Developing suitable anode materials for potassium-ion batteries(PIBs)remains a great challenge owing to the limited theoretical capacity of active materials and large radius of K+ion(1.38?).To solve these obstacles,by...Developing suitable anode materials for potassium-ion batteries(PIBs)remains a great challenge owing to the limited theoretical capacity of active materials and large radius of K+ion(1.38?).To solve these obstacles,by integrating the principles of multielectron transfer and rational porous crystal framework,we creatively propose the monoclinic Cu_(3)(OH)_(2)V_(2)O_(7)·2H_(2)O(CVO)as a novel anode for PIBs.Furthermore,inspired by the metastable nature of CVO under high temperature/pressure,we skillfully design a facile hydrothermal recrystallization strategy without the phase change and surfactants addition.Thus,for the first time,the porous composite of Cu_(3)(OH)_(2)V_(2)O_(7)·2H_(2)O nanobelts covered in situ by reduced graphene oxide(CVO NBs/r GO)was assembled,greatly improving the deficiencies of CVO.When used as a novel anode for PIBs,CVO NBs/r GO delivers large specific capacity(up to 551.4 m Ah g^(-1)at 50 m A g^(-1)),high-rate capability(215.3 m Ah g^(-1)at 2.5 A g^(-1))and super durability(203.6 m Ah g^(-1)at 500 m A g^(-1)even after 1000 cycles).The outstanding performance can be ascribed to the synergistic merits of desirable structural features of monoclinic CVO nanobelts and the highly conductive graphene 3D network,thus promoting the composite material stability and electrical/ionic conductivity.This work reveals a novel metal vanadate-based anode material for PIBs,would further motivate the subsequent batteries research on M_(3)(OH)_(2)V_(2)O_(7)-n H_(2)O(M;Co,Ni,Cu,Zn),and ultimately expands valuable fundamental understanding on designing other high-performance electrode materials,including the combined strategies of multielectron transfer with rational porous crystal framework,and the composite fabrication of 1D electrode nanostructure with conductive carbon matrix.展开更多
Electromagnetic wave absorber is critical for reducing increasingly serious electromagnetic wave pollu-tion,however,the development of lightweight and broadband microwave absorbers remains a pressing challenge.We repo...Electromagnetic wave absorber is critical for reducing increasingly serious electromagnetic wave pollu-tion,however,the development of lightweight and broadband microwave absorbers remains a pressing challenge.We report here the rational design and synthesis of N-doped Ni@SiO_(2)/graphene composite con-structed from 3D interconnected porous graphene network and Ni@SiO_(2) core-shell architecture,which fulfills lightweight and broadband requirements while exhibiting highly efficient electromagnetic wave absorption.The porous graphene network,functioning both as lightweight support and dielectric medi-ator,was synthesized via NaCl template-assisted high-temperature calcination method.Upon uniformly attached with core-shell Ni@SiO_(2) on the surface,the resulting abundant heterogeneous interfaces con-structed by graphene-Ni and Ni-SiO_(2) strongly reinforce polarization loss.The presence of low dielectric SiO_(2) allows facile tuning of the complex permittivity of ternary composite by adjusting coating thick-ness to balance the attenuation ability and impedance matching.Moreover,further N-doping of graphene assists in the optimization of dielectric loss ability.Taking account of the advantages arising from the porous hierarchical architecture,multiple absorption centers and diverse interfaces,the lightweight com-posite exhibits an ultra-strong reflection loss(RL)value of-71.13 dB at 13.76 GHz with a thickness of 2.46 mm and broad effective absorption bandwidth of 7.04 GHz at a low filler content of 15 wt.%.More importantly,the effective absorption range covers 13.28 GHz(4.72-18 GHz)with the optimized thickness of 1.6-5 mm,representing 83%of the whole range of frequencies.Our results demonstrate that the novel 3D porous N-doped Ni@SiO_(2)/graphene network with hierarchical architecture is a promising candidate for high-performance electromagnetic wave absorption.展开更多
Carbon nanotube (CNT) clusters grown in situ in three-dimensional (3D) porous graphene networks (3DG-CNTs), with integrated structure and remarkable electronic conductivity, are desirable S host materials for Li...Carbon nanotube (CNT) clusters grown in situ in three-dimensional (3D) porous graphene networks (3DG-CNTs), with integrated structure and remarkable electronic conductivity, are desirable S host materials for Li-S batteries. 3DG-CNT exhibits a high surface area (1,645 m^2·g^-1), superior electronic conductivity of 1,055 S·m^-1, and a 3D porous networked structure. Large clusters of CNTs anchored on the inner walls of 3D graphene networks act as capillaries, benefitting restriction of agglomeration by high contents of immersed S. Moreover, the capillary-like CNT clusters grown in situ in the pores efficiently form restricted spaces for Li polysulfides, significantly reducing the shuttling effect and promoting S utilization throughout the charge/discharge process. With an areal S mass loading of 81.6 wt.%, the 3DG-CNT/S electrode exhibits an initial specific capacity reaching 1,229 mA·h·g^-1 at 0.5 C and capacity decays of 0.044% and 0.059% per cycle at 0.5 and 1 C, respectively, over 500 cycles. The electrode material also reveals a remarkable rate performance and the large capacity of 812 mA·h·g^-1 at 3 C.展开更多
