Co-reporter:Ting Li, Aiqiong Qin, Lanlan Yang, Jie Chen, Qiufan Wang, Daohong Zhang, and Hanxi Yang
ACS Applied Materials & Interfaces June 14, 2017 Volume 9(Issue 23) pp:19900-19900
Publication Date(Web):May 24, 2017
DOI:10.1021/acsami.7b04407
Electrochemical conversion reactions of metal oxides provide a new avenue to build high capacity anodes for sodium-ion batteries. However, the poor rate performance and cyclability of these conversion anodes remain a significant challenge for Na-ion battery applications because most of the conversion anodes suffer from sluggish kinetics and irreversible structural change during cycles. In this paper, we report an Fe2O3 single crystallites/reduced graphene oxide composite (Fe2O3/rGO), where the Fe2O3 single crystallites with a particle size of ∼300 nm were uniformly anchored on the rGO nanosheets, which provide a highly conductive framework to facilitate electron transport and a flexible matrix to buffer the volume change of the material during cycling. This Fe2O3/rGO composite anode shows a very high reversible capacity of 610 mAh g–1 at 50 mA g–1, a high Coulombic efficiency of 71% at the first cycle, and a strong cyclability with 82% capacity retention after 100 cycles, suggesting a potential feasibility for sodium-ion batteries. More significantly, the present work clearly illustrates that an electrochemical conversion anode can be made with high capacity utilization, strong rate capability, and stable cyclability through appropriately tailoring the lattice structure, particle size, and electronic conduction channels for a simple transition-metal oxide, thus offering abundant selections for development of low-cost and high-performance Na-storage electrodes.Keywords: conversion anode; Fe2O3 single crystal; metal oxide; reduced graphene oxide nanosheets; sodium-ion batteries;
Co-reporter:Chun Fang;Yunhui Huang;Wuxing Zhang;Jiantao Han;Zhe Deng;Yuliang Cao;Hanxi Yang
Advanced Energy Materials 2016 Volume 6( Issue 5) pp:
Publication Date(Web):
DOI:10.1002/aenm.201501727
Sodium-ion batteries (SIBs) are now being actively developed as low cost and sustainable alternatives to lithium-ion batteries (LIBs) for large-scale electric energy storage applications. In recent years, various inorganic and organic Na compounds, mostly mimicked from their Li counterparts, have been synthesized and tested for SIBs, and some of them indeed demonstrate comparable specific capacity to the presently developed LIB electrodes. However, the lack of suitable cathode materials is still a major obstacle to the commercial development of SIBs. Here, we present a brief review on the recent developments of SIB cathodes, with a focus on low cost and high energy density materials (> 450 Wh kg−1 vs Na) together with discussion of their Na-storage mechanisms. The considerable differences in the structural requirements for Li- and Na-storage reactions mean that it is not sufficient to design SIB cathode materials by simply mimicking LIB materials, and therefore great efforts are needed to discover new materials and reaction mechanisms to further develop variable cathodes for advanced SIB technology. Some directions for future research and possible strategies for building advanced cathode materials are also proposed here.
Co-reporter:Fei Xu, Hongtao Wang, Jianghui Lin, Xiao Luo, Shun-an Cao and Hanxi Yang
Journal of Materials Chemistry A 2016 vol. 4(Issue 29) pp:11491-11497
Publication Date(Web):30 Jun 2016
DOI:10.1039/C6TA03956A
Redox-active organic imides are potential alternatives to transition-metal based cathodes for material-sustainable and environmentally friendly Na-ion batteries; however, their poor cyclability remains a challenge for battery applications. To address this issue, we use a redox-active anthraquinone to link the small carbonyl molecules to obtain a conjugated polymer with multiple redox-active centers. Herein, we synthesize four cathode-active poly(anthraquinonyl imide)s (PAQIs) from pyromellitic dianhydride (or 1,4,5,8-naphthalenetetracarboxylic dianhydride) and 1,4-diaminoanthraquinone (or 1,5-diaminoanthraquinone). The as-prepared PAQI materials exhibit a high reversible capacity of 190 mA h g−1 and a stable cyclability with 93% capacity retention over 150 cycles, suggesting a possible use of these organic cathode materials for high capacity Na-ion batteries.
Co-reporter:Ya Xiong, Jiangfeng Qian, Yuliang Cao, Xinping Ai and Hanxi Yang
Journal of Materials Chemistry A 2016 vol. 4(Issue 29) pp:11351-11356
Publication Date(Web):22 Jun 2016
DOI:10.1039/C6TA04402F
Anatase TiO2 has low-cost and potentially high capacity as a Na-storage anode, but its low capacity utilization and poor rate capability remain a challenge for practical battery applications. To address this issue, we synthesized graphene-supported TiO2 nanospheres through a facile hydrothermal process, aiming at enhancing the electrochemical capacity and kinetics of this material. The porous TiO2 nanospheres offer abundant electrochemically active surface sites and ionic channels, enabling high utilization of the TiO2 nanoparticles, meanwhile the rGO matrices provide high electronic conduction and prevent the aggregation of the TiO2 nanoparticles during repeated cycles. The as-prepared rGO–TiO2 electrode demonstrates a high capacity of 300 mA h g−1 and a cycling stability with a capacity retention of 208 mA h g−1 over 300 cycles. Also, this rGO–TiO2 electrode exhibits a high rate capability of 123.1 mA h g−1 at a very high rate of 4.0 A g−1. The structural design and synthesis route described in this work may provide an effective approach to promote the electrochemical performance of Na-insertion materials for high-rate and high capacity Na-ion batteries.
Co-reporter:Xianyong Wu, Chenghao Wu, Congxiao Wei, Ling Hu, Jiangfeng Qian, Yuliang Cao, Xinping Ai, Jiulin Wang, and Hanxi Yang
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 8) pp:5393
Publication Date(Web):February 5, 2016
DOI:10.1021/acsami.5b12620
Prussian blue and its analogues have received particular attention as superior cathodes for Na-ion batteries due to their potential 2-Na storage capacity (∼170 mAh g–1) and low cost. However, most of the Prussian blue compounds obtained from the conventional synthetic routes contain large amounts of Fe(CN)6 vacancies and coordinated water molecules, which leads to the collapse of cyano-bridged framework and serious deterioration of their Na-storage ability. Herein, we propose a facile citrate-assisted controlled crystallization method to obtain low-defect Prussian blue lattice with greatly improved Na-storage capacity and cycling stability. As an example, the as-prepared Na2CoFe(CN)6 nanocrystals demonstrate a reversible 2-Na storage reaction with a high specific capacity of 150 mAh g–1 and a ∼ 90% capacity retention over 200 cycles, possibly serving as a low cost and high performance cathode for Na-ion batteries. In particular, the synthetic strategy described in this work may be extended to other coordination-framework materials for a wide range of energy conversion and storage applications.Keywords: controlled crystallization method; lattice defects; Prussian blue framework; sodium cobalt hexacyanoferrate; sodium-ion batteries
Co-reporter:Ya Xiong, Jiangfeng Qian, Yuliang Cao, Xinping Ai, and Hanxi Yang
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 26) pp:16684-16689
Publication Date(Web):June 17, 2016
DOI:10.1021/acsami.6b03757
Nanosized TiO2 is now actively developed as a low-cost and potentially high capacity anode material of Na-ion batteries, but its poor capacity utilization and insufficient cyclability remains an obstacle for battery applications. To overcome these drawbacks, we synthesized electrospun TiO2/C nanofibers, where anatase TiO2 nanocrystals with a diameter of ∼12 nm were densely embedded in the conductive carbon fibers, thus preventing them from aggregating and attacking by electrolyte. Due to its abundant active surfaces of well-dispersed TiO2 nanocrytals and high electronic conductivity of the carbon matrix, the TiO2/C anode shows a high redox capacity of ∼302.4 mA h g–1 and a high-rate capability of 164.9 mAh g–1 at a very high current of 2000 mA g–1. More significantly, this TiO2/C anode can be cycled with nearly 100% capacity retention over 1000 cycles, showing a sufficiently long cycle life for battery applications. The nanofibrous architecture of the TiO2/C composite and its superior electrochemical performance may provide new insights for development of better host materials for practical Na-ion batteries.
