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Nano-Micro Letters 2022年第9期14卷 132-146页

作者： Na Cheng Wang Zhou Jilei Liu Zhigang Liu Bingan Lu School of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082People’s Republic of China School of Materials Science and Engineering Hunan UniversityChangsha 410082People’s Republic of China School of Physics and Electronics Hunan UniversityChangsha 410082People’s Republic of China

Studies have found that oxygen-rich-containing functional groups in carbon-based materials can be used as active sites for the storage performance of K^(+),but the basic storage mechanism is still unclear.Herein,we construct and optimize 3D honeycomb-like carbon grafted with plentiful COOH/C=O functional groups(OFGC)as anodes for potassium ion batteries.The OFGC electrode with steady structure and rich functional groups can effectively contribute to the capacity enhancement and the formation of stable solid electrolyte interphase(SEI)film,achieving a high reversible capacity of 230 mAh g^(-1) at 3000 mA g^(-1) after 10,000 cycles(almost no capacity decay)and an ultra-long cycle time over 18 months at 100 mA g^(-1).The study results revealed the reversible storage mechanism between K^(+)and COOH/C=O functional groups by forming C-O-K compounds.Meanwhile,the in situ electrochemical impedance spectroscopy proved the highly reversible and rapid de/intercalation kinetics of K+in the OFGC electrode,and the growth process of SEI films.In particular,the full cells assembled by Prussian blue cathode exhibit a high energy density of 113 Wh kg^(-1) after 800 cycles(calculated by the total mass of anode and cathode),and get the light-emitting diodes lamp and ear thermometer running.

关键词： Honeycomb-like Super-long Carbon anode Potassium-ion batteries

半离子C-F键在钾离子电池碳负极中诱导快速离子储存和电子转移

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Science China Materials 2023年第7期66卷 2630-2640页

作者：袁飞宋薇张迪吴玉胜李昭进王欢王伟王秋君王波 School of Materials Science and Engineering Shenyang University of TechnologyShenyang 110870China Hebei Key Laboratory of Flexible Functional Materials School of Materials Science and EngineeringHebei University of Science and TechnologyShijiazhuang 050018China School of Metallurgical and Ecological Engineering University of Science and Technology BeijingBeijing 100083China

氟(F)杂原子功能化的碳负极可以形成更多的缺陷位点,从而有效提高钾的存储容量.然而,提高电化学性能的机制尚不清楚,尤其是对何种C-F键深入影响钾储存性能仍缺乏基本认识.本文报道了一系列F掺杂的碳,并证明了C-F是半离子键而不是离子键... 详细信息

氟(F)杂原子功能化的碳负极可以形成更多的缺陷位点,从而有效提高钾的存储容量.然而,提高电化学性能的机制尚不清楚,尤其是对何种C-F键深入影响钾储存性能仍缺乏基本认识.本文报道了一系列F掺杂的碳,并证明了C-F是半离子键而不是离子键;碳化温度对缺陷程度有显著影响.并且,高比例半离子C-F键诱导的丰富缺陷可以作为活性位点来吸附大量与电容行为相关的钾离子,不仅有利于长循环寿命,而且提升了在高电流密度下的倍率容量.密度泛函理论计算证实半离子C-F键的存在可以提高碳基体对钾离子的吸附能力并同时提高电子电导率,有利于高容量和倍率.此外,通过耦合半离子C-F键和吡啶N键,钾吸附能和电导率被进一步提升,这使得半电池实现了优异的容量(245.2 mA h g^(-1))和倍率,并且组装的全电池具有高能量密度(143.9 W h kg^(-1)).

关键词： F-doping adsorption energy Carbon anode potassium-ion battery

Interconnected carbon nanocapsules with high N/S co-doping as stable and high-capacity potassium-ion battery anode

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Journal of Energy Chemistry 2022年第3期31卷 195-204,I0007页

