.5）O_4 and cerium doped LiCe_xNi_（0.5–x）Mn_（1.5）O_4（x=0.005, 0.01, 0.02） cathode materials were synthesized by solid-state method. The effect of Ce doping content on structure and electrochemical properties of LiNi_（0.5）Mn_（1.5）O_4 cathode material was systematically investigated. The samples were characterized by X-ray diffraction（XRD）, Fourier transformation infrared spectrometer（FT-IR）, scanning electron microscopy（SEM）, electrochemical impedance spectroscopy（EIS）, cyclic voltammetry（CV） and constant-current charge/discharge tests. The results showed that Ce doping did not change the cubic spinel structure with Fd3m space group, but effectively restrained the formation of Li_xNi_（1–x）O impurity phase. Appropriate Ce doping（x=0.005） could decrease the extent of confusion between lithium ions and transition metal ions, increase the lattice parameter and Ni/Mn disordering degree（Mn^（3＋） content）. The synergic effects of the above factors led to the optimal electrochemical performance of LiCe_（0.005）Ni_（0.495）Mn_（1.5）O_4 sample. The discharge capacity at 10 C rate could reach 115.4 mAh/g, 94.82% of that at 0.2C rate, and the capacity retention rate after 100 cycles at 1C rate could reach 94.51%. However, heavier Ce doping had an adverse effect on the electrochemical properties, which might be due to the lower disordering degree and existence of more CeO_2 secondary phase.
文摘A solid state reaction method was used to synthesize barium titanate （BT） and barium cerium titanate （BCT） ceramics at sintering temperature of 1473 K for 4 h. The effect of cerium （Ce） on the structure, microstructure and dielectric properties of BCT was investigated. The scanning electron microscopy （SEM） investigations revealed that the grain size increases with increasing Ce content. The X-ray diffraction （XI^D） patterns showed mostly the BT phase, where the lattice parameter decreased with the addition of Ce. The temperature dependence of dielectric constant showed decrease in the phase transition temperature with higher Ce content. The dielectric constant decreased slightly with increasing frequency. The direct current （dc） density-voltage characteristics of the ceramics showed ohmic behavior for both the BT and BCT. As the temperature increased, the dc resistivity of the ceramics decreased. The activation energy increased with increasing Ce content.
文摘Effect of doping cerium in the support on the catalytic activity and side product of the reaction in the oxidative carbonylation of phenol to diphenyl carbonate (DPC) over the catalyst Pd-Co/Cu-Co-Mn mixed oxides was studied. The specific surface areas, crystal phase, valency, and content of the element on the surface of the catalysts were determined, and the products were detected by gas chromatograph/mass spectrometry (GC-MS). It is found that the catalyst without Ce shows higher activity than that with Ce, and the yields of DPC for the two cata-lysts can reach 30% and 23%, respectively. However, doping cerium can prevent the formation of 2-hydroxyphenyl benzoate and p-bromophenyl phenyl carbonate.
基金the National Natural Science Foundation of China (20476070,20771080)Natural Science Foundation of Shanxi Province (20031024 ,20041020)
文摘The acid-proof anode Ti/SnO2+Mn2O3/PbO2 doped with Ce was prepared by thermal decomposition and electrodeposition combination technology, the effect of Ce on the morphology and structure of anode was also studied in this paper. The results obtained by cyclic voltammetry (CV), electrochemical impedance spectroscopic (EIS), X-ray Diffraction (XRD) and scanning electron microscopy (SEM) indicated that PbO2 crystal grains presented honeycomb structure were formed on the electrode surface by doping with Ce. The specific surface areas and catalytic active sites of the Ce-PbO2 doped electrode were increased and the catalytic activity was evidently greater than the undoped one. However, when Ce was doped into the intermediate layer (SnO2+Mn2O3), a more cracked surface structure formed, thus leading electrode deactivation by passivation of the Ti-substrate. So the anodic stability was decreased according to the accelerated life tests.