Co-reporter:Xianyong Wu, Miaomiao Shao, Chenghao Wu, Jiangfeng Qian, Yuliang Cao, Xinping Ai, and Hanxi Yang
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 36) pp:23706
Publication Date(Web):August 24, 2016
DOI:10.1021/acsami.6b06880
Low cost and high performance Li-ion batteries have been extensively pursued for grid-scale energy storage applications; however, their development has been impeded for a long time due to the lack of qualified cathode materials with not only decent electrochemical performance but also resource abundance and low price. In this paper, we report Prussian-blue type FeFe(CN)6 nanocrystals with well-controlled lattice defects and perfect nanocubic morphology, which can exhibit a high Li-storage capacity of 160 mAh g–1, a strong rate performance at 24 C, and a superior cycle stability with 90% capacity retention over 300 cycles. This low defect lattice and its excellent Li-insertion performance might provide a new insight into the design of advanced Li-ion battery materials and also a competitive alternative to the presently developed Li+ insertion cathodes to develop low cost and high performance Li-ion batteries for grid-scale energy storage applications.Keywords: cathode material; FeFe(CN)6 nanocrystal; lithium ion batteries; low-defect lattice; Prussian blue compounds
Co-reporter:Wenwen Deng, Yifei Shen, Jiangfeng Qian, Yuliang Cao, and Hanxi Yang
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 38) pp:21095
Publication Date(Web):September 11, 2015
DOI:10.1021/acsami.5b04325
Organic Na-host materials have are now actively pursued as an attractive alternative to conventional transition-metal compounds for development of sustainable sodium ion batteries; however, most of the organic compounds reported so far suffer from their low reversible capacity and poor cyclability. Here, we report a simple perylene diimide, 3,4,9,10-perylene-bis(dicarboximide) (PTCDI), which demonstrates remarkable electrochemical performances as an organic cathode for Na-ion batteries. With the high density of redox-active carbonyl groups in a stable π-conjugated structure, the PTCDI molecule can undergo a two-electron redox reaction with reversible insertion/extraction of 2 Na+ ions per molecular unit, demonstrating a high capacity of 140 mAh g–1, a strong rate performance with a reversible capacity of 103 mAh g–1 at 600 mA g–1 (5 C,1 C = 120 mA g–1) and a long-term cyclability with 90% capacity retention over 300 cycles. Because this PTCDI material is commercially available and nontoxic, it may serve as a new alternative cathode for Na-ion battery applications.Keywords: electrochemical enolization reaction; Na-host material; organic cathode; perylene diimide; sodium ion batteries
Co-reporter:Wenwen Deng, Yifei Shen, Jiangfeng Qian and Hanxi Yang
Chemical Communications 2015 vol. 51(Issue 24) pp:5097-5099
Publication Date(Web):17 Feb 2015
DOI:10.1039/C5CC00073D
A redox-active and water-insoluble polyimide, poly-(naphthalene four formyl ethylenediamine), demonstrates a high capacity of 130 mA h g−1, a strong rate capability at 10 C rate and an excellent capacity retention of 91.2% over 1000 cycles, offering a low cost and environmentally benign anode for aqueous Na-ion batteries.
Co-reporter:Xianyong Wu, Yang Luo, Mengying Sun, Jiangfeng Qian, Yuliang Cao, Xinping Ai, Hanxi Yang
Nano Energy 2015 Volume 13() pp:117-123
Publication Date(Web):April 2015
DOI:10.1016/j.nanoen.2015.02.006
•Low-defect Prussian blue nanocubes were synthesized in concentrated KCl solution.•The Prussian blue nanocubes demonstrate a high capacity, a strong rate capability and long cycle life.•The Prussian blue nanocubes offer an competitive cathode for aqueous Na-ion batteries.Prussian blue compounds have potential advantages of high working potentials and multi-electron redox capacities as Na-ion battery cathodes; however, they suffer from their poor capacity utilization in aqueous electrolytes due to the blockage of the active lattice sites by coordinating and zeolitic water for Na insertion reaction. To overcome this problem, we synthesized low-defect Prussian blue FeFe(CN)6 nanocrystals and revealed their Na-storage performance in aqueous electrolytes. Benefitting from its suppressed lattice defects and well-defined nanocubic morphology, the as-prepared Prussian blue nanocrystals exhibit a greatly improved capacity of ~125 mAh g−1, a strong rate capability with 102 mAh g−1 at a high rate of 20C and a remarkably long cycle life with 83% capacity retention over 500 cycles, exceeding considerably the aqueous Na-storage cathodes reported so far and capably serving as a high performance cathode for aqueous Na-ion batteries. As a model compound, the superior electrochemical performance arising from the low-defect Prussian blue nanocrystals provide a new insight into the design of high capacity Na-storage host materials for large scale electric storage applications.Prussian blue nanocrystals with suppressed lattice vacancies demonstrate a reversible 1.6 Na storage capacity of 125 mAh g−1, a strong rate capability at 20C, and an excellent long-term cyclability with 83% capacity retention over 500 cycles, capably serving as a low-cost, environmentally benign cathode for aqueous Na-ion batteries .
Co-reporter:Dingding Yuan;Xinmiao Liang;Lin Wu;Yuliang Cao;Xinping Ai;Jiwen Feng;Hanxi Yang
Advanced Materials 2014 Volume 26( Issue 36) pp:6301-6306
Publication Date(Web):
DOI:10.1002/adma.201401946
Co-reporter:Jiangfeng Qian, Ya Xiong, Yuliang Cao, Xinping Ai, and Hanxi Yang
Nano Letters 2014 Volume 14(Issue 4) pp:1865-1869
Publication Date(Web):March 10, 2014
DOI:10.1021/nl404637q
Room-temperature Na-ion batteries have attracted great interest as a low cost and environmentally benign technology for large scale electric energy storage, however their development is hindered by the lack of suitable anodic host materials. In this paper, we described a green approach for the synthesis of Sn4P3/C nanocomposite and demonstrated its excellent Na-storage performance as a novel anode of Na-ion batteries. This Sn4P3/C anode can deliver a very high reversible capacity of 850 mA h g–1 with a remarkable rate capability with 50% capacity output at 500 mA g–1 and can also be cycled with 86% capacity retention over 150 cycles due to a synergistic Na-storage mechanism in the Sn4P3 anode, where the Sn nanoparticles act as electronic channels to enable electrochemical activation of the P component, while the elemental P and its sodiated product Na3P serve as a host matrix to alleviate the aggregation of the Sn particles during Na insertion reaction. This mechanism may offer a new approach to create high capacity and cycle-stable alloy anodes for Na-ion batteries and other electrochemical energy storage applications.