作者： Honghui Bi Xiaojun He Lei Yang Hongqiang Li Biyu Jin Jieshan Qiu School of Chemistry and Chemical Engineering Anhui Key Laboratory of Coal Clean Conversion and High Valued UtilizationKey Lab of Metallurgical Emission Reduction&Resources RecyclingMinistry of EducationAnhui University of TechnologyMaanshan 243002AnhuiChina College of Chemical Engineering Beijing University of Chemical TechnologyBeijing 100029China

carbonaceous materials have drawn much attention in potassium-ion batteries (PIBs) due to their low price and superior physicochemical properties. However, the application of carbonaceous materials in PIB anodes is hindered by sluggish kinetics and large volume expansion. Herein, N/S co-doped carbon nanocapsule (NSCN) is constructed for superior K+ storage. The NSCN possesses 3D nanocapsule framework with abundant meso/macropores, which guarantees structural robustness and accelerates ions/electrons transportation. The high-level N/S co-doping in carbon matrix not only generates ample defects and active sites for K+ adsorption, but also expands interlayer distance for facile K+ intercalation/deintercalation. As a result, the NSCN electrode delivers a high reversible capacity (408 mAh g^(−1) at 0.05 A g^(−1)), outstanding rate capability (149 mAh g^(−1) at 5 A g^(−1)) and favorable cycle stability (150m Ah g^(−1) at 2 A g^(−1) after 2000 cycles). Ex situ TEM, Raman and XPS measurements demonstrate the excellent stability and reversibility of NSCN electrode during potassiation/depotassiation process. This work provides inspiration for the optimization of energy storage materials by structure and doping engineering.

关键词： 3D carbon nanocapsules N/S co-doping Carbon anode Potassium-ion battery

Nitrogen and oxygen co-doped mesoporous carbon spheres as capacitive anode for high performance sodium-ion capacitors

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Journal of Materials Science & Technology 2021年第24期83卷 188-195页

作者： Chunhai Jiang Wenyang Zhou Zhimin Zou Fujian Provincial Key Laboratory of Functional Materials and Applications Institute of Advanced Energy MaterialsSchool of Materials Science and EngineeringXiamen University of TechnologyXiamen361024China

The poor rate capability of battery-type anode is usually the bottleneck of the power-energy outputs of a hybrid alkaline metal ion capacitor.In this work,nitrogen and oxygen co-doped mesoporous carbon spheres with excellent rate performance and cycle stability are used as anode materials of sodium ion capacitors(SICs).The high N and O element doping levels as well as the amorphous and mesoporous structure have enabled prominent capacitive Na ion storage behavior,which in turn match well with the capacitive cathode in the hybrid device.Under optimum conditions,the SIC delivers a high energy density of 103.1 Wh kg^(-1)at a power density of 205.6 W kg^(-1).Even at a high power density of 7520 W kg^(-1),an energy density of 23.5 Wh kg^(-1)is still maintained.Moreover,a robust cycle stability with capacity retention of 84.6%after 2500 cycles at 1 A g^(-1)is maintained.Such excellent electrochemical performances convincingly demonstrate that the all-carbon based SICs with the highly capacitive N and O co-doped mesoporous Carbon anode can be promising Na ion-based energy storage devices alternative to their Li ion-based counterparts.

关键词： N and O co-doping Carbon anode Na-ion capacitors Energy density Cycle stability

Hollow carbon microbox from acetylacetone as anode material for sodium-ion batteries

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Journal of Energy Chemistry 2020年第12期29卷 293-302页

作者： Tianyun Qiu Wanwan Hong Lin Li Yu Zhang Peng Cai Cheng Liu Jiayang Li Guoqiang Zou Hongshuai Hou Xiaobo Ji Hunan Province Key Laboratory of Chemical Power Source.State Key Laboratory of Powder Metallurgy College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083HunanChina

carbon-based materials have attracted much interest as one of the promising anodes for sodium-ion batteries. However, low utilization of electrolyte and slow ion-transfer rate during electrochemical process hinder the further application of traditional bulk carbon. In order to enhance the diffusion kinetics and maintain the reversibility, hierarchical hollow carbon microbox was successfully prepared through a tunable bottom-up self-template routine for sodium-ion batteries. During annealing process, the morphology construction and activation happened synchronously. Based on that, a range of cross-linked porous nanosheet and hollow microbox were attained by manipulating reactant condition. The generation of texture and physical property are analyzed and are established linkages related to the electrochemical behavior. As results depicted in kinetic exploration and simulation based on cyclic voltammetry, the surfacecontrolled electrochemical behavior gradually turns to be the diffusion-controlled behavior as the hollow microbox evolves to porous nanosheet. The probable reason is that the rational microstructure/texture design leads to the accelerated diffusion kinetic procedure and the reduced concentration difference polarization. Sodium storage mechanism was deduced as reversible binding of Na-ions with local defects,including vacancies on sp2 graphitic layers, at the edges of flakes and other structural defects instead of intercalation. Bestowed by the morphology design, the broad pore width distribution, abundant defects/active sites and surface functionality, hollow microbox electrode delivers great electrochemical performances. This work is expected to propose a novel and effective strategy to prepare tunable hierarchical hollow carbon microbox and induce the fast kinetic of Carbon anode material.

