Josephson junction plays a key role not only in studying the basic physics of unconventional iron-based superconductors but also in realizing practical application of thin-film based devices,therefore the preparation ...Josephson junction plays a key role not only in studying the basic physics of unconventional iron-based superconductors but also in realizing practical application of thin-film based devices,therefore the preparation of high-quality iron pnictide Josephson junctions is of great importance.In this work,we have successfully fabricated Josephson junctions from Co-doped BaFe_(2)As_(2)thin films using a direct junction fabrication technique which utilizes high energy focused helium ion beam(FHIB).The electrical transport properties were investigated for junctions fabricated with various He^(+)irradiation doses.The junctions show sharp superconducting transition around 24 K with a narrow transition width of 2.5 K,and a dose correlated foot-structure resistance which corresponds to the effective tuning of junction properties by He^(+)irradiation.Significant J_c suppression by more than two orders of magnitude can be achieved by increasing the He^(+)irradiation dose,which is advantageous for the realization of low noise ion pnictide thin film devices.Clear Shapiro steps are observed under 10 GHz microwave irradiation.The above results demonstrate the successful fabrication of high quality and controllable Co-doped BaFe_(2)As_(2)Josephson junction with high reproducibility using the FHIB technique,laying the foundation for future investigating the mechanism of iron-based superconductors,and also the further implementation in various superconducting electronic devices.展开更多
Planar Na ion micro-supercapacitors(NIMSCs) that offer both high energy density and power density are deemed to a promising class of miniaturized power sources for wearable and portable microelectron-ics. Nevertheless...Planar Na ion micro-supercapacitors(NIMSCs) that offer both high energy density and power density are deemed to a promising class of miniaturized power sources for wearable and portable microelectron-ics. Nevertheless, the development of NIMSCs are hugely impeded by the low capacity and sluggish Na ion kinetics in the negative electrode.Herein, we demonstrate a novel carbon-coated Nb_(2)O_5 microflower with a hierarchical structure composed of vertically intercrossed and porous nanosheets, boosting Na ion storage performance. The unique structural merits, including uniform carbon coating, ultrathin nanosheets and abun-dant pores, endow the Nb_(2)O_5 microflower with highly reversible Na ion storage capacity of 245 mAh g^(-1) at 0.25 C and excellent rate capability.Benefiting from high capacity and fast charging of Nb_(2)O_5 microflower, the planar NIMSCs consisted of Nb_(2)O_5 negative electrode and activated car-bon positive electrode deliver high areal energy density of 60.7 μWh cm^(-2),considerable voltage window of 3.5 V and extraordinary cyclability. Therefore, this work exploits a structural design strategy towards electrode materials for application in NIMSCs, holding great promise for flexible microelectronics.展开更多
The large volumetric variations experienced by metal selenides within conversion reaction result in inferior rate capability and cycling stability,ultimately hindering the achievement of superior electrochemical perfo...The large volumetric variations experienced by metal selenides within conversion reaction result in inferior rate capability and cycling stability,ultimately hindering the achievement of superior electrochemical performance.Herein,metallic Cu_(2)Se encapsulated with N-doped carbon(Cu_(2)Se@NC)was prepared using Cu_(2)O nanocubes as templates through a combination of dopamine polymerization and hightemperature selenization.The unique nanocubic structure and uniform N-doped carbon coating could shorten the ion transport distance,accelerate electron/charge diffusion,and suppress volume variation,ultimately ensuring Cu_(2)Se@NC with excellent electrochemical performance in sodium ion batteries(SIBs)and potassium ion batteries(PIBs).The composite exhibited excellent rate performance(187.7 mA h g^(-1)at 50 A g^(-1)in SIBs and 179.4 mA h g^(-1)at 5 A g^(-1)in PIBs)and cyclic stability(246,8 mA h g^(-1)at 10 A g^(-1)in SIBs over 2500 cycles).The reaction mechanism of intercalation combined with conversion in both SIBs and PIBs was disclosed by in situ X-ray diffraction(XRD)and ex situ transmission electron microscope(TEM).In particular,the final products in PIBs of K_(2)Se and K_(2)Se_(3)species were determined after discharging,which is different from that in SIBs with the final species of Na_(2)Se.The density functional theory calculation showed that carbon induces strong coupling and charge interactions with Cu_(2)Se,leading to the introduction of built-in electric field on heterojunction to improve electron mobility.Significantly,the theoretical calculations discovered that the underlying cause for the relatively superior rate capability in SIBs to that in PIBs is the agile Na~+diffusion with low energy barrier and moderate adsorption energy.These findings offer theoretical support for in-depth understanding of the performance differences of Cu-based materials in different ion storage systems.展开更多
