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Novel Bilayer-Shelled N,O-Doped Hollow Porous Carbon Microspheres as High Performance Anode for Potassium-Ion Hybrid Capacitors

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Nano-Micro Letters 2023年第9期15卷 423-435页

作者： Zhen Pan Yong qian Yang Li Xiaoning Xie Ning Lin yitai qian Department of Applied Chemistry University of Science and Technology of ChinaHefei 230026People’s Republic of China Yongjiang Laboratory Ningbo 315202People’s Republic of China China National Building Material Design&Research Institute Co. Ltd.No.208Huazhong RoadGongshu DistrictHangzhou 310022People’s Republic of China

With the advantages of high energy/power density,long cycling life and low cost,dual-carbon potassium ion hybrid capacitors(PIHCs)have great potential in the field of energy storage.Here,a novel bilayer-shelled N,O-doped hollow porous carbon microspheres(NOHPC)anode has been prepared by a self-template method,which is consisted of a dense thin shell and a hollow porous spherical core.Excitingly,the NOHPC anode possesses a high K-storage capacity of 325.9 mA h g^(−1)at 0.1 A g^(−1)and a capacity of 201.1 mAh g^(−1)at 5 A g^(−1)after 6000 cycles.In combination with ex situ characterizations and density functional theory calculations,the high reversible capacity has been demonstrated to be attributed to the co-doping of N/O heteroatoms and porous structure improved K+adsorption and intercalation capabilities,and the stable long-cycling performance originating from the bilayer-shelled hollow porous carbon sphere structure.Meanwhile,the hollow porous activated carbon microspheres(HPAC)cathode with a high specific surface area(1472.65 m^(2)g^(−1))deriving from etching NOHPC with KOH,contributing to a high electrochemical adsorption capacity of 71.2 mAh g^(−1)at 1 A g^(−1).Notably,the NOHPC//HPAC PIHC delivers a high energy density of 90.1 Wh kg^(−1)at a power density of 939.6 W kg^(−1)after 6000 consecutive charge-discharge cycles.

关键词： Self-template method Bilayer-shelled hollow porous structure N,O-doped carbon microspheres Dual-carbon potassium‐ion hybrid capacitor

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Molten-LiCl induced thermochemical prelithiation of SiOx:Regulating the active Si/O ratio for high initial Coulombic efficiency

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Nano Research 2022年第1期15卷 230-237页

作者： Yang Li Yong qian Jie Zhou Ning Lin yitai qian Department of Applied Chemistry University of Science and Technology of ChinaHefei 230026China Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China

The low initial Coulombic efficiency(ICE)of SiOx anode caused by the irreversible generation of LiySiOz and Li20 during lithiation process limits its application for high energy-density lithium-ion batteries.Herein,we report a molten-salt-induced thermochemical.prelithiation strategy for regulating the electrochemically active Si/O ratio of SiOx and thus enhancing ICE through thermal treatment of pre-synthesized LiNH2-coated SiOx in molten LiCl at 700℃.Bulk SiOx micro-particle was transformed into pomegranatelike prelithiated micro-cluster composite(M-Li-SiOx)with SiOx core and outer nano-sized agglomerates consisting of Li2Si20s,SiO2,and Si.Through the analysis of the reaction intermediates,molten-UC!could initiate reactions and promote mass transfer by the continuous extraction of oxygen component from SiOx particle inner in the form of inert Li2Si20s and SiO2 nanotubes to realize the.prelithiation.The degree of prelithiation can be regulated by adjusting the coating amount of LiNH2 layer,and the resulted M-Li-SiOx displays a prominent improvement of ICE from 58.73%to 88.2%.The graphite/M-Li-SiOx(8:2)composite electrode delivers a.discharge capacity of 497.29 mAh·g^(-1) with an ICE of 91.79%.By pairing graphite/M-Li-SiOx anode and LiFeP04 cathode in a full-cell an enhancement of energy density of 37.25%is realized compared with the full-cell containing graphite/SiOx anode.Furthermore,,ex-situ X-ray photoelectron spectroscopy(XPS)/Raman/X-ray diffraction(XRD)and related electrochemical measurements reveal the SiOx core and Si of M-Li-SiOx participate in the lithiation,and pre-generated Li2Si20s with u+diffusivity and pomegranate-like.structure reduces the reaction resistance and interface impedance of the solid electrolyte interphase(SEI)film.