Co-reporter:W.W. Deng, Y.F. Shen, X.M. Liang, J.W. Feng, H.X. Yang
Electrochimica Acta 2014 Volume 147() pp:426-431
Publication Date(Web):20 November 2014
DOI:10.1016/j.electacta.2014.09.103
•A cycle-stable perylene-3,4,9,10-tetracarboxydiimide/polypyrrole composite (PTCDI/PPy) is synthesized by physical doping method.•The PTCDI/PPy composite demonstrates a synergistic electrochemical activation with greatly enhanced capacity and cyclability.•The physical doping method is extendable for a variety of organic molecules and polymers.A high capacity and cycle-stable organic molecule/polymer composite is synthesized by physical doping of redox-active perylene-3,4,9,10-tetracarboxydiimide (PTCDI) in polypyrrole (PPy). The as-prepared PTCDI/PPy composite demonstrates a synergistic electrochemical activation, in which the insoluble large PTCDI anions act as a redox-active dopant to activate the PPy backbones, while the activated PPy backbones form a conductive network to promote the redox activity of PTCDI molecules for Li insertion/extraction reactions. As a result, the PTCDI/PPy composite demonstrated a considerably high reversible capacity of >100 mAh g−1 and a stable cyclability with 92% capacity retention over 200 cycles, possibly serving as a low cost and renewable alternative to the inorganic cathode materials for Li-ion batteries. Since such a physical doping method is simple and easily adoptable for different organic molecules and polymers, it may offer a new route for developing low cost and electrochemically active organic electrode materials.
Co-reporter:Xian-yong Wu;Meng-ying Sun;Yi-fei Shen;Dr. Jiang-feng Qian;Dr. Yu-liang Cao;Dr. Xin-ping Ai ; Han-xi Yang
ChemSusChem 2014 Volume 7( Issue 2) pp:407-411
Publication Date(Web):
DOI:10.1002/cssc.201301036
Abstract
Aqueous rechargeable sodium-ion batteries have the potential to meet growing demand for grid-scale electric energy storage because of the widespread availability and low cost of sodium resources. In this study, we synthesized a Na-rich copper hexacyanoferrate(II) Na2CuFe(CN)6 as a high potential cathode and used NaTi2(PO4)3 as a Na-deficient anode to assemble an aqueous sodium ion battery. This battery works very well with a high average discharge voltage of 1.4 V, a specific energy of 48 Wh kg−1, and an excellent high-rate cycle stability with approximately 90 % capacity retention over 1000 cycles, achieving a new record in the electrochemical performance of aqueous Na-ion batteries. Moreover, all the anode, cathode, and electrolyte materials are low cost and naturally abundant and are affordable for widespread applications.
Co-reporter:Xianyong Wu, Wenwen Deng, Jiangfeng Qian, Yuliang Cao, Xinping Ai and Hanxi Yang
Journal of Materials Chemistry A 2013 vol. 1(Issue 35) pp:10130-10134
Publication Date(Web):21 Jun 2013
DOI:10.1039/C3TA12036H
Prussian blue analogues are actively explored as low cost and high capacity cathodes for Na ion batteries; however, their applications are hindered by low capacity utilization and poor cyclability of these compounds. Here we show that this problem can be solved by controlling the purity and crystallinity of the Prussian blue lattices. As a model compound, single-crystal FeIIIFeIII(CN)6 nanoparticles are synthesized and found to have a sufficiently high capacity of 120 mA h g−1, an exceptional rate capability at 20 C and superior cyclability with 87% capacity retention over 500 cycles, showing great promise for Na ion battery applications. More significantly, these results provide a new insight into the intercalation chemistry of Prussian blue analogues and open new perspectives to develop Na storage cathodes for widespread applications of electric energy storage.
Co-reporter:Lin Wu, Xiaohong Hu, Jiangfeng Qian, Feng Pei, Fayuan Wu, Rongjun Mao, Xinping Ai, Hanxi Yang and Yuliang Cao
Journal of Materials Chemistry A 2013 vol. 1(Issue 24) pp:7181-7184
Publication Date(Web):18 Apr 2013
DOI:10.1039/C3TA10920H
A Sn–SnS–C nanocomposite is prepared by simply mechanically ball-milling Sn, SnS and C powders. In this composite, Sn nanocrystals are surface-coated with SnS nanoparticles and uniformly dispersed in the carbon matrix. During discharge, the SnS particles undergo an electrochemical conversion reaction to generate Sn and Na2S nanocrystals and then the Sn particles alloy with Na to produce the NaSn alloy. The conversion reaction of SnS and the alloying reaction of Sn with Na are completely reversible, producing a very high reversible Na-storage capacity of >600 mA h g−1 at an appropriate low potential of ∼0.7 V. Since the SnS phase provides an effective buffering matrix to alleviate the volumetric change of the Sn particles during Na insertion and extraction, and also serves as a separator to prevent the aggregation of the Sn nanoparticles, the Sn–SnS–C composite anode demonstrates a very good cycling stability with 87% capacity retention over 150 cycles, possibly usable for Na-ion batteries.
Co-reporter:Dingding Yuan, Wei He, Feng Pei, Fayuan Wu, Yue Wu, Jiangfeng Qian, Yuliang Cao, Xinping Ai and Hanxi Yang
Journal of Materials Chemistry A 2013 vol. 1(Issue 12) pp:3895-3899
Publication Date(Web):17 Jan 2013
DOI:10.1039/C3TA01430D
Stable Na+ ion storage cathodes with adequate reversible capacity are now greatly needed for enabling Na-ion battery technology for large scale and low cost electric storage applications. In light of the superior Li+ ion storage performance of layered oxides, pure P2-phase Na0.67[Mn0.65Ni0.15Co0.2]O2 microflakes are synthesized by a simple sol–gel method and tested as a Na+ ion storage cathode. These layered microflakes exhibit a considerably high reversible capacity of 141 mA h g−1 and a slow capacity decay to 125 mA h g−1 after 50 cycles, showing much better cyclability than previous NaMnO2 compounds. To further enhance the structural and cycling stability, we partially substituted Co3+ by Al3+ ions in the transition-metal layer to synthesize Na0.67[Mn0.65Ni0.15Co0.15Al0.05]O2. As expected, the Al-substituted material demonstrates a greatly improved cycling stability with a 95.4% capacity retention over 50 cycles, possibly serving as a high capacity and stable cathode for Na-ion battery applications.