Zinc metal anodes are gaining popularity in aqueous electrochemical energy storage systems for their high safety,cost-effectiveness,and high capacity.However,the service life of zinc metal anodes is severely constrain...Zinc metal anodes are gaining popularity in aqueous electrochemical energy storage systems for their high safety,cost-effectiveness,and high capacity.However,the service life of zinc metal anodes is severely constrained by critical challenges,including dendrites,water-induced hydrogen evolution,and passivation.In this study,a protective two-dimensional metal–organic framework interphase is in situ constructed on the zinc anode surface with a novel gel vapor deposition method.The ultrathin interphase layer(~1μm)is made of layer-stacking 2D nanosheets with angstrom-level pores of around 2.1Å,which serves as an ion sieve to reject large solvent–ion pairs while homogenizes the transport of partially desolvated zinc ions,contributing to a uniform and highly reversible zinc deposition.With the shielding of the interphase layer,an ultra-stable zinc plating/stripping is achieved in symmetric cells with cycling over 1000 h at 0.5 mA cm−2 and~700 h at 1 mA cm^(−2),far exceeding that of the bare zinc anodes(250 and 70 h).Furthermore,as a proof-of-concept demonstration,the full cell paired with MnO_(2) cathode demonstrates improved rate performances and stable cycling(1200 cycles at 1 A g−1).This work provides fresh insights into interphase design to promote the performance of zinc metal anodes.展开更多
Ion beam-induced luminescence(IBIL) experiments were performed to investigate the in situ luminescence of GaN/Al_(2)O_(3) at varying ion energies,which allowed for the measurement of defects at different depths within...Ion beam-induced luminescence(IBIL) experiments were performed to investigate the in situ luminescence of GaN/Al_(2)O_(3) at varying ion energies,which allowed for the measurement of defects at different depths within the material.The energies of H^(+)were set to 500 keV,640 keV and 2 MeV,the Bragg peaks of which correspond to the GaN film,GaN/Al_(2)O_(3) heterojunction and Al_(2)O_(3) substrate,respectively.A photoluminescence measurement at 250 K was also performed for comparison,during which only near band edge(NBE) and yellow band luminescence in the GaN film were observed.The evolution of the luminescence of the NBE and yellow band in the GaN film was discussed,and both exhibited a decrease with the fluence of H^(+).Additionally,the luminescence of F centers,induced by oxygen vacancies,and Cr^(3+),resulting from the ^(2)E →^(4)A_(2) radiative transition in Al_(2)O_(3),were measured using 2 MeV H^(+).The luminescence intensity of F centers increases gradually with the fluence of H^(+).The luminescence evolution of Cr^(3+)is consistent with a yellow band center,attributed to its weak intensity,and it is situated within the emission band of the yellow band in the GaN film.Our results show that IBIL measurement can effectively detect the luminescence behavior of multilayer films by adjusting the ion energy.Luminescence measurement can be excited by various techniques,but IBIL can satisfy in situ luminescence measurement,and multilayer structural materials of tens of micrometers can be measured through IBIL by adjusting the energy of the inducing ions.The evolution of defects at different layers with ion fluence can be obtained.展开更多
Cu-based catalysts are widely employed for CO_(2) hydrogenation to methanol,which is expected as a promising process to achieving carbon neutrality.However,most Cu-based catalysts still suffer from low methanol yield ...Cu-based catalysts are widely employed for CO_(2) hydrogenation to methanol,which is expected as a promising process to achieving carbon neutrality.However,most Cu-based catalysts still suffer from low methanol yield with a passable CO_(2) conversion and lack insight into its reaction mechanism for guiding the design of catalysts.In this work,Cu^(+)/CeZrO_(x) interfaces are engineered by employing a series of ceria-zirconia solid solution catalysts with various Ce/Zr ratios,forming a Cu^(+)-O_(v)-Ce^(3+)structure where Cu^(+)atoms are bonded to the oxygen vacancies(O_(v))of ceria.Compared to Cu/CeO_(2) and Cu/ZrO_(2),the optimized catalyst(i.e.,Cu_(0.3)Ce_(0.3)Zr_(0.7))exhibits a much higher mass-specific methanol formation rate(192g_(MeOH)/kg_(cat)/h)at 240℃and 3 MPa.Through a series of in-situ and ex-situ characterization,it is revealed that oxygen vacancies in solid solutions can effectively assist the activation of CO_(2) and tune the electronic state of copper to promote the formation of Cu^(+)/CeZrO_(x) interfaces,which stabilizes the key*CO intermediate,inhibits its desorption and facilitates its further hydrogenation to methanol via the reverse watergas-shift(RWGS)+CO-Hydro pathway.Therefore,the concentration of*CO or the apparent Cu^(+)/(Cu^(+)+Cu^(0))ratio could be employed as a quantitative descriptor of the methanol formation rate.This work is expected to give a deep insight into the mechanism of metal/support interfaces in CO_(2) hydrogenation to methanol,offering an effective strategy to develop new catalysts with high performance.展开更多
