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
Orthorhombic Nb_(2)O_(5)(T-Nb_(2)O_(5))is attractive for fast-charging Li-ion batteries,but it is still hard to realize rapid charge transfer kinetics for Li-ion storage.Herein,F-doped T-Nb_(2)O_(5) microflowers(F-Nb_(...Orthorhombic Nb_(2)O_(5)(T-Nb_(2)O_(5))is attractive for fast-charging Li-ion batteries,but it is still hard to realize rapid charge transfer kinetics for Li-ion storage.Herein,F-doped T-Nb_(2)O_(5) microflowers(F-Nb_(2)O_(5))are rationally synthesized through topotactic conversion.Specifically,F-Nb_(2)O_(5) are assembled by single-crystal nanoflakes with nearly 97%exposed(100)facet,which maximizes the exposure of the feasible Li^(+)transport pathways along loosely packed 4g atomic layers to the electrolytes,thus effectively enhancing the Li^(+)-intercalation performance.Besides,the band gap of F-Nb_(2)O_(5) is reduced to 2.87 eV due to the doping of F atoms,leading to enhanced electrical conductivity.The synergetic effects between tailored exposed crystal facets,F-doping,and ultrathin building blocks,speed up the Li^(+)/electron transfer kinetics and improve the pseudocapacitive properties of F-Nb_(2)O_(5).Therefore,F-Nb_(2)O_(5) exhibit superior rate capability(210.8 and 164.9 mAh g^(-1) at 1 and 10 C,respectively)and good long-term 10 C cycling performance(132.7 mAh g^(-1) after 1500 cycles).展开更多
Although different NbO_(x) units are present in Nb_(2)O_(5)‐based catalysts,the correlations between these structures and activity remain unclear,which considerably hinders the further development of Nb_(2)O_(5) phot...Although different NbO_(x) units are present in Nb_(2)O_(5)‐based catalysts,the correlations between these structures and activity remain unclear,which considerably hinders the further development of Nb_(2)O_(5) photocatalysis.Herein,we utilized N‐hydroxyphthalimide(NHPI)as the probe molecule to distinguish the role of different NbO_(x) units in the activation of C–H bond under visible light irradia‐tion.With the addition of NHPI,Nb_(2)O_(5) catalysts with highly disordered NbO_(6) units exhibited higher activities than that with slightly disordered NbO_(6) units(419‒495 vs.82μmol·g^(-1)·h^(-1))in photocata‐lytic selective oxidation of ethylbenzene.Revealed by Raman spectra,electron paramagnetic reso‐nance spectra,and transmission‐electron‐microscopy images,highly disordered NbO_(6) units were confirmed to act as the active sites for the transfer of photogenerated electrons from NHPI,pro‐moting the generation of phthalimide‐N‐oxyl(PINO)radicals for the enhanced conversion of ethylbenzene under visible light irradiation.This study provides guidance on the role of local NbO_(x) units in Nb_(2)O_(5) photocatalysis.展开更多
Two-dimensional carbon nitride(2 D-C_(3) N_(4))nanosheets are promising materials in photocatalytic water splitting,but still suffer from easy agglomeration and fast photogene rated electron-hole pairs recombination.T...Two-dimensional carbon nitride(2 D-C_(3) N_(4))nanosheets are promising materials in photocatalytic water splitting,but still suffer from easy agglomeration and fast photogene rated electron-hole pairs recombination.To tackle this issue,herein,a hierarchical Nb_(2) O_(5)/2 D-C_(3) N_(4) heterostructure is precisely constructed and the built-in electric field between Nb_(2)O_(5) and 2 D-C_(3) N_(4) can provide the driving force to separate/transfer the charge carriers efficiently.Moreover,the strongly Lewis acidic Nb_(2)O_(5) can adsorb TEOA molecules on its surface at locally high concentrations to facilitate the oxidation reaction kinetics under irradiation,resulting in efficient photogene rated electrons-holes separation and exceptional photocatalytic hydrogen evolution.As expected,the champion Nb_(2)O_(5)/2 D-C_(3)N_(4) heterostructure achieves an exceptional H2 evolution rate of 31.6 mmol g^(-1) h^(-1),which is 213.6 times and 4.3 times higher than that of pristine Nb_(2)O_(5) and2 D-C_(3)N_(4),respectively.Moreover,the champion heterostructure possesses a high apparent quantum efficiency(AQE)of 45.08%atλ=405 nm and superior cycling stability.Furthermore,a possible photocatalytic mechanism of the energy band alignment at the hetero-interface is proposed based on the systematical characterizations accompanied by density functional theory(DFT)calculations.This work paves the way for the precise construction of a high-quality heterostructured photocatalyst with efficient charge separation to boost hydrogen production.展开更多