Co-reporter:Zhongxue Chen, Shen Qiu, Yuliang Cao, Jiangfeng Qian, Xinping Ai, Kai Xie, Xiaobin Hong and Hanxi Yang
Journal of Materials Chemistry A 2013 vol. 1(Issue 16) pp:4988-4992
Publication Date(Web):12 Feb 2013
DOI:10.1039/C3TA00611E
A hierarchical porous Li2FeSiO4/C composite was prepared using an in situ template synthesis by tetraconstituent co-assembly of resols, nitrates, silica oligomers, and a triblock copolymer surfactant. The structural and electrochemical characterizations revealed that the Li2FeSiO4/C composite has a hierarchical micro-, meso- and macro-porous structure, in which macrosized pores provide abundant electrolyte channels for fast ionic transport, while the microporous network offers large accessible electrochemically active areas for the Li insertion reaction. The Li2FeSiO4/C composite demonstrates a very high capacity of 254 mA h g−1 at room temperature with excellent cycling stability and rate capability, corresponding to 77.5% utilization of its theoretical 2 Li storage capacity. The results from this study suggest a feasible approach to improve dramatically the electrochemical utilization and cyclability of the kinetically sluggish intercalation compounds by creating an electrochemically favorable porous structure and the synthetic strategy described in this work may be extended to fabricate other types of porous multifunctional materials for energy storage, catalysis and other applications.
Co-reporter:Limin Zhu, Yifei Shen, Mengying Sun, Jiangfeng Qian, Yuliang Cao, Xinping Ai and Hanxi Yang
Chemical Communications 2013 vol. 49(Issue 97) pp:11370-11372
Publication Date(Web):16 Oct 2013
DOI:10.1039/C3CC46642F
A Na-host cathode is developed by grafting the polypyrrole chains with ionizable sodium sulfonate. Due to the immobile p-doping of organic anions, the self-doped polymer can act as a Na-host for reversible Na insertion–extraction reaction, thus offering a low cost and renewable organic cathode for Na ion battery applications.
Co-reporter:L. M. Zhu, A. W. Lei, Y. L. Cao, X. P. Ai and H. X. Yang
Chemical Communications 2013 vol. 49(Issue 6) pp:567-569
Publication Date(Web):23 Nov 2012
DOI:10.1039/C2CC36622C
An all-organic rechargeable battery is realized by use of polyparaphenylene as both cathode- and anode-active material. This new battery can operate at a high voltage of 3.0 V with fairly high capacity, offering a renewable and cheaper alternative to conventional batteries.
Co-reporter:Xianyong Wu, Yuliang Cao, Xinping Ai, Jiangfeng Qian, Hanxi Yang
Electrochemistry Communications 2013 Volume 31() pp:145-148
Publication Date(Web):June 2013
DOI:10.1016/j.elecom.2013.03.013
•An aqueous rechargable Na-ion battery is developed.•Na2NiFe(CN)6 and NaTi2(PO4)3 serve as cathode and anode, respectively.•A Na2SO4 aqueous solution serves as the electrolyte.•An output of ∼1.27 V and 42.5 Wh kg− 1 is achieved.•This battery is safe, low cost and environmentally friendly.An aqueous rechargable Na-ion battery is developed by use of Na-deficient NaTi2(PO4)3 anode, Na-rich Na2NiFe(CN)6 cathode and aqueous Na2SO4 electrolyte. This battery system can give an average output voltage of 1.27 V, a energy density of 42.5 Wh kg− 1 and can retain 88% of initial capacity for 250 cycles cycled at the 5 C rate. Moreover, this aqueous Na-ion battery has the advantages of low cost, environmentally friendliness and inherent safety, particularly attractive for grid-scale energy storage applications.
Co-reporter:Lin Wu, Feng Pei, Rongjun Mao, Fayuan Wu, Yue Wu, Jiangfeng Qian, Yuliang Cao, Xinping Ai, Hanxi Yang
Electrochimica Acta 2013 Volume 87() pp:41-45
Publication Date(Web):1 January 2013
DOI:10.1016/j.electacta.2012.08.103
SiC–Sb–C nanocomposites with core–shell structure were prepared by simple mechanical ball-milling method. This core–shell structure is composed of rigid SiC nanoparticles as inner core, Sb nanoparticles as an electrochemical active layer anchored on the surface of SiC, and carbon outlayer. The electrochemical experiments show that the SiC–Sb–C electrode improve electrochemical utilization and cycling stability of Sb during Na-storage reaction in comparison with Sb–C composites, indicating that such core–shell structure can effectively buffer the volume change and remain structural stability. Particularly, after incorporating Cu into Sb layer, the SiC–Sb–Cu–C electrode exhibits higher capacity and cycling stability (595 mAh g−1 after 100 cycles) than the SiC–Sb–C electrode. Therefore, the core–shell structure can provide a viable strategy to develop high capacity and stable cycling alloy anode for sodium ion batteries.Highlights► SiC–Sb–C nanocomposites with core–shell structure were prepared by simple mechanical ball-milling method as anode materials for Na-ion batteries. ► Such core–shell structure of the SiC–Sb–C electrode can effectively buffer the volume change and remain structural stability. ► After adding Cu, the SiC–Sb–Cu–C electrode exhibits higher capacity of 511 mAh g−1 at 800 mA g−1 and 595 mAh g−1 after 100 cycles.
Co-reporter:L.M. Zhu, W. Shi, R.R. Zhao, Y.L. Cao, X.P. Ai, A.W. Lei, H.X. Yang
Journal of Electroanalytical Chemistry 2013 Volume 688() pp:118-122
Publication Date(Web):1 January 2013
DOI:10.1016/j.jelechem.2012.06.019
All-organic rechargeable batteries may have low cost, materials sustainability and environmental friendliness, particularly suitable for large scale electric energy storage applications. However, development of such a new generation of batteries is now hindered by the lack of appropriate organic anode materials. In this paper, we report a novel polythiophene/carbon composite, where n-dopable poly (3,4-dihexylthiophene) is in situ chemically polymerized on carbon nanofibers. This organic-carbon composite exhibits an exceptionally high reversible electrochemical capacity of ∼300 mAh g−1 (or ∼ 200 Ah L−1) through n-type redox reactions and superior capacity retention of ⩾95% after a hundred cycles. Based on this n-type redox-active material, an all-organic Li-ion cell using polytriphenylamine as cathode-active material was constructed and found to operate successfully, demonstrating possible applications of this composite as a high capacity anode material for all-organic storage batteries.Graphical abstractn-Type redox-active poly (3,4-dihexylthiophene) was synthesized by oxidative coupling polymerization and found to exhibit exceptionally high reversible electric storage capacity of −300 mAh g−1 through Lithium insertion/extraction reactions, possibly serving as a high capacity anodic material for all organic Li-ion batteries.Highlights► n-Type redox-active polythiophene/carbon composite was synthesized via an oxidative coupling polymerization. ► The polythiophene/carbon composite demonstrates a superior high capacity and reversibility as an organic anodic material. ► The polythiophene/carbon composite was successfully used for constructing all-organic Li-ion batteries.
