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
Germanium(Ge), an alloy-type anode material for lithium-ion batteries(LIBs), possesses many advantages such as high theoretical capacity and decent electrical conductivity. Nevertheless, its application is restricted ...Germanium(Ge), an alloy-type anode material for lithium-ion batteries(LIBs), possesses many advantages such as high theoretical capacity and decent electrical conductivity. Nevertheless, its application is restricted by tremendous volume variation and tardy reaction kinetic during discharge/charge process.In this paper, the Ge/3DPG composites with Ge nanoparticles uniformly dispersed in 3D interconnected porous graphene(3DPG) skeleton are successfully prepared using a template-assisted in-situ reduction method. The unique 3D interconnected porous graphene can not only enhance the electronic conductivity and reaction kinetics of the materials, but also provide sufficient buffer space to effectively mitigate the volume expansion during cycling and strengthen the structural integrity. Moreover, the small-sized Ge nanoparticles in close conjunction with the 3D graphene can boost the surface-controlled reaction of the electrode, which contributes to a fast charge–discharge rate capability. The Ge/3DPG composite with optimized Ge/graphene mass ratio delivers high reversible specific capacity(1102 mAh g^(-1) after 100 cycles at 0.2 C), outstanding rate capability(494 mAh g^(-1) at 5 C), and admirable cycling stability(85.3% of capacity retention after 250 cycles at 0.5 C). This work provides a significant inspiration for the design and fabrication of advanced Ge-based anode materials for next-generation highperformance LIBs.展开更多
A new intercalation-type anode material is reported herein to improve the lithium storage kinetics for high-rate lithium ion capacitors.The crystal structure of orthorhombic NaNbO3 indicates two possible tunnels for l...A new intercalation-type anode material is reported herein to improve the lithium storage kinetics for high-rate lithium ion capacitors.The crystal structure of orthorhombic NaNbO3 indicates two possible tunnels for lithium ions insertion into NaNbO3 host along the<101>and<141>directions.Moreover,in situ XRD is conducted to investigate the lithium storage mechanism and structural evolution of the NaNb O_(3) anode,demonstrating its intercalation behavior through(101)and(141)planes.Furthermore,the rGO nanosheets are introduced to facilitate the charge transfer,which also effectively prevent the aggregation of NaNbO3 nanocubes.As expected,the NaNbO_(3)/rGO nanocomposites possess remarkable reversible capacity(465 mA h g^(-1) at 0.1 A g^(-1)),superior rate capability(325 mA h g^(-1) at 1.0 A g^(-1))and cycling stability,attributed to their synergistic effect and high Li+diffusion coefficient DLi[D(NaNbO_(3)/rGO)/D(NaNbO_(3))≈31.54].Remarkably,the NaNbO3/rGO-based LIC delivers a high energy density of 166.7 W h kg^(-1) at 112.4 W kg^(-1) and remains 24.1 W h kg^(-1) at an ultrahigh power density of26621.2 W kg^(-1),with an outstanding cycling durability(90%retention over 3000 cycles at 1.0 A g^(-1)).This study provides new insights on novel intercalation-type anode material to enrich the materials system of LICs.展开更多
High-efficiency sodium-ion batteries(SIBs) are in great demand for energy storage applications,which are dominated by the Na+storage performance of electrode materials.Here,a one-pot solvothermal method is developed t...High-efficiency sodium-ion batteries(SIBs) are in great demand for energy storage applications,which are dominated by the Na+storage performance of electrode materials.Here,a one-pot solvothermal method is developed to construct amorphous/crystalline MoO_(2)(a/c-MoO_(2)) homojunction for boosting Na+storage.Theoretical simulations signify that electrons redistribute at the homogenous interface of a/c-MoO_(2),resulting in an inbuilt driving force to easily adsorb charge carriers and promote the electron/ion transfer ability.Relying on its crystallographic superiorities,the a/c-MoO_(2)homojunction with high Na adsorbability(-1.61 eV) and low Na diffusion energy barrier(0.519 eV) achieves higher capacity(307 mA h g^(-1)at 0.1 A/g),better rate capability and cycling stability than either a-MoO_(2)or c-MoO_(2)counterpart.Combining in-situ X-ray diffraction(XRD) and ex-situ X-ray photoelectron spectroscopy(XPS)techniques,the ’adsorption-insertion-conversion’ mechanism is well established for Na+storage of MoO_(2).Our work opens new opportunities to optimize electrode materials via crystallographic engineering for efficient Na+storage,and helps to better understand the effects of homojunction structure in enhanced electrochemical performance.展开更多