关键词： initial Coulombic efficiency thermochemical prelithiation liquid coating molten-salt mass transfer

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A chiral salen-Co(Ⅱ)complex as soluble redox mediator for promoting the electrochemical performance of Li-O_(2) batteries

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Nano Research 2022年第9期15卷 8101-8108页

作者： Hao Wan Yingjie Sun Jia Yu qianqi Shi Yongchun Zhu yitai qian Hefei National Laboratory for Physical Science at Microscale and Department of Chemistry University of Science and Technology of ChinaHefei 230026China Hebei Key Laboratory of Photoelectric Control on Surface and Interface College of ScienceHebei University of Science and TechnologyShijiazhuang 050018China Materials Genome Institute Shanghai UniversityShanghai 200444China

Low discharge capacity and poor cycle stability are the major obstacles hindering the operation of Li-O_(2)batteries with highenergy-density.These obstacles are mainly caused by the cathode passivation behaviours and the accumulation of by-products.Promoting the discharge process in solution and accelerating the decomposition of discharge products and by-products are able to alleviate above problems to some extent.Herein,chiral salen-Co(Ⅱ)complex,(1R,2R)-(-)-N,N-bis(3,5-di-t-butylsalicylidene)-1,2-cyclohexanediaminocobalt(Ⅱ)(Co(Ⅱ))as a multi-functional redox mediator was introduced into electrolyte to induce solution phase formation of Li_(2)O_(2)and catalyze the oxidation of Li_(2)O_(2)and main by-products Li_(2)CO3.Due to the Co(Ⅱ)has the solvation effect towards Li+,it can drive solution phase formation of Li_(2)O_(2),to prevent electrode from passivation and then increase the discharge capacity with a high Li_(2)O_(2)yield of 96.09%.Furthermore,the Co(Ⅱ)possesses suitable redox couple potentials,and it does so while simultaneously boosting the oxidization of Li_(2)O_(2)and the decomposition of Li_(2)CO3,reducing charge overpotential,and promoting cycle lifespan.Thereby,a cell with Co(Ⅱ)achieved a long cycling stability at low charge plateau(3.66 V)over 252 cycles with a specific capacity of 500 mAh·gcarbon^(−1).

关键词： chiral salen-Co(Ⅱ)complex soluble redox mediator multi-redox potential trifunctional Li-O_(2)batteries

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Synthesis of carbon nanotubes-supported porous silicon microparticles in low-temperature molten salt for highperformance Li-ion battery anodes

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Nano Research 2022年第7期15卷 6184-6191页

作者： qianliang Zhang Baojuan Xi Weihua Chen Jinkui Feng yitai qian Shenglin Xiong Key Laboratory of Colloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringState Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100China Key Laboratory of Material Processing and Mold of Ministry of Education Zhengzhou UniversityZhengzhou 450001China Key Laboratory for Liquid-Solid Structural Evolution&Processing of Materials Ministry of EducationSchool of Materials Science and EngineeringShandong UniversityJinan 250061China

Silicon-based materials has attracted attention as a promising candidate for lithium-ion batteries(LIBs)with high energy density.However,severe volume variation,pulverization,and poor conductivity hindered the development of Si based materials.In this study,porous Si microparticles supported by carbon nanotubes(p-Si/CNT)are fabricated through simple molten salt assisted dealloying process at low temperature followed by acid treatment.The ZnCl2 molten salt not only provides the liquid environment to enhance the reaction,but also participates the dealloying process and works as template for porous structure when removes by acid treatment.Additionally,distribution of defect sites in CNTs also increases after molten salt process.Density function theory(DFT)calculations further prove the defects could improve the adsorption of Li+.The participation of CNTs can also contribute to the reaction kinetics and retain the integrity of the electrode.As expected,the p-Si/CNT anode manifests enhanced lithium-storage performance in terms of superior cycling stability and good rate capability.The p-Si/CNT//LiCoO_(2) full cell assembly further demonstrates its potential as a prospective anode for high-performance LIBs.