Co-reporter:R.R. Zhao, Y.L. Cao, X.P. Ai, H.X. Yang
Journal of Electroanalytical Chemistry 2013 Volume 688() pp:93-97
Publication Date(Web):1 January 2013
DOI:10.1016/j.jelechem.2012.07.019
Rechargeable batteries using organic materials have potential advantages of low cost and materials sustainability for large-scale electric storage applications. The key issue to realize such sustainable batteries is to develop suitable organic electrode materials with sufficient redox capacity and cycling stability. Herein, we introduce lithium and sodium salt of 3, 4, 9,10-perylenetetracarboxylic acid (Li4C24H8O8, Na4C24H8O8) as new organic anode materials for Li-ion and Na-ion batteries. The Li4C24H8O8 electrode can deliver a reversible capacity of ∼200 mAh g−1 at quite low charge/discharge plateaus of 1.20/1.10 V, and remains 98% of its initial capacity after 100 cycles. Similarly, the Na4C24H8O8 electrode exhibits a reversible Na storage capacity of ∼100 mAh g−1 at a low voltage region of 0.8–0.6 V (vs Na) with almost indiscernible capacity decay during 100 cycles. These results demonstrate a potential possibility to use the organic anodes for Li-ion and Na-ion batteries.Highlights► Li4C24H8O8 and Na4C24H8O8 are introduced as organic anodic materials for Li- and Na-ion batteries. ► The Li4C24H8O8 anode demonstrates a high Li-storage capacity and cycling stability. ► The Na4C24H8O8 anode delivers a sufficient Na-storage capacity with superior cycling performance for Na-ion batteries.
Co-reporter:Dr. Jiangfeng Qian;Dr. Xianyong Wu;Dr. Yuliang Cao; Xinping Ai ; Hanxi Yang
Angewandte Chemie 2013 Volume 125( Issue 17) pp:4731-4734
Publication Date(Web):
DOI:10.1002/ange.201209689
Co-reporter:Dr. Jiangfeng Qian;Dr. Xianyong Wu;Dr. Yuliang Cao; Xinping Ai ; Hanxi Yang
Angewandte Chemie International Edition 2013 Volume 52( Issue 17) pp:4633-4636
Publication Date(Web):
DOI:10.1002/anie.201209689
Co-reporter:Min Zhou;Ya Xiong;Yuliang Cao;Xinping Ai ;Hanxi Yang
Journal of Polymer Science Part B: Polymer Physics 2013 Volume 51( Issue 2) pp:114-118
Publication Date(Web):
DOI:10.1002/polb.23184
Abstract
We demonstrate here a remarkable electrochemical activation of polypyrrole chains by doping with redox-active diphenylamine sulfonate anions. The organic redox dopant can not only serve as anionic counterions to enhance electrochemical activity of the polymer chains, but also contributes their redox capacity to the material. This organic-polymer composite exhibits a quite high reversible capacity of 115 mA h g−1, excellent rate capability and cycling stability, capable of serving as a low cost, and renewable cathode for Na-ion batteries. Since the chemical doping method is simple and easily extendable for a large variety of organic anions and polymer networks, it is possible to adopt this new strategy for creating low cost and electrochemically active polymer materials for widespread electric storage applications. © 2012 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2013
Co-reporter:Ping Liu;Yu-liang Cao;Guo-Ran Li;Xue-Ping Gao;Xin-Ping Ai; Han-Xi Yang
ChemSusChem 2013 Volume 6( Issue 5) pp:802-806
Publication Date(Web):
DOI:10.1002/cssc.201200962
Co-reporter:Jianfeng Qian;Min Zhou;Yuliang Cao;Xinping Ai ;Hanxi Yang
Advanced Energy Materials 2012 Volume 2( Issue 4) pp:410-414
Publication Date(Web):
DOI:10.1002/aenm.201100655
Co-reporter:Zhongxue Chen, Shen Qiu, Yuliang Cao, Xinping Ai, Kai Xie, Xiaobin Hong and Hanxi Yang
Journal of Materials Chemistry A 2012 vol. 22(Issue 34) pp:17768-17772
Publication Date(Web):06 Jul 2012
DOI:10.1039/C2JM33338D
Spinel LiNi0.5Mn1.5O4 has attracted extensive interest as an appealing cathode material of next generation lithium-ion batteries to meet the cost/performance requirements for electric vehicle applications and renewable electric energy storage. In this paper, we report, for the first time, a nanoflake-stacked LiNi0.5Mn1.5O4 spinel with oriented growth of the (001) planes synthesized via an in situ template route. The resultant LiNi0.5Mn1.5O4 cathode delivers an initial discharge capacity of 133.5 mA h g−1 at 1 C with capacity retention of 86% after 500 cycles. X-ray diffraction and transmission electron microscopy results suggest that the growth of (111) facets on the surfaces of the nanoflake-stacked LiNi0.5Mn1.5O4 spinel is significantly restricted, which helps to inhibit the dissolution of manganese from the lattice and ensure an excellent cycling stability. Moreover, the very thin nanoflakes and large interspaces between the nanoflakes are favorable for Li ion transportation, leading to a fast kinetics of the LiNi0.5Mn1.5O4 spinel. As a result, the material demonstrates a reversible capacity of 96 mA h g−1 even at 50 C rate, showing a feasible application for high-power lithium ion batteries. In particular, this study provides a synthetic strategy to fabricate insertion materials with a surface-oriented morphology and nanoflake-stacked structure for energy storage, fast-ion conductors and other applications.
Co-reporter:Jiangfeng Qian, Yao Chen, Lin Wu, Yuliang Cao, Xinping Ai and Hanxi Yang
Chemical Communications 2012 vol. 48(Issue 56) pp:7070-7072
Publication Date(Web):29 May 2012
DOI:10.1039/C2CC32730A
A Sb/C nanocomposite was synthesized and found to deliver a reversible 3 Na storage capacity of 610 mA h g−1, a strong rate capability at a very high current of 2000 mA g−1 and a long-term cycling stability with 94% capacity retention over 100 cycles, offering practical feasibility as a high capacity and cycling-stable anode for room temperature Na-ion batteries.
Co-reporter:Jiangfeng Qian, Dan Qiao, Xinping Ai, Yuliang Cao and Hanxi Yang
Chemical Communications 2012 vol. 48(Issue 71) pp:8931-8933
Publication Date(Web):17 Jul 2012
DOI:10.1039/C2CC34388F
An amorphous phosphorus/carbon nanocomposite demonstrates a reversible 3-Li storage capacity of 2355 mAh g−1 with an excellent capacity retention of 90% over 100 cycles and a superior power capability with 62% of its capacity realizable at a very high rate of 8000 mA g−1, possibly serving as a high capacity and high rate alternative anode for next-generation Li-ion batteries.
