The branching ratios of ions and the angular distributions of electrons ejected from the Eu 4f^76p_（1/2）nd auto-ionizing states are investigated with the velocity-map-imaging technique.To populate the above auto-ion...The branching ratios of ions and the angular distributions of electrons ejected from the Eu 4f^76p_（1/2）nd auto-ionizing states are investigated with the velocity-map-imaging technique.To populate the above auto-ionizing states,the relevant bound Rydberg states have to be detected first.Two new bound Rydberg states are identified in the region between41150 cm^（-1）and 44580 cm^（-1）,from which auto-ionization spectra of the Eu 4f^76p_（1/2）nd states are observed with isolated core excitation method.With all preparations above,the branching ratios from the above auto-ionizing states to different final ionic states and the angular distributions of electrons ejected from these processes are measured systematically.Energy dependence of branching ratios and anisotropy parameters within the auto-ionization spectra are carefully analyzed,followed by a qualitative interpretation.展开更多
Optical properties of Pr^3＋ doped in Y2SiO5, including absorption spectra, emission spectra, and fluorescence decay, have been investigated with a special attention in the UV region. Broad band （270-350nm） UV fluor...Optical properties of Pr^3＋ doped in Y2SiO5, including absorption spectra, emission spectra, and fluorescence decay, have been investigated with a special attention in the UV region. Broad band （270-350nm） UV fluorescence assigned to the transitions 4f5d → 4f^2 ^3Hj, ^3Fj is found. The spontaneous transition probabilities in the 4f^2 intraconfiguration are calculated by utilizing the 3udd-Ofelt theory, by which three phenomenological parameters （Ω2, Ω4, Ω6,） are obtained by fitting the absorption spectra. For the evaluation of transition probability of the interconfiguration 4f5d → 4f^2, a formula for electric dipole transition is employed. In comparison of the measured fluorescence lifetime with the calculated spontaneous radiative lifetime, the fluorescence quantum efficiency is deduced.展开更多
The vacuum ultraviolet (VUV) spectroscopic properties of praseodymium (Pr3+, 1at%) doped LaF3 nanocrystals/glass at room temperature and 20 K are reported. Two types of Pr3+ ions, those in LaF3 nanocrystals and those ...The vacuum ultraviolet (VUV) spectroscopic properties of praseodymium (Pr3+, 1at%) doped LaF3 nanocrystals/glass at room temperature and 20 K are reported. Two types of Pr3+ ions, those in LaF3 nanocrystals and those in the glass host, were excited to 4f 5d band by VUV using synchrotron radiation as an excitation source, and emissions of 1S0 → 1D2 (336 nm), 1S0 → 1I6 (397 nm ) of Pr3+ in the nanocrystals and emissions of 4f 5d → 3HJ, 3FJ of Pr3+ in the glass appeared at the same time. But unlike in the bulk sample crystals, emission of 3P0 → 3HJ, 3FJ as the second step of the quantum splitting (QS) of Pr3+ in the LaF3 nanocrystals was not observed at room temperature, which could be explained that Pr3+ ions in the glass absorbed the energy of 3P0 → 3H4 of Pr3+ in the nanocrystals. Two types of excitation spectra monitoring different emissions were also measured, so it could be observed that the lowest energy of 4f 5d band of Pr3+ in the nanocrystals was about 53 500 cm-1 (186 nm) and in the glass about 33 800 cm-1(295 nm), respectively. These emission and excitation spectra were contrasted to those of bulk sample crystals LaF3∶Pr3+.展开更多
Flexible Na-ion storage cathodes are still very few due to the challenge in achieving both reliable mechanical flexibility and excellent electrochemical performances.Herein,a new type of flexible Na_(3)(VOPO_(4))_(2)F...Flexible Na-ion storage cathodes are still very few due to the challenge in achieving both reliable mechanical flexibility and excellent electrochemical performances.Herein,a new type of flexible Na_(3)(VOPO_(4))_(2)F cathode with nanocubes tightly assembled on carbon cloth is fabricated by a facile solvothe rmal method for the first time.The cathode is able to exhibit superior rate capability and stable cycling performa nce up to 1000 cycles,due to the surface-assembling of crystalline nanocubes on carbon fibers.In addition,it shows good mechanical flexibility,nearly no capacity decay is observed after continuous bending of 500 times.With this novel cathode and a directly-grown Na_(2)Ti_(2)O_(5) anode,a fully binde r-free Na-ion battery is assembled.It can deliver a high wo rking voltage and increased gravimetric energy/power densities(maximum values:220.2 Wh/kg;5674,7 W/kg),and can power a LED indicator at bending angles fro m 0° to 180°.展开更多