关键词： porous Si microparticles carbon nanotubes molten salt lithium-ion batteries

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Bipolar electrode architecture enables high-energy aqueous rechargeable sodium ion battery

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Nano Research 2022年第6期15卷 5072-5080页

作者： Zhiguo Hou Wutao Mao Zixiang Zhang Jiawu Chen Huaisheng Ao yitai qian School of Chemistry and Materials University of Science and Technology of ChinaHefei 230026China Jiangsu University of Technology Changzhou 213001China

Aqueous rechargeable sodium ion batteries(ARSIBs),with intrinsic safety,low cost,and greenness,are attracting more and more attentions for large scale energy storage application.However,the low energy density hampers their practical application.Here,a battery architecture designed by bipolar electrode with graphite/amorphous carbon film as current collector shows high energy density and excellent rate-capability.The bipolar electrode architecture is designed to not only improve energy density of practical battery by minimizing inactive ingredient,such as tabs and cases,but also guarantee high rate-capability through a short electron transport distance in the through-plane direction instead of in-plane direction for traditional cell architecture.As a proof of concept,a prototype pouch cell of 8 V based on six Na_(2)MnFe(CN)_(6)||NaTi_(2)(PO_(4))_(3)bipolar electrodes stacking using a“water-in-polymer”gel electrolyte is demonstrated to cycle up to 4,000 times,with a high energy density of 86 Wh·kg^(−1)based on total mass of both cathode and anode.This result opens a new avenue to develop advance high-energy ARSIBs for grid-scale energy storage applications.

关键词： aqueous rechargeable sodium ion battery bipolar electrode current collector water-in-polymer electrolyte

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Rational screening of metal coating on Zn anode for ultrahigh-cumulative-capacity aqueous zinc metal batteries

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Journal of Energy Chemistry 2023年第9期84卷 81-88页

作者： Dan Lv Huili Peng Cheng Wang Hongxia Liu Dongdong Wang Jian Yang yitai qian Key Laboratory of Colloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShandong UniversityJinan 250100ShandongChina School of Chemistry and Chemical Engineering Wuhan Textile UniversityWuhan 430200HubeiChina Hefei National Laboratory for Physical Science at Microscale Department of ChemistryUniversity of Science and Technology of ChinaHefei 230026AnhuiChina

Aqueous zinc metal batteries feature intrinsic safety,but suffer from severe dendrite growth and water-derived side reactions.Many metal coatings have been explored for stabilizing Zn metal anode via a trialand-error approach.Here,we propose an exercisable way to screen the potential metal coating on Zn anodes in view of de-polarization effect and dendrite-suppressing ability theoretically.As an output of this screening,cadmium(Cd) metal is checked experimentally.Therefore,symmetric ZnllZn cells using Cd coated Zn(Zn@Cd) exhibit an ultra-long cycle life of 3500 h(nearly 5 months) at a high current density of 10 mA cm^(-2),achieving a record-high cumulative capacity(35 A h cm^(-2)) compared to the previous reports.The full cells of Zn@Cd‖MnO_(2) display a markedly improved cycling performance under harsh conditions including a limited Zn supply(N/P ratio=1.7) and a high areal capacity(3.5 mA h cm^(-2)).The significance of this work lies in not only the first report of Cd coating for stabilizing Zn metal anode,but also a feasible way to screen the promising metal materials for other metal anodes.