Co-reporter:Ting Li, Zhong X. Chen, Xin P. Ai, Yu L. Cao, Han X. Yang
Journal of Power Sources 2012 Volume 217() pp:54-58
Publication Date(Web):1 November 2012
DOI:10.1016/j.jpowsour.2012.05.111
Lithium-rich LiF/Fe nanocomposite is prepared by a simple route of mechanical ball-milling of lithium fluoride and iron using rigid TiN nanoparticles as the grinding powders, and studied as a lithium-rich cathode material for satisfying the present Li-ion battery technology. The structural characterizations reveal that the nanocomposite is composed of well-dispersed and intimately contacted LiF and Fe particles created by high-energy ball-milling, forming appropriate electrode-active nanodomains for the reversible conversion reaction of LiF and Fe. Electrochemical measurements demonstrate that the LiF/Fe nanocomposite containing 50 wt% active materials of LiF and Fe can deliver a high reversible capacity of 568 mAh g−1 at 20 mA g−1 (calculated using the weight of LiF and Fe only), approaching the theoretical capacity of the composite (600 mAh g−1), and also show a strong power capability with a reversible capacity of ∼300 mAh g−1 even at a very high rate of 500 mA g−1 at room temperature. CV and XRD analyses confirm that the LiF/Fe nanocomposite can nearly realize a three-electron transfer through electrochemical conversion of LiF/Fe to FeF3 and vice versa. These results suggest the possibility to utilize the inexpensive lithium-rich composites of lithium fluoride and metals as high-capacity cathode materials for future-generation Li-ion batteries through the electrochemical conversion.Highlights► The composite was prepared by a simple ball-milling of LiF and Fe powders. ► The composite delivers 568 mAh g−1 at 20 mA g−1 and exhibits a high rate capability. ► The composite can realize the conversion reaction of LiF/Fe to FeF3 and vice versa.
Co-reporter:Ruirui Zhao, Limin Zhu, Yuliang Cao, Xinping Ai, Han X. Yang
Electrochemistry Communications 2012 Volume 21() pp:36-38
Publication Date(Web):July 2012
DOI:10.1016/j.elecom.2012.05.015
An aniline/o-nitroaniline copolymer was prepared simply by grafting electron-withdrawing o-nitroaniline groups onto polyaniline chains through a chemical oxidative polymerization and tested as a high voltage cathode material for Na-ion batteries. The experimental results demonstrated that the as-prepared P(AN-NA) can deliver a reversible capacity of 180 mAh g− 1 at an average potential of ~ 3.2 V ( vs. Na+/Na ) and remain 173 mAh g− 1 after 50 cycles, showing a high potential capability and a strong capacity retention. In addition, the copolymer is low cost and easy to make, possibly serving as a cycling-stable and high capacity cathode for practical Na-ion battery applications.Graphical abstractAn aniline/o-nitroaniline copolymer was prepared simply by through a chemical oxidative polymerization and found to have a reversible redox capacity of 180 mAh g− 1 at an average potential of ~ 3.2 V and a strong capacity retention of retention of 95% over 50 cycles, capable to serve as a cycling-stable and high capacity cathode for Na-ion battery applications.Highlights► An aniline/o-nitroaniline copolymer was synthesized through a chemical oxidative polymerization. ► The P(An-NA) copolymer demonstrates a superior high redox capacity and strong capacity retention. ► The P(An-NA) copolymer can serve as a cycling-stable and high capacity cathode for Na-ion batteries.
Co-reporter:P. Liu, H.X. Yang, X.P. Ai, G.R. Li, X.P. Gao
Electrochemistry Communications 2012 Volume 16(Issue 1) pp:69-72
Publication Date(Web):March 2012
DOI:10.1016/j.elecom.2011.11.035
A solar rechargeable battery is constructed by use of a hybrid TiO2/poly(3,4-ethylenedioxythiophene, PEDOT) photo-anode and a ClO4− doped polypyrrole counter electrode. Here, the dye-sensitized TiO2/PEDOT photo-anode serves for positive charge storage and a p-doped PPy counter electrode acts for electron storage in LiClO4 electrolyte. The proposed device demonstrates a rapid photo-charge at light illumination and a stable electrochemical discharge in the dark, realizing an in situ solar-to-electric conversion and storage.Highlights► A solar rechargeable battery (SRB) is developed based on hole and electron storage. ► The SRB demonstrates an effective solar-to-electric conversion and storage. ► The photo-charge/discharge reactions proceed via reversible doping/de-doping of ClO4−.
Co-reporter:Limin Zhu, Yijie Niu, Yuliang Cao, Aiwen Lei, Xinping Ai, Hanxi Yang
Electrochimica Acta 2012 Volume 78() pp:27-31
Publication Date(Web):1 September 2012
DOI:10.1016/j.electacta.2012.05.152
A polybithiophene-carbon (PBT/C) composite was synthesized by ball-milling chemically polymerized polybithiophene with carbon nanofibers and found to have n-type redox properties with exceptional reversible capacity and cycling stability. The experimental results demonstrated that the as-synthesized (PBT/C) composite can realize a total two-electron redox capacity of ∼850 mAh g−1 with half of the capacity delivered at a low potential plateau of 1.25 V in Li+ electrolyte, possibly serving as a high capacity organic anode for Li-ion batteries. More significantly, the PBT/C composite can also be cycled in Na+-electrolyte, delivering a reversible redox capacity of ∼500 mAh g−1 through the doping–dedoping reactions of Na+ ions into/from the polymer chains. These n-type redox performances suggest a possible application of the polymers of this type as high capacity and cycling-stable anodes for Li-ion and Na-ion batteries.
Co-reporter:Min Zhou, Limin Zhu, Yuliang Cao, Ruirui Zhao, Jianfeng Qian, Xinping Ai and Hanxi Yang
RSC Advances 2012 vol. 2(Issue 13) pp:5495-5498
Publication Date(Web):18 Apr 2012
DOI:10.1039/C2RA20666H
A redox-active Fe(CN)6−4-doped polypyrrole was synthesized and found to have a remarkable redox capacity of 135 mA h g−1 in Na+ electrolyte, an excellent rate capability of 1600 mA g−1 and a strong capacity retention of 85% over 100 cycles, showing great promise for enabling low-cost and environmentally benign Na-ion batteries for large-scale electric energy storage.
Co-reporter:Wei He, Jiangfeng Qian, Yuliang Cao, Xinping Ai and Hanxi Yang
RSC Advances 2012 vol. 2(Issue 8) pp:3423-3429
Publication Date(Web):26 Jan 2012
DOI:10.1039/C2RA20122D
Layered Li[Li0.2Co0.13Ni0.13Mn0.54]O2 nanoparticles were synthesized by a simple polymer-pyrolysis method and then coated with 3 wt% Al2O3 to form a ∼4 nm thick protective skin. The Al2O3-coated Li[Li0.2Co0.13Ni0.13Mn0.54]O2 electrode demonstrates a high initial coulombic efficiency of 96.1%, a large reversible capacity of ∼311 mAh g−1, and a good cyclability with 83.8% capacity retention after 70 cycles. Particularly, this material can deliver a quite high capacity of ∼239 mAh g−1 at a high rate of 400 mA g−1. This superior electrochemical performance results from the well-crystallized nanocores and effective surface modification of the material. The former provides a short diffusion path and fast transport channels for lithium ion insertion/extraction reactions and the latter restrains the elimination of oxide ion vacancies and metal ion rearrangement during charge–discharge cycling. Due to their simplicity and applicability, the synthetic method along with the surface modification technique is easily adopted to make high performance xLi2MnO3·(1 − x)LiMO2 materials for practical battery applications.