MoS_(2)targets were irradiated by infra-red(IR)pulsed laser in a high vacuum to determine hot plasma parameters,atomic,molecular and ion emission,and angular and charge state distributions.In this way,pulsed laser dep...MoS_(2)targets were irradiated by infra-red(IR)pulsed laser in a high vacuum to determine hot plasma parameters,atomic,molecular and ion emission,and angular and charge state distributions.In this way,pulsed laser deposition(PLD)of thin films on graphene oxide substrates was also realized.An Nd:YAG laser,operating at the 1064 nm wavelength with a 5 ns pulse duration and up to a 1 J pulse energy,in a single pulse or at a 10 Hz repetition rate,was employed.Ablation yield was measured as a function of the laser fluence.Plasma was characterized using different analysis techniques,such as time-of-flight measurements,quadrupole mass spectrometry and fast CCD visible imaging.The so-produced films were characterized by composition,thickness,roughness,wetting ability,and morphology.When compared to the MoS_(2)targets,they show a slight decrease of S with respect to Mo,due to higher ablation yield,low fusion temperature and high sublimation in vacuum.The pulsed IR laser deposited Mo Sx(with 1<x<2)films are uniform,with a thickness of about 130 nm,a roughness of about 50 nm and a higher wettability than the MoS_(2)targets.Some potential applications of the pulsed IR laser-deposited Mo Sx films are also presented and discussed.展开更多
基金Project supported by the National Key Research and Development Program of China (Grant Nos.2020YFF01014706 and 2017YFC0601901)the National Natural Science Foundation of China (Grant Nos.61571019 and 52177026)。
文摘Josephson junction plays a key role not only in studying the basic physics of unconventional iron-based superconductors but also in realizing practical application of thin-film based devices,therefore the preparation of high-quality iron pnictide Josephson junctions is of great importance.In this work,we have successfully fabricated Josephson junctions from Co-doped BaFe_(2)As_(2)thin films using a direct junction fabrication technique which utilizes high energy focused helium ion beam(FHIB).The electrical transport properties were investigated for junctions fabricated with various He^(+)irradiation doses.The junctions show sharp superconducting transition around 24 K with a narrow transition width of 2.5 K,and a dose correlated foot-structure resistance which corresponds to the effective tuning of junction properties by He^(+)irradiation.Significant J_c suppression by more than two orders of magnitude can be achieved by increasing the He^(+)irradiation dose,which is advantageous for the realization of low noise ion pnictide thin film devices.Clear Shapiro steps are observed under 10 GHz microwave irradiation.The above results demonstrate the successful fabrication of high quality and controllable Co-doped BaFe_(2)As_(2)Josephson junction with high reproducibility using the FHIB technique,laying the foundation for future investigating the mechanism of iron-based superconductors,and also the further implementation in various superconducting electronic devices.
基金financially supported by the National Natural Science Foundation of China (Grants. 22075279, 22279137, 22125903, 22109040)National Key R&D Program of China (Grant 2022YFA1504100)+2 种基金Dalian Innovation Support Plan for High Level Talents (2019RT09)Dalian National Labo- ratory For Clean Energy (DNL), CAS, DNL Cooperation Fund, CAS (DNL202016, DNL202019), DICP (DICP I2020032)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy (YLU-DNL Fund 2021002, YLU- DNL Fund 2021009)。
文摘Planar Na ion micro-supercapacitors(NIMSCs) that offer both high energy density and power density are deemed to a promising class of miniaturized power sources for wearable and portable microelectron-ics. Nevertheless, the development of NIMSCs are hugely impeded by the low capacity and sluggish Na ion kinetics in the negative electrode.Herein, we demonstrate a novel carbon-coated Nb_(2)O_5 microflower with a hierarchical structure composed of vertically intercrossed and porous nanosheets, boosting Na ion storage performance. The unique structural merits, including uniform carbon coating, ultrathin nanosheets and abun-dant pores, endow the Nb_(2)O_5 microflower with highly reversible Na ion storage capacity of 245 mAh g^(-1) at 0.25 C and excellent rate capability.Benefiting from high capacity and fast charging of Nb_(2)O_5 microflower, the planar NIMSCs consisted of Nb_(2)O_5 negative electrode and activated car-bon positive electrode deliver high areal energy density of 60.7 μWh cm^(-2),considerable voltage window of 3.5 V and extraordinary cyclability. Therefore, this work exploits a structural design strategy towards electrode materials for application in NIMSCs, holding great promise for flexible microelectronics.