文摘Cerium-doped titanium dioxide nano-powders were prepared through the sol-gel method and the compound sampies were characterized by X-ray diffraction （XRD）, transmission electron microscopy （TEM）, and UV/Vis diffuse reflectance spectra （DRS）. The photocatalytic activity was evaluated by photocatalytic degradation of phenol in water. The results of XRD, TEM, and DRS show that pure TiO2 and Ce-doped TiO2 powder crystallines are a mixture of anatase and rutile ; the doping can retard the development of the grain size of TiO2 and decrease the diameter of TiO2 from more than 20 nm of pure TiO2 to about 10 nm; the doped TiO2 can improve the light absorption of TiO2 and suitable doping content tends to move the DRS spectrum of TiO2 towards visible light, but too much doping is not good for the light absorption ability. The results of the photocatalytic experiments show that doping with Ce content of 0.08% -0.4% can increase the photocatalytic activity of TiO2; however, doping with Ce content of 0.5% -2.5% can significantly decrease the photocatalytic activity of TiO2. The favorite doping content is 0.4% in the range of our experiments.
基金Funded by the Guiding Research Project of Hubei Province Department of Education(No.B2016098)
文摘Metal-organic framework（MOF） material MIL-53（A1） with high thermal stability was prepared by a solvothermal method,serving as a support material of cerium doped copper catalyst（Ce-Cu）/MIL-53（A1） material for CO oxidation with high catalytic activity.The catalytic performance between the（CuCe）/MIL-53（A1） and the Cu/MIL-53（A1） catalytic material was compared to understand the catalytic behavior of the catalysts.The catalysts were characterized by thermogravimetric-differential scanning calorimetry（TGDSC）,N2 adsorption- desorption,X-ray diffraction（XRD）,and transmission electron microscopy（TEM）.The characterization results showed that MIL-53（A1） had good stability and high surface areas,the（Ce-Cu）nanoparticles on the MIL-53（A1） support was uniform.Therefore,the heterogeneous catalytic composite materials（Ce-Cu）/MIL-53（A1） catalyst exhibited much higher activity than that of the Cu/MIL- 53（A1） catalyst in CO oxidation test,with 100%conversion at 80 ℃.The results reveal that（Cu-Ce）/MIL-53（A1） is the suitable candidate for achieving low temperature and higher activity CO oxidation catalyst of MOFs.
基金the financial support from the Open Research Fund of Jiangsu Key Laboratory of Resources and Environmental Information Engineering,China(No.JS201810)。
文摘A new magnetic mesoporous As(Ⅲ)adsorbent of Fe_(3)O_(4)@SiO_(2)@Ce-ZrO_(2)was prepared by solvothermal and sol^(-)gel method.The core-shell adsorbent presented a high specific surface area(168.2 m^(2)/g)and fast magnetic separation performance(5.37 A·m^(2)/kg).Compared with Fe_(3)O_(4)@SiO_(2)@ZrO_(2),the Ce-doped sample exhibited 12%-23%increase in As(Ⅲ)uptake over p H 3-11,which was mainly attributed to the formation of bimetal M—O—As complexes.The coexisted SO^_(4)(2-)and PO^_(4)(3-)weakened As(Ⅲ)adsorption,Ca^(2+)worked oppositely,but the impact of Cl^(-)and NO_(3)^(-)was negligible.The As(Ⅲ)maximum adsorption capacity was 24.52 mg/g at 313 K with an initial As(Ⅲ)concentration of 5 mg/L at pH 7,and its kinetics was well fitted by the pseudo-second-order model.Moreover,the adsorbent exhibited remarkable recyclability.It is suggested that Fe_(3)O_(4)@SiO_(2)@Ce-ZrO_(2)is a promising adsorbent for the advanced treatment of As(Ⅲ)contaminated wastewater.
基金Funded by Shan’xi Educational Committee(No.17JK0395)
文摘Al2O3 powders with different morphologies,namely fibrous,sheet-like,and spherical,were prepared by the hydrothermal-thermolysis method.Subsequently,polycrystalline,transparent cerium doped lutetium aluminum garnet（Lu3Al5O（12）：Ce^3＋）green phosphors were synthesized by high temperature solidstate method using commercial lutetium（III）oxide,cerium（III）oxide,and as-prepared Al2O3 powders with different morphologies.The phases,morphologies,and photoluminescent properties of the prepared phosphors were investigated by X-ray diffraction（XRD）,scanning electron microscopy（SEM）,and photoluminescence spectroscopy（PL）.Moreover,the influences of the morphologies ofα-Al2O3 on the types of crystal structure,morphologies,and photoluminescent properties of LuAG：Ce^3＋green phosphors were investigated.The results indicated that the morphologies and particle sizes of theα-Al2O3 powders could be controlled by the additives and parameters.Notably,the sphericalα-Al2O3 powders with good dispersibility were found to be the excellent base materials of LuAG：Ce^3＋green phosphors for white light emitting diodes.