关键词： Na-ion battery Carbon anode Hollow carbon Sodium storage Electrochemistry

Electrocatalysis of Carbon anode in aluminium electrolysis

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Rare Metals 2002年第2期21卷 117-122页

作者： LAIYanqing LIUYexiang YANGJianhong THONSTADJomar Dept.MetallurgicalScience&Engineering CentralSouthUniversityChangsha410083.China Dept.MaterialsTechnologyandElectrochemistry NorwegianUniversityofScienceandTechnologyTrondheim7491Norway

The anodic over voltage of the Carbon anode in aluminumelectrolysis is of the order of 0.6 V at normal current densities.However, it can be reduced somewhat by doping the anode carbon withvarious inorganic compounds. A new apparatus was designed to improvethe precision of over voltage measurements. anodes were doped withMgAl_2O_4 and AlF_3 both by impregnation of the coke and by addingpowder, and the measured over voltage was compared with that ofUndoped samples. For prebake type anodes baked at around 1150 deg. C,the anodic overvoltage was reduced by 40-60 mV, And for Soderbergtype anodes, baked at 950 deg. C, by 60-80 mV.

关键词： electrocatalysis Carbon anode aluminum electrolysis

Porous current collector enables carbon superior electrochemical performance for K-ion capacitors

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Rare Metals 2023年第1期42卷 134-145页

作者： Mei-Qi Liu Hui-Ming Li Zai-Yuan Le Jin-Fu Zhao Li-Min Chang Luan Fang Mei-Qi Hou Hai-Rui Wang Tian-Hao Xu Ping Nie Key Laboratory of Preparation and Applications of Environmental Friendly Material of the Ministry of Education College of ChemistryJilin Normal UniversityChangchun130103China Department of Chemical and Biomolecular Engineering University of CaliforniaLos AngelesCA90095USA

The current collector is an indispensable component in potassium-ion hybrid capacitors,which not only provides mechanical support to load electrode materials,but also collects and outputs the current generated.Herein,we investigate the effect of three different current collectors on the electrochemical properties of potassium ion capacitors using carbon black anode as a demonstration.Because of better adhesion and lower charge transfer resistance,the specific capacity of half-cells assembled using three-dimensional(3D)porous copper foil(PCu)and copper as current collector is better than that of Al foil,which stabilizes at 138.2 and 132.8 mAh·g^(-1)after 100 cycles at 0.05 A·g^(-1).The potassium-ion capacitor assembled using PCu exhibits an excellent energy/power density of 86.1 Wh·kg^(-1)and 4000 W·kg^(-1),respectively.This work will boost the rational design and provide an effective strategy to improve the performance of potassium-ion capacitors.

关键词： Porous copper Current collector anode Carbon anode Potassium-ion capacitor(PIC)

carbon materials toward efficient potassium storage:Rational design,performance evaluation and potassium storage mechanism

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Green Energy & Environment 2023年第1期8卷 115-140页

作者： Daping Qiu Yanglong Hou Beijing Key Laboratory for Magnetoelectric Materials and Devices Beijing Innovation Centre for Engineering Science and Advanced TechnologySchool of Materials Science and EngineeringPeking UniversityBeijing100871China

Potassium-ion batteries(PIBs)are potential“Beyond Li-ion Batteries”candidates for their resource advantage and low standard electrode potential.To date,the research on PIBs is in its early stages,the most urgent task is to develop high-performance electrode materials and reveal their potassium storage mechanism.For PIBs anode materials,carbon with tunable microstructure,excellent electrochemical activity,nontoxicity and low price is considered as one of the most promising anode materials for commercialization.Although some breakthrough works have emerged,the overall electrochemical performance of the reported Carbon anode is still far away from practical application.Herein,we carry out a comprehensive overview of PIBs Carbon anode in terms of three aspects of rational design of structure,performance evaluation criteria and characterization of potassium storage mechanism.First,the regulation mechanism of key structural features of Carbon anode on its potassium storage performance and the representative structural regulation strategies are introduced.Then,in view of the undefined performance evaluation criteria of PIBs Carbon anode,a reference principle for evaluating the potassium storage performance of Carbon anode is proposed.Finally,the advanced characterization techniques for the potassium storage mechanism of Carbon anode are summarize.This review aims to provide guidance for the development of practical PIBs anode.