基金The Natural Science Foundation of Henan Province(222300420083)the Opening Foundation of State Key Laboratory of Chemistry and Utilization of Carbon-based Energy Resource of Xinjiang University(KFKT2021004)。
文摘The large volumetric variations experienced by metal selenides within conversion reaction result in inferior rate capability and cycling stability,ultimately hindering the achievement of superior electrochemical performance.Herein,metallic Cu_(2)Se encapsulated with N-doped carbon(Cu_(2)Se@NC)was prepared using Cu_(2)O nanocubes as templates through a combination of dopamine polymerization and hightemperature selenization.The unique nanocubic structure and uniform N-doped carbon coating could shorten the ion transport distance,accelerate electron/charge diffusion,and suppress volume variation,ultimately ensuring Cu_(2)Se@NC with excellent electrochemical performance in sodium ion batteries(SIBs)and potassium ion batteries(PIBs).The composite exhibited excellent rate performance(187.7 mA h g^(-1)at 50 A g^(-1)in SIBs and 179.4 mA h g^(-1)at 5 A g^(-1)in PIBs)and cyclic stability(246,8 mA h g^(-1)at 10 A g^(-1)in SIBs over 2500 cycles).The reaction mechanism of intercalation combined with conversion in both SIBs and PIBs was disclosed by in situ X-ray diffraction(XRD)and ex situ transmission electron microscope(TEM).In particular,the final products in PIBs of K_(2)Se and K_(2)Se_(3)species were determined after discharging,which is different from that in SIBs with the final species of Na_(2)Se.The density functional theory calculation showed that carbon induces strong coupling and charge interactions with Cu_(2)Se,leading to the introduction of built-in electric field on heterojunction to improve electron mobility.Significantly,the theoretical calculations discovered that the underlying cause for the relatively superior rate capability in SIBs to that in PIBs is the agile Na~+diffusion with low energy barrier and moderate adsorption energy.These findings offer theoretical support for in-depth understanding of the performance differences of Cu-based materials in different ion storage systems.
基金supported by the grants from the Research Grants Council of the Hong Kong Special Administrative Region,China(Project No.C5031-20)the Guangdong Major Project of Basic and Applied Basic Research(2023B0303000002).
文摘Zinc metal anodes are gaining popularity in aqueous electrochemical energy storage systems for their high safety,cost-effectiveness,and high capacity.However,the service life of zinc metal anodes is severely constrained by critical challenges,including dendrites,water-induced hydrogen evolution,and passivation.In this study,a protective two-dimensional metal–organic framework interphase is in situ constructed on the zinc anode surface with a novel gel vapor deposition method.The ultrathin interphase layer(~1μm)is made of layer-stacking 2D nanosheets with angstrom-level pores of around 2.1Å,which serves as an ion sieve to reject large solvent–ion pairs while homogenizes the transport of partially desolvated zinc ions,contributing to a uniform and highly reversible zinc deposition.With the shielding of the interphase layer,an ultra-stable zinc plating/stripping is achieved in symmetric cells with cycling over 1000 h at 0.5 mA cm−2 and~700 h at 1 mA cm^(−2),far exceeding that of the bare zinc anodes(250 and 70 h).Furthermore,as a proof-of-concept demonstration,the full cell paired with MnO_(2) cathode demonstrates improved rate performances and stable cycling(1200 cycles at 1 A g−1).This work provides fresh insights into interphase design to promote the performance of zinc metal anodes.