基金This work was supported by the National Natural Science Foundation of China(51602250,51802256 and 21875181)the Innovation Capability Support Program of Shaanxi(2018PT-28 and 2019PT-05).
文摘Lithium(Li)metal is regarded as the holy grail anode material for high-energy-density batteries owing to its ultrahigh theoretical specific capacity.However,its practical application is severely hindered by the high reactivity of metallic Li against the commonly used electrolytes and uncontrolled growth of mossy/dendritic Li.Different from widely-used approaches of optimization of the electrolyte and/or interfacial engineering,here,we report a strategy of in-situ cerium(Ce)doping of Li metal to promote the preferential plating along the[200]direction and remarkably decreased surface energy of metallic Li.The in-situ Ce-doped Li shows a significantly reduced reactivity towards a standard electrolyte and,uniform and dendrite-free morphology after plating/stripping,as demonstrated by spectroscopic,morphological and electrochemical characterizations.In symmetric half cells,the in-situ Ce-doped Li shows a low corrosion current density against the electrolyte and drastically improved cycling even at a lean electrolyte condition.Furthermore,we show that the stable Li|LiCoO2 full cells with improved coulombic efficiency and cycle life are also achieved using the Ce-doped Li metal anode.This work provides an inspiring approach to bring Li metal towards practical application in high energy-density batteries.
基金This work was supported by the National Natural Science Foundation of China(Grant No.50238020).
文摘In this paper,factors influencing themineralization of dimethyl phthalate(DMP)during catalytic ozonation with a cerium-doped Ru/Al_(2)O_(3) catalyst were studied.The catalytic contribution was calculated through the results of a comparison experiment.It showed that doping cerium significantly enhanced catalytic activity.The total organic carbon(TOC)removal over the doped catalyst at 100 min reached 75.1%,61.3% using Ru/Al_(2)O_(3) catalyst and only 14.0% using ozone alone.Catalytic activity reached the maximum when 0.2% of ruthenium and 1.0% of cerium were simultaneously loaded onto Al_(2)O_(3) support.Results of experiments on oxidation by ozone alone,adsorption of the catalyst,Ce ion’s and heterogeneous catalytic ozonation confirmed that the contribution of heterogeneous catalytic ozonation was about 50%,which showed the obvious effect of Ru-Ce/Al_(2)O_(3) on catalytic activity.
基金The APXPS experiments were performed at BL02B01 of SSRF with the approval of the Proposal Assessing Committee of SiP.ME2 platform project(Proposal No.2019-SSRF-PT-011613)the Natural Science Foundation of China(No.11227902)the Shanghai Key Research Program(No.20ZR1436700).
文摘Understanding how defect chemistry of oxide material influences the thermal stability of noble metal dopant ions plays an important role in designing high-performance heterogeneous catalytic systems.Here we use in-situ ambient-pressure X-ray photoemission spectroscopy(APXPS)to experimentally determine the role of grain boundary in the thermal stability of platinum doped cerium oxide(Pt/CeO_(2)).The grain boundaries were introduced in Pt/CeO_(2)thin films by pulsed laser deposition without significantly change of the surface microstructure.The defect level was tuned by the strain field obtained using a highly/low mismatched substrate.The Pt/CeO_(2)thin film models having well defined crystallographic properties but different grain boundary structural defect levels provide an ideal platform for exploring the evolution of Pt–O–Ce bond with changing the temperature in reducing conditions.We have direct demonstration and explanation of the role of Ce^(3+)induced by grain boundaries in enhancing Pt2+stability.We observe that the Pt^(2+)–O–Ce^(3+)bond provides an ideal coordinated site for anchoring of Pt^(2+)ions and limits the further formation of oxygen vacancies during the reduction with H_(2).Our findings demonstrate the importance of grain boundary in the atomic-scale design of thermally stable catalytic active sites.