Co-reporter:Min Zhou;JiangFeng Qian;YuLiang Cao;HanXi Yang
Science Bulletin 2012 Volume 57( Issue 32) pp:4164-4169
Publication Date(Web):2012 November
DOI:10.1007/s11434-012-5068-4
Mesoporous LiFePO4 microspheres were simply synthesized by a low temperature (130°C), template-free hydrothermal route using low cost LiOH, Fe(NO3)3 and NH4H2PO4 as starting raw materials. These microspheres are composed of densely aggregated LiFePO4 nanoparticles and filled with interconnected mesochannels, which demonstrates not only a high tap density (⩾1.4 g cm−3), a high capacity of 150 mAh g-1 (∼90% of its theoretical capacity) at 0.5 C rate, but also a ⩾ 80% utilization of its theoretical capacity at a high rate of 1 C. In addition, the hydrothermal synthesis developed in this work is simple and cost-effective, it may provide a new route for production of the LiFePO4 material in battery applications.
Co-reporter:Min Zhou;Jianfeng Qian;Xinping Ai ;Hanxi Yang
Advanced Materials 2011 Volume 23( Issue 42) pp:4913-4917
Publication Date(Web):
DOI:10.1002/adma.201102867
Co-reporter:Ting Li ; Xin P. Ai ;Han X. Yang
The Journal of Physical Chemistry C 2011 Volume 115(Issue 13) pp:6167-6174
Publication Date(Web):March 11, 2011
DOI:10.1021/jp112399r
Novel Li2O/CuO nanocomposites were prepared by ball-milling the CuO and Li2O nanoparticles with rigid TiN nanopowders, where TiN nanopowders act as a conductive substrate to immobilize the electroactive nanolayer of a biphasic Li2O/CuO mixture. The as-prepared samples demonstrate a superior electrochemical capacity of 560 mAh g−1 at a moderate charge−discharge rate of 50 mA g−1 and also exhibit a quite high reversible capacity of ∼438 mAh g−1 even at a very high rate of 500 mA g−1 at room temperature. CV and XRD analyses revealed that the Li2O/CuO nanocomposite can realize nearly a three-electron transfer through electrochemical conversion of Cu2O/Cu to LiCuO2 and vice versa, involving lithium intercalation and deintercalation. This conversion reaction can proceed reversibly and rapidly as long as the different phases of the cathode-active particles are well-dispersed and closely contacted to create electrochemically favorable nanodomains in the electrode. The experimental results demonstrated in this study suggest the possibility to use inexpensive multivalent metal oxides as high-capacity cathode materials for construction of future-generation lithium-ion batteries through an electrochemical conversion mechanism.
Co-reporter:Xue-Ping Gao and Han-Xi Yang
Energy & Environmental Science 2010 vol. 3(Issue 2) pp:174-189
Publication Date(Web):29 Oct 2009
DOI:10.1039/B916098A
The need for high energy density batteries becomes increasingly important for the development of new and clean energy technologies, such as electric vehicles and electrical storage from wind and solar power. The search for new energetic materials of primary and secondary batteries with higher energy density has been highlighted in recent years. This review surveys recent advances in the research field of high energy density electrode materials with focus on multi-electron reaction chemistry of light-weight elements and compounds. In the first section, we briefly introduce the basic strategies for enhancement of the energy density of primary batteries based on multi-electron reactions. The following sections present overviews of typical electrode materials with multi-electron chemistry and their secondary battery applications in aqueous and non-aqueous electrolytes. Finally, the challenges and ongoing research strategies of these novel electrode materials and battery systems for high density energy storage and conversion are discussed.
Co-reporter:Zhongxue Chen, Yuliang Cao, Jiangfeng Qian, Xinping Ai and Hanxi Yang
Journal of Materials Chemistry A 2010 vol. 20(Issue 34) pp:7266-7271
Publication Date(Web):27 Jul 2010
DOI:10.1039/C0JM00829J
A simple synthetic route was developed to obtain Sn-sandwiched composite nanoparticles by mechanical ball-milling ductile Sn particles with rigid SiC nanocores to form a SiC@Sn core-shell nanocomposite and then carbon-coating the SiC@Sn nanoparticles with graphite to produce the SiC@Sn@C nanoparticles. Such a novel nanostructure can effectively buffer the mechanical stress and prevent the aggregation of the Sn nanolayer and therefore improve the electrochemical utilization and cycling stability of electroactive Sn during Li-storage reaction. The Sn-sandwiched nanoparticles as-prepared exhibited a considerable high Li-storage capacity of ∼600 mA h g−1 and an excellent cycling stability with ∼90% capacity retention at 100 cycles, showing a prospect for practical lithium battery applications. In particular, the reported synthetic method is very simple, low-cost and pollution-free, enabling it to be readily adopted for large-scale production and also to be extended for other attractive lithium storage metals and alloys.
Co-reporter:Y. Jiang, Y.L. Cao, P. Liu, J.F. Qian, H.X. Yang
Electrochimica Acta 2010 Volume 55(Issue 22) pp:6415-6419
Publication Date(Web):1 September 2010
DOI:10.1016/j.electacta.2010.06.046
Three types of alkyl-substituted poly(N-alkyl-1-vinyl-imidazolium) iodides were synthesized and plasticized using succinonitrile as a solid plasticizer to develop a series of novel solvent-free plastic–polymer composite electrolytes. All these electrolytes appeared as a soft solid at room temperature and became sticky gel state at high temperature of 100 °C. Among the as-prepared plastic–polymer electrolytes, the SCN–PMVII (succinonitrile–poly(1-vinyl-3-methylimidazolium) iodide) electrolytes with a SCN content of 40–60 wt.% showed a room temperature conductivity of 1.0–1.6 mS cm−1and a photoconversion efficiency of >4.1%, which are comparable to those observed from liquid organic carbonate electrolyte and the DSSCs using the liquid electrolyte at the same experimental conditions. Also, the DSSCs assembled with the SCN–PMVII electrolytes maintained their photoconversion efficiency very steadily during aging test of 50 days despite of being placed at 40 °C under 1 sun illumination or stored at 60 °C in an oven. Since these plastic–polymer electrolytes are solvent-free, highly conductive and electrochemically compatible, it is possible to use this type electrolyte for development of practical DSSCs.