Na_(3)(VO)_(2)(PO_(4))_(2)F(NVPOF)has been considered as one potential candidate for sodium-ion batteries because of its high operating voltage and theoretical capacity.However,the poor intrinsic electronic conductivi...Na_(3)(VO)_(2)(PO_(4))_(2)F(NVPOF)has been considered as one potential candidate for sodium-ion batteries because of its high operating voltage and theoretical capacity.However,the poor intrinsic electronic conductivity significantly restricts its widespread application.In response to this drawback,we adopt the optimization strategy of tuning the morphology and structure to boost the electrical conductivity and mitigate the capacity fading.In this paper,NVPOF microspheres with unique porous yolk-shell structure were fabricated via a facile one-step solvothermal method for the first time.By monitoring the morphological evolution with time-dependent experiments,the self-sacrifice and Ostwald ripening mechanism from rough spheres to yolk-shell structure was revealed.Benefited from the favorable interwoven nanosheets shell,inner cavity and porous core structure,the resulting NVPOF electrode exhibits superior rate capability of 63 m A h g^(-1)at 20 C as well as outstanding long-cycling performance with the capacity retention up to 92.1%over 1000 cycles at 5 C.展开更多
柔性钠离子电池(SIBs)在便携式和可穿戴设备中具有巨大的应用潜力,因为它们在特定情况下具有适用性和价格优势.在正极材料中,磷酸盐电极材料具有结构稳定性好、工作电位高和寿命长的优点.然而,由于对制造要求苛刻,反应复杂,以及柔性基...柔性钠离子电池(SIBs)在便携式和可穿戴设备中具有巨大的应用潜力,因为它们在特定情况下具有适用性和价格优势.在正极材料中,磷酸盐电极材料具有结构稳定性好、工作电位高和寿命长的优点.然而,由于对制造要求苛刻,反应复杂,以及柔性基材的缺失等问题,柔性磷酸盐电极材料的设计仍然是一个巨大的挑战.在此,我们报道了在柔性多孔碳纳米纤维上垂直生长的VO_(2)纳米片原位转化为三维氟磷酸钒钠纳米棒阵列(PCNF@NVOPF NR).PCNF@NVOPF NR实现了兼具柔性与高压正极电极的特点,并具有长期循环稳定性(4500次循环后容量保持率为87.6%).阵列结构可以确保快速的钠反应动力学和低界面电阻.此外,PCNF@NVOPF NR//PCNF@VO_(2)NS@C钠离子全电池表现出高能量和功率密度(220.5 W h kg^(-1)和9400 W kg^(-1)).这种用于柔性正极的材料设计策略可促进实用钠离子电池的商业化.展开更多
Flexible power sources featuring high-performance,prominent flexibility and raised safety have received mounting attention in the area of wearable electronic devices.However,many great challenges remain to be overcome...Flexible power sources featuring high-performance,prominent flexibility and raised safety have received mounting attention in the area of wearable electronic devices.However,many great challenges remain to be overcome,notably the design and fabrication of flexible electrodes with excellent electrochemical performance and matching them with safe and reliable electrolytes.Herein,a facile approach for preparing flexible electrodes,which employs carbon cloth derived from commercial cotton cloth as the substrate of cathode and a flexible anode,is proposed and investigated.The promising cathode(NVPOF@FCC)with high conductivity and outstanding flexibility is prepared by efficiently coating Na_(3)V_(2)(PO_(4))_(2)O_(2)F(NVPOF)on flexible carbon cloth(FCC),which exhibits remarkable electrochemical performance and the significantly improved reaction kinetics.More importantly,a novel flexible quasi-solid-state sodium-ion full battery(QSFB)is feasibly assembled by sandwiching a P(VDF-HFP)-NaClO_(4) gel-polymer electrolyte film between the advanced NVPOF@FCC cathode and FCC anode.And the QSFBs are further evaluated in flexible pouch cells,which not only demonstrates excellent energy-storage performance in aspect of great cycling stability and high-rate capability,but also impressive flexibility and safety.This work offers a feasible and effective strategy for the design of flexible electrodes,paving the way for the progression of practical and sustainable flexible batteries.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant No.11174218)
文摘The branching ratios of ions and the angular distributions of electrons ejected from the Eu 4f^76p_（1/2）nd auto-ionizing states are investigated with the velocity-map-imaging technique.To populate the above auto-ionizing states,the relevant bound Rydberg states have to be detected first.Two new bound Rydberg states are identified in the region between41150 cm^（-1）and 44580 cm^（-1）,from which auto-ionization spectra of the Eu 4f^76p_（1/2）nd states are observed with isolated core excitation method.With all preparations above,the branching ratios from the above auto-ionizing states to different final ionic states and the angular distributions of electrons ejected from these processes are measured systematically.Energy dependence of branching ratios and anisotropy parameters within the auto-ionization spectra are carefully analyzed,followed by a qualitative interpretation.