文摘Ion beam-induced luminescence(IBIL) experiments were performed to investigate the in situ luminescence of GaN/Al_(2)O_(3) at varying ion energies,which allowed for the measurement of defects at different depths within the material.The energies of H^(+)were set to 500 keV,640 keV and 2 MeV,the Bragg peaks of which correspond to the GaN film,GaN/Al_(2)O_(3) heterojunction and Al_(2)O_(3) substrate,respectively.A photoluminescence measurement at 250 K was also performed for comparison,during which only near band edge(NBE) and yellow band luminescence in the GaN film were observed.The evolution of the luminescence of the NBE and yellow band in the GaN film was discussed,and both exhibited a decrease with the fluence of H^(+).Additionally,the luminescence of F centers,induced by oxygen vacancies,and Cr^(3+),resulting from the ^(2)E →^(4)A_(2) radiative transition in Al_(2)O_(3),were measured using 2 MeV H^(+).The luminescence intensity of F centers increases gradually with the fluence of H^(+).The luminescence evolution of Cr^(3+)is consistent with a yellow band center,attributed to its weak intensity,and it is situated within the emission band of the yellow band in the GaN film.Our results show that IBIL measurement can effectively detect the luminescence behavior of multilayer films by adjusting the ion energy.Luminescence measurement can be excited by various techniques,but IBIL can satisfy in situ luminescence measurement,and multilayer structural materials of tens of micrometers can be measured through IBIL by adjusting the energy of the inducing ions.The evolution of defects at different layers with ion fluence can be obtained.
基金sponsored by the National Natural Science Foundation of China(21808120,21978148)。
文摘Cu-based catalysts are widely employed for CO_(2) hydrogenation to methanol,which is expected as a promising process to achieving carbon neutrality.However,most Cu-based catalysts still suffer from low methanol yield with a passable CO_(2) conversion and lack insight into its reaction mechanism for guiding the design of catalysts.In this work,Cu^(+)/CeZrO_(x) interfaces are engineered by employing a series of ceria-zirconia solid solution catalysts with various Ce/Zr ratios,forming a Cu^(+)-O_(v)-Ce^(3+)structure where Cu^(+)atoms are bonded to the oxygen vacancies(O_(v))of ceria.Compared to Cu/CeO_(2) and Cu/ZrO_(2),the optimized catalyst(i.e.,Cu_(0.3)Ce_(0.3)Zr_(0.7))exhibits a much higher mass-specific methanol formation rate(192g_(MeOH)/kg_(cat)/h)at 240℃and 3 MPa.Through a series of in-situ and ex-situ characterization,it is revealed that oxygen vacancies in solid solutions can effectively assist the activation of CO_(2) and tune the electronic state of copper to promote the formation of Cu^(+)/CeZrO_(x) interfaces,which stabilizes the key*CO intermediate,inhibits its desorption and facilitates its further hydrogenation to methanol via the reverse watergas-shift(RWGS)+CO-Hydro pathway.Therefore,the concentration of*CO or the apparent Cu^(+)/(Cu^(+)+Cu^(0))ratio could be employed as a quantitative descriptor of the methanol formation rate.This work is expected to give a deep insight into the mechanism of metal/support interfaces in CO_(2) hydrogenation to methanol,offering an effective strategy to develop new catalysts with high performance.
基金supported by OP RDE,MEYS,Czech Republic under the project CANAM OP(No.CZ.02.1.01/0.0/0.0/16_013/0001812)by the Czech Science Foundation GACR(No.23-06702S)。
文摘MoS_(2)targets were irradiated by infra-red(IR)pulsed laser in a high vacuum to determine hot plasma parameters,atomic,molecular and ion emission,and angular and charge state distributions.In this way,pulsed laser deposition(PLD)of thin films on graphene oxide substrates was also realized.An Nd:YAG laser,operating at the 1064 nm wavelength with a 5 ns pulse duration and up to a 1 J pulse energy,in a single pulse or at a 10 Hz repetition rate,was employed.Ablation yield was measured as a function of the laser fluence.Plasma was characterized using different analysis techniques,such as time-of-flight measurements,quadrupole mass spectrometry and fast CCD visible imaging.The so-produced films were characterized by composition,thickness,roughness,wetting ability,and morphology.When compared to the MoS_(2)targets,they show a slight decrease of S with respect to Mo,due to higher ablation yield,low fusion temperature and high sublimation in vacuum.The pulsed IR laser deposited Mo Sx(with 1<x<2)films are uniform,with a thickness of about 130 nm,a roughness of about 50 nm and a higher wettability than the MoS_(2)targets.Some potential applications of the pulsed IR laser-deposited Mo Sx films are also presented and discussed.