关键词： Zinc metal batteries Cadmium coating Redox potentials Surface energy Cumulative capacity

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Phase-separated bimetal enhanced sodium storage:Dimer-like Sn-Bi@C heterostructures with high capacity and long cycle life

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Journal of Energy Chemistry 2023年第4期79卷 468-476页

作者： Xiaoxiao Hou Yansong Zhu qian Yao Jinmei Song Chunsheng Wang Yanli Zhou Suyuan Zeng Jian Yang yitai qian Key Laboratory of Colloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShandong UniversityJinan 250100ShandongChina Department of Environmental and Material Engineering Yantai UniversityYantai 264005ShandongChina Department of Chemistry and Chemical Engineering Liaocheng UniversityLiaocheng 252059ShandongChina Hefei National Laboratory for Physical Science at Microscale Department of ChemistryUniversity of Science and Technology of ChinaHefei 230026AnhuiChina

Phase boundaries facilitate the charge transportation and alleviate the intrinsic stress upon cycles.Therefore,how to achieve regular phase boundaries is very attractive.Herein,dimer-like Sn-Bi@C nanostructures,where is a well-defined phase boundary between Sn and Bi,have been prepared by a two-step process for the first time.The phase boundary not only provides additional and fast transportation for Na+,but also mitigates the structure stress/strain upon cycling.Therefore,Sn-Bi@C exhibits a high capacity(472.1 m A h g^(-1)at 2 A g^(-1)for 200 cycles),an ultra-long cyclic life(355.6 mA h g^(-1)at 5 A g^(-1)for 4500cycles)and an excellent rate performance(372 mA h g^(-1)at 10 A g^(-1))for sodium storage,much higher than those of Sn@C,Bi@C,and Sn@C+Bi@C.Notably,the full cells of Sn-Bi@C//Na_(3)V_(2)(PO_(4))_(3)/rGO(SnBi@C//NVP/rGO)demonstrate impressive performance(323 mA h g^(-1)at 2 A g^(-1)for 300 cycles).The underlying mechanism for such an excellent performance is elucidated by in-situ X-ray diffraction,exsitu scanning electron microscopy/high-resolution transmission electron microscopy and atomic force microscopy,revealing the good electrode stability and improved mechanical properties of Sn-Bi@C.The synthetic method is extended to dimer-like Sn-Pb@C and Sn-Ag@C heterostructures,which also exhibit the good cycle stability for sodium storage.

关键词： Bi Sn Alloy-type anodes Sodium-ion batteries Phase boundaries

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Cu_(3)P nanoparticles confined in nitrogen/phosphorus dual-doped porous carbon nanosheets for efficient potassium storage

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Journal of Energy Chemistry 2022年第3期31卷 339-347,I0009页

作者： Yuanxing Yun Baojuan Xi Yu Gu Fang Tian Weihua Chen Jinkui Feng yitai qian Shenglin Xiong Key Laboratory of Colloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringState Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100ShandongChina Key Laboratory of Material Processing and Mold of Ministry of Education Zhengzhou UniversityZhengzhou 450001HenanChina Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials Ministry of EducationSchool of Materials Science and EngineeringShandong UniversityJinan 250061ShandongChina

Immobilizing primary electroactive nanomaterials in porous carbon matrix is an effective approach for boosting the electrochemical performance of potassium-ion batteries (PIBs) because of the synergy among functional components. Herein, an integrated hybrid architecture composed of ultrathin Cu_(3)P nanoparticles (~20 nm) confined in porous carbon nanosheets (Cu_(3)P⊂NPCSs) as a new anode material for PIBs is synthesized through a rational self-designed self-templating strategy. Benefiting from the unique structural advantages including more active heterointerfacial sites, intimate and stable electrical contact, effectively relieved volume change, and rapid K^(+) ion migration, the Cu_(3)P⊂NPCSs indicate excellent potassium-storage performance involving high reversible capacity, exceptional rate capability, and cycling stability. Moreover, the strong adsorption of K^(+) ions and fast potassium-ion reaction kinetics in Cu_(3)P⊂NPCSs is verified by the theoretical calculation investigation. Noted, the intercalation mechanism of Cu_(3)P to store potassium ions is, for the first time, clearly confirmed during the electrochemical process by a series of advanced characterization techniques.