基金Supported by the National Natural Science Foundation of China under Grant No 10074020.
文摘Optical properties of Pr^3＋ doped in Y2SiO5, including absorption spectra, emission spectra, and fluorescence decay, have been investigated with a special attention in the UV region. Broad band （270-350nm） UV fluorescence assigned to the transitions 4f5d → 4f^2 ^3Hj, ^3Fj is found. The spontaneous transition probabilities in the 4f^2 intraconfiguration are calculated by utilizing the 3udd-Ofelt theory, by which three phenomenological parameters （Ω2, Ω4, Ω6,） are obtained by fitting the absorption spectra. For the evaluation of transition probability of the interconfiguration 4f5d → 4f^2, a formula for electric dipole transition is employed. In comparison of the measured fluorescence lifetime with the calculated spontaneous radiative lifetime, the fluorescence quantum efficiency is deduced.
文摘The vacuum ultraviolet (VUV) spectroscopic properties of praseodymium (Pr3+, 1at%) doped LaF3 nanocrystals/glass at room temperature and 20 K are reported. Two types of Pr3+ ions, those in LaF3 nanocrystals and those in the glass host, were excited to 4f 5d band by VUV using synchrotron radiation as an excitation source, and emissions of 1S0 → 1D2 (336 nm), 1S0 → 1I6 (397 nm ) of Pr3+ in the nanocrystals and emissions of 4f 5d → 3HJ, 3FJ of Pr3+ in the glass appeared at the same time. But unlike in the bulk sample crystals, emission of 3P0 → 3HJ, 3FJ as the second step of the quantum splitting (QS) of Pr3+ in the LaF3 nanocrystals was not observed at room temperature, which could be explained that Pr3+ ions in the glass absorbed the energy of 3P0 → 3H4 of Pr3+ in the nanocrystals. Two types of excitation spectra monitoring different emissions were also measured, so it could be observed that the lowest energy of 4f 5d band of Pr3+ in the nanocrystals was about 53 500 cm-1 (186 nm) and in the glass about 33 800 cm-1(295 nm), respectively. These emission and excitation spectra were contrasted to those of bulk sample crystals LaF3∶Pr3+.
基金supported by the National Natural Science Foundation of China (Nos.51972257,51672205 and 21673169)the National Key R&D Program of China (No.2016YFA0202602)。
文摘Flexible Na-ion storage cathodes are still very few due to the challenge in achieving both reliable mechanical flexibility and excellent electrochemical performances.Herein,a new type of flexible Na_(3)(VOPO_(4))_(2)F cathode with nanocubes tightly assembled on carbon cloth is fabricated by a facile solvothe rmal method for the first time.The cathode is able to exhibit superior rate capability and stable cycling performa nce up to 1000 cycles,due to the surface-assembling of crystalline nanocubes on carbon fibers.In addition,it shows good mechanical flexibility,nearly no capacity decay is observed after continuous bending of 500 times.With this novel cathode and a directly-grown Na_(2)Ti_(2)O_(5) anode,a fully binde r-free Na-ion battery is assembled.It can deliver a high wo rking voltage and increased gravimetric energy/power densities(maximum values:220.2 Wh/kg;5674,7 W/kg),and can power a LED indicator at bending angles fro m 0° to 180°.