The integration of nano-semiconductors into electromagnetic wave absorption materials is a highly desirable strategy for intensifying dielectric polarization loss;achieving high-attenuation microwave absorption and re...The integration of nano-semiconductors into electromagnetic wave absorption materials is a highly desirable strategy for intensifying dielectric polarization loss;achieving high-attenuation microwave absorption and realizing in-depth comprehension of dielectric loss mechanisms remain challenges.Herein,ultrafine oxygen vacancy-rich Nb_(2)O_(5)semiconductors are confined in carbon nanosheets(ov-Nb_(2)O_(5)/CNS)to boost dielectric polarization and achieve high attenuation.The polarization relaxation,electromagnetic response,and impedance matching of the ov-Nb_(2)O_(5)/CNS are significantly facilitated by the Nb_(2)O_(5)semiconductors with rich oxygen vacancies,which consequently realizes an extremely high attenuation performance of-80.8 dB(>99.999999%wave absorption)at 2.76 mm.As a dielectric polarization center,abundant Nb_(2)O_(5)–carbon heterointerfaces can intensify interfacial polarization loss to strengthen dielectric polarization,and the presence of oxygen vacancies endows Nb_(2)O_(5)semiconductors with abundant charge separation sites to reinforce electric dipole polarization.Moreover,the three-dimensional reconstruction of the absorber using microcomputer tomography technology provides insight into the intensification of the unique lamellar morphology regarding multiple reflection and scattering dissipation characteristics.Additionally,ov-Nb_(2)O_(5)/CNS demonstrates excellent application potential by curing into a microwave-absorbing,machinable,and heat-dissipating plate.This work provides insight into the dielectric polarization loss mechanisms of nano-semiconductor/carbon composites and inspires the design of high-performance microwave absorption materials.展开更多
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supported by the National Natural Science Foundation of China(No.51802163)the Natural Science Foundation of Henan Province of China(No.222300420252)the Natural Science Foundation of Henan Department of Education(No.20A480004).
文摘Orthorhombic Nb_(2)O_(5)(T-Nb_(2)O_(5))is attractive for fast-charging Li-ion batteries,but it is still hard to realize rapid charge transfer kinetics for Li-ion storage.Herein,F-doped T-Nb_(2)O_(5) microflowers(F-Nb_(2)O_(5))are rationally synthesized through topotactic conversion.Specifically,F-Nb_(2)O_(5) are assembled by single-crystal nanoflakes with nearly 97%exposed(100)facet,which maximizes the exposure of the feasible Li^(+)transport pathways along loosely packed 4g atomic layers to the electrolytes,thus effectively enhancing the Li^(+)-intercalation performance.Besides,the band gap of F-Nb_(2)O_(5) is reduced to 2.87 eV due to the doping of F atoms,leading to enhanced electrical conductivity.The synergetic effects between tailored exposed crystal facets,F-doping,and ultrathin building blocks,speed up the Li^(+)/electron transfer kinetics and improve the pseudocapacitive properties of F-Nb_(2)O_(5).Therefore,F-Nb_(2)O_(5) exhibit superior rate capability(210.8 and 164.9 mAh g^(-1) at 1 and 10 C,respectively)and good long-term 10 C cycling performance(132.7 mAh g^(-1) after 1500 cycles).
文摘Although different NbO_(x) units are present in Nb_(2)O_(5)‐based catalysts,the correlations between these structures and activity remain unclear,which considerably hinders the further development of Nb_(2)O_(5) photocatalysis.Herein,we utilized N‐hydroxyphthalimide(NHPI)as the probe molecule to distinguish the role of different NbO_(x) units in the activation of C–H bond under visible light irradia‐tion.With the addition of NHPI,Nb_(2)O_(5) catalysts with highly disordered NbO_(6) units exhibited higher activities than that with slightly disordered NbO_(6) units(419‒495 vs.82μmol·g^(-1)·h^(-1))in photocata‐lytic selective oxidation of ethylbenzene.Revealed by Raman spectra,electron paramagnetic reso‐nance spectra,and transmission‐electron‐microscopy images,highly disordered NbO_(6) units were confirmed to act as the active sites for the transfer of photogenerated electrons from NHPI,pro‐moting the generation of phthalimide‐N‐oxyl(PINO)radicals for the enhanced conversion of ethylbenzene under visible light irradiation.This study provides guidance on the role of local NbO_(x) units in Nb_(2)O_(5) photocatalysis.