关键词： Cu_(3)P Potassium-ion batteries Nitrogen/phosphorus dual-doped porous carbon sheets Intercalation mechanism Heterointerface

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In-situ formation of hierarchical solid-electrolyte interphase for ultra-long cycling of aqueous zinc-ion batteries

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Nano Research 2023年第1期16卷 449-457页

作者： Shaojie Zhang Jiajia Ye Huaisheng Ao Mingying Zhang Xilong Li Zhibin Xu Zhiguo Hou yitai qian School of Chemistry and Chemical Engineering Shandong UniversityJinan 250100China School of Chemistry and Material Science University of Science and Technology of ChinaHefei 230026China

Aqueous rechargeable zinc ion batteries have received widespread attention due to their high energy density and low cost.However,zinc metal anodes face fatal dendrite growth and detrimental side reactions,which affect the cycle stability and practical application of zinc ion batteries.Here,an in-situ formed hierarchical solid-electrolyte interphase composed of InF3,In,and ZnF2 layers with outside-in orientation on the Zn anode(denoted as Zn@InF3)is developed by a sample InF3 coating.The inner ultrathin ZnF2 interface between Zn anode and InF3 layer formed by the spontaneous galvanic replacement reaction between InF3 and Zn,is conductive to achieving uniform Zn deposition and inhibits the growth of Zinc dendrites due to the high electrical resistivity and Zn2+conductivity.Meanwhile,the middle uniformly generated metallic In and outside InF3 layers functioning as corrosion inhibitor suppressing the side reaction due to the waterproof surfaces,good chemical inactivity,and high hydrogen evolution overpotential.Besides,the as-prepared zinc anode enables dendrite-free Zn plating/stripping for more than 6,000 h at nearly 100%coulombic efficiency(CE).Furthermore,coupled with the MnO2 cathode,the full battery exhibits the long cycle of up to 1,000 cycles with a low negative-to-positive electrode capacity(N/P)ratio of 2.8.

关键词： zinc ion batteries solid-electrolyte interphase in-situ formation hierarchical coating

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Petroleum coke derived porous carbon/NiCoP with efficient reviving catalytic and adsorptive activity as sulfur host for high performance lithium-sulfur batteries

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Nano Research 2022年第5期15卷 4058-4067页

作者： Bo Zhang Lu Wang Bin Wang Yanjun Zhai Shuyuan Zeng Meng Zhang yitai qian Liqiang Xu Key Laboratory of Colloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringState Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100China Key Laboratory/Collaborative Innovation Center of Chemical Energy Storage&Novel Cell Technology School of Chemistry and Chemical EngineeringLiaocheng UniversityLiaocheng 252000China

Sulfur-host material with abundant pore structure and high catalysis plays an important role in development of high-energy-density lithium-sulfur(Li-S)batteries.Herein,we implanted NiCoP nanoparticles into the N,S co-doped porous carbon derived from petroleum coke(PCPC)to fabricate the sulfur-host of PCPC/NiCoP composites.The high specific surface area of PCPC provides abundant adsorption sites for capturing LiPSs and the NiCoP nanoparticles to improve the polarity and boost the LiPSs conversion kinetics of PCPC.The Li-S cells fabricated with PCPC/NiCoP as sulfur-host deliver high discharge capacity of 1,462.7 mAh·g^(-1)under the current density of 0.1 C and exhibit ultralong lifespan over 800 cycles under the current density of 1,2,and even 5 C.Additionally,the prepared composites cathodes deliver an outstanding discharge capacity of 932.5 and 826.4 mAh·g^(-1)at 0.5 and 1 C with a high sulfur loading of over 3.90 mg·cm^(-2),and remain stable about 60 cycles.Furthermore,the promoted adsorption-conversion process of polysulfides by introducing NiCoP nanoparticles into PCPC was investigated by experimental and theoretical calculation studies.This work offers a new light for tacking the obstacles of porous carbon-based sulfur-host and propelling the development of petroleum coke-based porous carbon for high performance Li-S batteries.

关键词： porous carbon derived from petroleum coke(PCPC) NiCoP nanoparticles(NPs) lithium polysulfides(LiPSs) catalytic andadsorptiveactivity

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