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financially supported by the National Natural Science Foundation of China (21875091 and 51672114)the Shanghai Municipal Education Commission (QD2019008)。
文摘Germanium(Ge), an alloy-type anode material for lithium-ion batteries(LIBs), possesses many advantages such as high theoretical capacity and decent electrical conductivity. Nevertheless, its application is restricted by tremendous volume variation and tardy reaction kinetic during discharge/charge process.In this paper, the Ge/3DPG composites with Ge nanoparticles uniformly dispersed in 3D interconnected porous graphene(3DPG) skeleton are successfully prepared using a template-assisted in-situ reduction method. The unique 3D interconnected porous graphene can not only enhance the electronic conductivity and reaction kinetics of the materials, but also provide sufficient buffer space to effectively mitigate the volume expansion during cycling and strengthen the structural integrity. Moreover, the small-sized Ge nanoparticles in close conjunction with the 3D graphene can boost the surface-controlled reaction of the electrode, which contributes to a fast charge–discharge rate capability. The Ge/3DPG composite with optimized Ge/graphene mass ratio delivers high reversible specific capacity(1102 mAh g^(-1) after 100 cycles at 0.2 C), outstanding rate capability(494 mAh g^(-1) at 5 C), and admirable cycling stability(85.3% of capacity retention after 250 cycles at 0.5 C). This work provides a significant inspiration for the design and fabrication of advanced Ge-based anode materials for next-generation highperformance LIBs.
基金supported by the Natural Science Foundation of Jiangsu Province(No.BK20170549)the National Natural Science Foundation of China(No.21706103)Postdoctoral Science Foundation of Jiangsu Province(No.2019K295)。
文摘A new intercalation-type anode material is reported herein to improve the lithium storage kinetics for high-rate lithium ion capacitors.The crystal structure of orthorhombic NaNbO3 indicates two possible tunnels for lithium ions insertion into NaNbO3 host along the<101>and<141>directions.Moreover,in situ XRD is conducted to investigate the lithium storage mechanism and structural evolution of the NaNb O_(3) anode,demonstrating its intercalation behavior through(101)and(141)planes.Furthermore,the rGO nanosheets are introduced to facilitate the charge transfer,which also effectively prevent the aggregation of NaNbO3 nanocubes.As expected,the NaNbO_(3)/rGO nanocomposites possess remarkable reversible capacity(465 mA h g^(-1) at 0.1 A g^(-1)),superior rate capability(325 mA h g^(-1) at 1.0 A g^(-1))and cycling stability,attributed to their synergistic effect and high Li+diffusion coefficient DLi[D(NaNbO_(3)/rGO)/D(NaNbO_(3))≈31.54].Remarkably,the NaNbO3/rGO-based LIC delivers a high energy density of 166.7 W h kg^(-1) at 112.4 W kg^(-1) and remains 24.1 W h kg^(-1) at an ultrahigh power density of26621.2 W kg^(-1),with an outstanding cycling durability(90%retention over 3000 cycles at 1.0 A g^(-1)).This study provides new insights on novel intercalation-type anode material to enrich the materials system of LICs.
基金Financial support by National Natural Science Foundation of China(21706103 and U21A20311)Natural Science Foundation of Jiangsu Province(BK20170549)China Postdoctoral Science Foundation(2022M711381)。
文摘High-efficiency sodium-ion batteries(SIBs) are in great demand for energy storage applications,which are dominated by the Na+storage performance of electrode materials.Here,a one-pot solvothermal method is developed to construct amorphous/crystalline MoO_(2)(a/c-MoO_(2)) homojunction for boosting Na+storage.Theoretical simulations signify that electrons redistribute at the homogenous interface of a/c-MoO_(2),resulting in an inbuilt driving force to easily adsorb charge carriers and promote the electron/ion transfer ability.Relying on its crystallographic superiorities,the a/c-MoO_(2)homojunction with high Na adsorbability(-1.61 eV) and low Na diffusion energy barrier(0.519 eV) achieves higher capacity(307 mA h g^(-1)at 0.1 A/g),better rate capability and cycling stability than either a-MoO_(2)or c-MoO_(2)counterpart.Combining in-situ X-ray diffraction(XRD) and ex-situ X-ray photoelectron spectroscopy(XPS)techniques,the ’adsorption-insertion-conversion’ mechanism is well established for Na+storage of MoO_(2).Our work opens new opportunities to optimize electrode materials via crystallographic engineering for efficient Na+storage,and helps to better understand the effects of homojunction structure in enhanced electrochemical performance.