基金supported by the National Natural Science Foundation of China(52072118,51772089)the Youth 1000 Talent Program of China+3 种基金the Research and Development Plan of Key Areas in Hunan Province(2019GK2235)the Key Research and Development Program of Ningxia(2020BDE03007)the China Postdoctoral Science Foundation(2019M653649)the Guangdong Basic and Applied Basic Research Fund(2019A1515110518,2019A1515111188,2020B0909030004)。
文摘Developing suitable anode materials for potassium-ion batteries(PIBs)remains a great challenge owing to the limited theoretical capacity of active materials and large radius of K+ion(1.38?).To solve these obstacles,by integrating the principles of multielectron transfer and rational porous crystal framework,we creatively propose the monoclinic Cu_(3)(OH)_(2)V_(2)O_(7)·2H_(2)O(CVO)as a novel anode for PIBs.Furthermore,inspired by the metastable nature of CVO under high temperature/pressure,we skillfully design a facile hydrothermal recrystallization strategy without the phase change and surfactants addition.Thus,for the first time,the porous composite of Cu_(3)(OH)_(2)V_(2)O_(7)·2H_(2)O nanobelts covered in situ by reduced graphene oxide(CVO NBs/r GO)was assembled,greatly improving the deficiencies of CVO.When used as a novel anode for PIBs,CVO NBs/r GO delivers large specific capacity(up to 551.4 m Ah g^(-1)at 50 m A g^(-1)),high-rate capability(215.3 m Ah g^(-1)at 2.5 A g^(-1))and super durability(203.6 m Ah g^(-1)at 500 m A g^(-1)even after 1000 cycles).The outstanding performance can be ascribed to the synergistic merits of desirable structural features of monoclinic CVO nanobelts and the highly conductive graphene 3D network,thus promoting the composite material stability and electrical/ionic conductivity.This work reveals a novel metal vanadate-based anode material for PIBs,would further motivate the subsequent batteries research on M_(3)(OH)_(2)V_(2)O_(7)-n H_(2)O(M;Co,Ni,Cu,Zn),and ultimately expands valuable fundamental understanding on designing other high-performance electrode materials,including the combined strategies of multielectron transfer with rational porous crystal framework,and the composite fabrication of 1D electrode nanostructure with conductive carbon matrix.
基金supported by the National Natural Science Foundation of China (Nos.91963204 and 51871053)Shanghai Pujiang Program (No.19PJ1400200)the Fundamental Research Funds for the Central Universities (Nos.2232019G-07 and 2232020A-02)。
文摘Electromagnetic wave absorber is critical for reducing increasingly serious electromagnetic wave pollu-tion,however,the development of lightweight and broadband microwave absorbers remains a pressing challenge.We report here the rational design and synthesis of N-doped Ni@SiO_(2)/graphene composite con-structed from 3D interconnected porous graphene network and Ni@SiO_(2) core-shell architecture,which fulfills lightweight and broadband requirements while exhibiting highly efficient electromagnetic wave absorption.The porous graphene network,functioning both as lightweight support and dielectric medi-ator,was synthesized via NaCl template-assisted high-temperature calcination method.Upon uniformly attached with core-shell Ni@SiO_(2) on the surface,the resulting abundant heterogeneous interfaces con-structed by graphene-Ni and Ni-SiO_(2) strongly reinforce polarization loss.The presence of low dielectric SiO_(2) allows facile tuning of the complex permittivity of ternary composite by adjusting coating thick-ness to balance the attenuation ability and impedance matching.Moreover,further N-doping of graphene assists in the optimization of dielectric loss ability.Taking account of the advantages arising from the porous hierarchical architecture,multiple absorption centers and diverse interfaces,the lightweight com-posite exhibits an ultra-strong reflection loss(RL)value of-71.13 dB at 13.76 GHz with a thickness of 2.46 mm and broad effective absorption bandwidth of 7.04 GHz at a low filler content of 15 wt.%.More importantly,the effective absorption range covers 13.28 GHz(4.72-18 GHz)with the optimized thickness of 1.6-5 mm,representing 83%of the whole range of frequencies.Our results demonstrate that the novel 3D porous N-doped Ni@SiO_(2)/graphene network with hierarchical architecture is a promising candidate for high-performance electromagnetic wave absorption.
基金This work was supported by the Innovation Project of Guangxi Graduate Education (No. P3090098101), the China Postdoctoral Science Foundation (No. 2017M612864), the Major International (Regional) Joint Research Project (No. 51210002), the National Basic Research Program of China (No. 2015CB932304) and the Natural Science Foundation of Guangdong province (No. 2015A030312007).
文摘Carbon nanotube (CNT) clusters grown in situ in three-dimensional (3D) porous graphene networks (3DG-CNTs), with integrated structure and remarkable electronic conductivity, are desirable S host materials for Li-S batteries. 3DG-CNT exhibits a high surface area (1,645 m^2·g^-1), superior electronic conductivity of 1,055 S·m^-1, and a 3D porous networked structure. Large clusters of CNTs anchored on the inner walls of 3D graphene networks act as capillaries, benefitting restriction of agglomeration by high contents of immersed S. Moreover, the capillary-like CNT clusters grown in situ in the pores efficiently form restricted spaces for Li polysulfides, significantly reducing the shuttling effect and promoting S utilization throughout the charge/discharge process. With an areal S mass loading of 81.6 wt.%, the 3DG-CNT/S electrode exhibits an initial specific capacity reaching 1,229 mA·h·g^-1 at 0.5 C and capacity decays of 0.044% and 0.059% per cycle at 0.5 and 1 C, respectively, over 500 cycles. The electrode material also reveals a remarkable rate performance and the large capacity of 812 mA·h·g^-1 at 3 C.