基金financially supported by the National Natural Science Foundation of China(No.51972259)the Hubei Provincial Natural Science Foundation of China(No.2019CFB519)+1 种基金the Fundamental Research Funds for the Central Universities(No.WUT:2020Ⅲ015GX)the National innovation and entrepreneurship training program for Undergraduate(No.201910497011)。
文摘Na_(3)(VO)_(2)(PO_(4))_(2)F(NVPOF)has been considered as one potential candidate for sodium-ion batteries because of its high operating voltage and theoretical capacity.However,the poor intrinsic electronic conductivity significantly restricts its widespread application.In response to this drawback,we adopt the optimization strategy of tuning the morphology and structure to boost the electrical conductivity and mitigate the capacity fading.In this paper,NVPOF microspheres with unique porous yolk-shell structure were fabricated via a facile one-step solvothermal method for the first time.By monitoring the morphological evolution with time-dependent experiments,the self-sacrifice and Ostwald ripening mechanism from rough spheres to yolk-shell structure was revealed.Benefited from the favorable interwoven nanosheets shell,inner cavity and porous core structure,the resulting NVPOF electrode exhibits superior rate capability of 63 m A h g^(-1)at 20 C as well as outstanding long-cycling performance with the capacity retention up to 92.1%over 1000 cycles at 5 C.
基金supported by the National Natural Science Foundation of China(51874362 and 22209208)。
文摘柔性钠离子电池(SIBs)在便携式和可穿戴设备中具有巨大的应用潜力,因为它们在特定情况下具有适用性和价格优势.在正极材料中,磷酸盐电极材料具有结构稳定性好、工作电位高和寿命长的优点.然而,由于对制造要求苛刻,反应复杂,以及柔性基材的缺失等问题,柔性磷酸盐电极材料的设计仍然是一个巨大的挑战.在此,我们报道了在柔性多孔碳纳米纤维上垂直生长的VO_(2)纳米片原位转化为三维氟磷酸钒钠纳米棒阵列(PCNF@NVOPF NR).PCNF@NVOPF NR实现了兼具柔性与高压正极电极的特点,并具有长期循环稳定性(4500次循环后容量保持率为87.6%).阵列结构可以确保快速的钠反应动力学和低界面电阻.此外,PCNF@NVOPF NR//PCNF@VO_(2)NS@C钠离子全电池表现出高能量和功率密度(220.5 W h kg^(-1)和9400 W kg^(-1)).这种用于柔性正极的材料设计策略可促进实用钠离子电池的商业化.
基金supported by the National Natural Science Foundation of China(No.91963118)Science Technology Program of Jilin Province(No.20200201066JC)+2 种基金Fundamental Research Funds for the Central Universities(No.2412020QD013)China Postdoctoral Science Foundation(No.2019M661187)the National Postdoctoral Program for Innovative Talents(BX20190064).
文摘Flexible power sources featuring high-performance,prominent flexibility and raised safety have received mounting attention in the area of wearable electronic devices.However,many great challenges remain to be overcome,notably the design and fabrication of flexible electrodes with excellent electrochemical performance and matching them with safe and reliable electrolytes.Herein,a facile approach for preparing flexible electrodes,which employs carbon cloth derived from commercial cotton cloth as the substrate of cathode and a flexible anode,is proposed and investigated.The promising cathode(NVPOF@FCC)with high conductivity and outstanding flexibility is prepared by efficiently coating Na_(3)V_(2)(PO_(4))_(2)O_(2)F(NVPOF)on flexible carbon cloth(FCC),which exhibits remarkable electrochemical performance and the significantly improved reaction kinetics.More importantly,a novel flexible quasi-solid-state sodium-ion full battery(QSFB)is feasibly assembled by sandwiching a P(VDF-HFP)-NaClO_(4) gel-polymer electrolyte film between the advanced NVPOF@FCC cathode and FCC anode.And the QSFBs are further evaluated in flexible pouch cells,which not only demonstrates excellent energy-storage performance in aspect of great cycling stability and high-rate capability,but also impressive flexibility and safety.This work offers a feasible and effective strategy for the design of flexible electrodes,paving the way for the progression of practical and sustainable flexible batteries.