关键词： Potassium-ion batteries Carbon anode Structural engineering Performance evaluation Potassium storage mechanism

From Micropores to Ultra-micropores inside Hard carbon: Toward Enhanced Capacity in Room-/ Low-Temperature Sodium-Ion Storage

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Nano-Micro Letters 2021年第6期13卷 297-310页

作者： Jinlin Yang Xiaowei Wang Wenrui Dai Xu Lian Xinhang Cui Weichao Zhang Kexin Zhang Ming Lin Ruqiang Zou Kian Ping Loh Quan-Hong Yang Wei Chen Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207People’s Republic of China Department of Chemistry National University of Singapore3 Science Drive 3Singapore 117543Singapore National University of Singapore(Suzhou)Research Institute 377 Lin Quan StreetSuzhou Industrial ParkSuzhou 215123JiangsuChina Department of Physics National University of Singapore2 Science Drive 3Singapore 117542Singapore Nanoyang Group State Key Laboratory of Chemical EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350People’s Republic of China Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials Department of Materials Science and EngineeringCollege of EngineeringPeking UniversityBeijing 100871People’s Republic of China Institute of Materials Research and Engineering(IMRE) Agency of ScienceTechnologyand Research(A*STAR)3 Research LinkSingapore 117602Singapore

Pore structure of hard carbon has a fundamental influence on the electrochemical properties in sodium-ion batteries(SIBs).Ultra-micropores(1 nm)inside carbon into ultra-micropores(<0.5 nm).Consequently,the designed ca... 详细信息

Pore structure of hard carbon has a fundamental influence on the electrochemical properties in sodium-ion batteries(SIBs).Ultra-micropores(carbon can function as ionic sieves to reduce the diffusion of slovated Na+but allow the entrance of naked Na^(+) into the pores,which can reduce the interficial contact between the electrolyte and the inner pores without sacrificing the fast diffusion kinetics.Herein,a molten diffusion-carbonization method is proposed to transform the micropores(>1 nm)inside carbon into ultra-micropores(Carbon anode displays an enhanced capacity of 346 mAh g^(−1) at 30 mA g^(−1) with a high ICE value of~80.6%and most of the capacity(~90%)is below 1 V.Moreover,the high-loading electrode(~19 mg cm^(−2))exhibits a good temperature endurance with a high areal capacity of 6.14 mAh cm^(−2) at 25℃ and 5.32 mAh cm^(−2) at −20℃.Based on the in situ X-ray diffraction and ex situ solid-state nuclear magnetic resonance results,the designed ultra-micropores provide the extra Na+storage sites,which mainly contributes to the enhanced capacity.This proposed strategy shows a good potential for the development of high-performance SIBs.

关键词： Carbon anode Ultra-micropores Extra sodium-ion storage sites Low-voltage capacity High areal capacity

Precise synthesis of N-doped graphitic carbon via chemical vapor deposition to unravel the dopant functions on potassium storage toward practical K-ion batteries

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Nano Research 2021年第5期14卷 1413-1420页

作者： Yu Zhao Zhongti Sun Yuyang Yi Chen Lu Menglei Wang Zhou Xia Xueyu Lian Zhongfan Liu Jingyu Sun College of Energy Soochow Institute for Energy and Materials InnovationS(SIEMIS)Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou215006China Center for Nanochemistry(CNC) Beijing Science and Engineering Center for NanocarbonsCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China

Nitrogen doped carbon is a burgeoning anode candidate for potassium-ion battery(PIBs)owing to its outstanding attributes.It is imperative to grasp further insight into specific effects of different nitrogen dopants in Carbon anode toward advanced K-ion storage.However,the prevailing fabrication method is plagued by the fact that considerable variations in the total N-doping concentration occur in the course of regulating the type of nitrogen dopants,incapable of distinguishing the certain roles of them under similar conditions.Herein,throughout the precise preparation of high edge-N doped carbon(HENC)and high graphitic-N doped carbon(HGNC)harnessing basically identical N-doping levels(5.78 at.%for HENC;5.07 at.%for HGNC)via chemical vapor deposition route,the effects of edge-N and graphitic-N in the Carbon anode on K-ion storage are revisited,offering guidance into the design of low-cost and high-performance PIB systems.

关键词： nitrogen doping Carbon anode potassium storage adsorption voltage