基金Finacial support from the Natural Science Foundation of Jiangsu Province(BK20170549,BK20180887)the National Natural Science Foundation of China(21706103,62004084)+3 种基金Guangdong Innovation Research Team for Higher Education(2017KCXTD030)the High-level Talents Project of Dongguan University of Technology(KCYKYQD2017017)the Young Talent Cultivation Plan of Jiangsu UniversityJiangsu Provincial Program for High-Level Innovative and Entrepreneurial Talents Introduction。
文摘Two-dimensional carbon nitride(2 D-C_(3) N_(4))nanosheets are promising materials in photocatalytic water splitting,but still suffer from easy agglomeration and fast photogene rated electron-hole pairs recombination.To tackle this issue,herein,a hierarchical Nb_(2) O_(5)/2 D-C_(3) N_(4) heterostructure is precisely constructed and the built-in electric field between Nb_(2)O_(5) and 2 D-C_(3) N_(4) can provide the driving force to separate/transfer the charge carriers efficiently.Moreover,the strongly Lewis acidic Nb_(2)O_(5) can adsorb TEOA molecules on its surface at locally high concentrations to facilitate the oxidation reaction kinetics under irradiation,resulting in efficient photogene rated electrons-holes separation and exceptional photocatalytic hydrogen evolution.As expected,the champion Nb_(2)O_(5)/2 D-C_(3)N_(4) heterostructure achieves an exceptional H2 evolution rate of 31.6 mmol g^(-1) h^(-1),which is 213.6 times and 4.3 times higher than that of pristine Nb_(2)O_(5) and2 D-C_(3)N_(4),respectively.Moreover,the champion heterostructure possesses a high apparent quantum efficiency(AQE)of 45.08%atλ=405 nm and superior cycling stability.Furthermore,a possible photocatalytic mechanism of the energy band alignment at the hetero-interface is proposed based on the systematical characterizations accompanied by density functional theory(DFT)calculations.This work paves the way for the precise construction of a high-quality heterostructured photocatalyst with efficient charge separation to boost hydrogen production.
基金supported by National Natural Science Foundation of China(No.22078100,No.52102098,and No.22008073)Fundamental Research Funds for the Central Universities(No.222201718002)。
文摘The integration of nano-semiconductors into electromagnetic wave absorption materials is a highly desirable strategy for intensifying dielectric polarization loss;achieving high-attenuation microwave absorption and realizing in-depth comprehension of dielectric loss mechanisms remain challenges.Herein,ultrafine oxygen vacancy-rich Nb_(2)O_(5)semiconductors are confined in carbon nanosheets(ov-Nb_(2)O_(5)/CNS)to boost dielectric polarization and achieve high attenuation.The polarization relaxation,electromagnetic response,and impedance matching of the ov-Nb_(2)O_(5)/CNS are significantly facilitated by the Nb_(2)O_(5)semiconductors with rich oxygen vacancies,which consequently realizes an extremely high attenuation performance of-80.8 dB(>99.999999%wave absorption)at 2.76 mm.As a dielectric polarization center,abundant Nb_(2)O_(5)–carbon heterointerfaces can intensify interfacial polarization loss to strengthen dielectric polarization,and the presence of oxygen vacancies endows Nb_(2)O_(5)semiconductors with abundant charge separation sites to reinforce electric dipole polarization.Moreover,the three-dimensional reconstruction of the absorber using microcomputer tomography technology provides insight into the intensification of the unique lamellar morphology regarding multiple reflection and scattering dissipation characteristics.Additionally,ov-Nb_(2)O_(5)/CNS demonstrates excellent application potential by curing into a microwave-absorbing,machinable,and heat-dissipating plate.This work provides insight into the dielectric polarization loss mechanisms of nano-semiconductor/carbon composites and inspires the design of high-performance microwave absorption materials.