Co-reporter:Ting Li, Lei Li, Yu L. Cao, Xin P. Ai and Han X. Yang
The Journal of Physical Chemistry C 2010 Volume 114(Issue 7) pp:3190-3195
Publication Date(Web):January 28, 2010
DOI:10.1021/jp908741d
Three types of FeF3 nanocrystals were synthesized by different chemical routes and investigated as a cathode-active material for rechargeable lithium batteries. XRD and TEM analyses revealed that the as-synthesized FeF3 samples have a pure ReO3-type structure with a uniformly distributed crystallite size of ∼10 to 20 nm. Charge−discharge experiments in combination with cyclic voltammetric and XRD evidence demonstrated that the FeF3 in the nanocomposite electrode can realize a reversible electrochemical conversion reaction from Fe3+ to Fe0 and vice versa, enabling a complete utilization of its three-electron redox capacity (∼712 mAh·g−1). Particularly, the FeF3/C nanocomposites can be well cycled at very high rates of 1000−2000 mA·g−1, giving a considerably high capacity of ∼500 mAh·g−1. These results seem to indicate that the electrochemical conversion reaction can not only give a high capacity but also proceed reversibly and rapidly at room temperature as long as the electroactive FeF3 particles are sufficiently downsized, electrically wired, and well-protected from aggregation. The high-rate capability of the FeF3/C nanocomposite also suggests its potential applications for high-capacity rechargeable lithium batteries.
Co-reporter:Zhongxue Chen, Yuliang Cao, Jiangfeng Qian, Xinping Ai and Hanxi Yang
The Journal of Physical Chemistry C 2010 Volume 114(Issue 35) pp:15196-15201
Publication Date(Web):August 12, 2010
DOI:10.1021/jp104099r
A simple synthetic route was developed to transform micrometer-sized Sb powders into new Sb-sandwiched nanocomposite particles (SiC−Sb−C) with Sb nanoparticles pinned on rigid SiC nanocores and surface-coated with carbon by use of a high-energy mechanical milling technique at ambient temperature. The as-prepared SiC−Sb−C nanoparticles exhibited excellent cycling ability and rate capability, delivering a specific capacity of >440 mA·h g−1 after 120 cycles and a quite high capacity of ≥220 mA·h g−1 at a very high-rate of 4 C (2000 mA g−1). This greatly improved electrochemical performance could be attributed to the structural stability of this material, which can not only effectively confine the volume expansion of the sandwiched Sb layer but also prevent the aggregation of Sb nanocrystallites and keep the mechanical integrity of the electrodes. In addition, this new synthetic method is completely green with a full utilization of raw materials and without any emission of wastes, easily adopted for large-scale production and also extended for other attractive lithium storage metals and alloys.
Co-reporter:Yan Jiang;Pin Liu;Yuliang Cao;Jiangfeng Qian
Journal of Applied Electrochemistry 2009 Volume 39( Issue 10) pp:
Publication Date(Web):2009 October
DOI:10.1007/s10800-009-9902-6
A new fire-retardant, diethyl ethyl phosphate (DEEP), was tested as a nonflammable electrolyte solvent for dye-sensitized solar cells (DSSCs). Electrochemical measurements demonstrated that the DEEP electrolyte has a wide potential window (>5 V), sufficient ionic conductivity (3.5 × 10−3 S cm−1 at 25 °C), and electrochemical activity for the \( I^{ - } /I_{3}^{ - } \) redox couple. The DEEP-based DSSCs exhibited an open circuit voltage of 0.72 V, short circuit photocurrent of 10.45 mA cm−2, and a light-to-electricity conversion efficiency of 4.53%, which are almost the same as those observed from the DSSCs using currently optimized organic carbonate electrolytes. Meanwhile, the long-term stability of the DSSCs was greatly improved with the use of the DEEP electrolyte, showing a potential application of this new electrolyte for the construction of efficient, stable, and nonflammable DSSCs.
Co-reporter:Yunyun Gui, Yuliang Cao, Guoran Li, Xinping Ai, Xueping Gao, Hanxi Yang
Energy Storage Materials (October 2016) Volume 5() pp:165-170
Publication Date(Web):1 October 2016
DOI:10.1016/j.ensm.2016.07.004
Solar fuels and fuel cells are two of the key enabling technologies for clean and sustainable electricity generation. However, photo-synthesis of hydrocarbon or hydrogen fuels is kinetically slow and low efficient, while the current fuel cells use pure hydrogen fuel and precious metal electro-catalysts, which pose severe cost and resource restraints for commercial application. Here, we propose and construct a solar storable fuel cell (SSFC) based on the photo-oxidation of organic wastes and the oxygen reduction reaction at the MnO2 air cathode, which generates electricity with simultaneous photo-degradation of organic contaminants in waste water. As a proof-of-principle device, the SSFC delivers a stable voltage of +0.6 V at constant current of 20 μA cm−2 with almost complete degradation of methyl orange in aqueous solution in an hour, demonstrating an effective utilization of the organic waste for direct electricity generation.
Co-reporter:Lin Wu, Xiaohong Hu, Jiangfeng Qian, Feng Pei, Fayuan Wu, Rongjun Mao, Xinping Ai, Hanxi Yang and Yuliang Cao
Journal of Materials Chemistry A 2013 - vol. 1(Issue 24) pp:NaN7184-7184
Publication Date(Web):2013/04/18
DOI:10.1039/C3TA10920H
A Sn–SnS–C nanocomposite is prepared by simply mechanically ball-milling Sn, SnS and C powders. In this composite, Sn nanocrystals are surface-coated with SnS nanoparticles and uniformly dispersed in the carbon matrix. During discharge, the SnS particles undergo an electrochemical conversion reaction to generate Sn and Na2S nanocrystals and then the Sn particles alloy with Na to produce the NaSn alloy. The conversion reaction of SnS and the alloying reaction of Sn with Na are completely reversible, producing a very high reversible Na-storage capacity of >600 mA h g−1 at an appropriate low potential of ∼0.7 V. Since the SnS phase provides an effective buffering matrix to alleviate the volumetric change of the Sn particles during Na insertion and extraction, and also serves as a separator to prevent the aggregation of the Sn nanoparticles, the Sn–SnS–C composite anode demonstrates a very good cycling stability with 87% capacity retention over 150 cycles, possibly usable for Na-ion batteries.
Co-reporter:Dingding Yuan, Wei He, Feng Pei, Fayuan Wu, Yue Wu, Jiangfeng Qian, Yuliang Cao, Xinping Ai and Hanxi Yang
Journal of Materials Chemistry A 2013 - vol. 1(Issue 12) pp:NaN3899-3899
Publication Date(Web):2013/01/17
DOI:10.1039/C3TA01430D
Stable Na+ ion storage cathodes with adequate reversible capacity are now greatly needed for enabling Na-ion battery technology for large scale and low cost electric storage applications. In light of the superior Li+ ion storage performance of layered oxides, pure P2-phase Na0.67[Mn0.65Ni0.15Co0.2]O2 microflakes are synthesized by a simple sol–gel method and tested as a Na+ ion storage cathode. These layered microflakes exhibit a considerably high reversible capacity of 141 mA h g−1 and a slow capacity decay to 125 mA h g−1 after 50 cycles, showing much better cyclability than previous NaMnO2 compounds. To further enhance the structural and cycling stability, we partially substituted Co3+ by Al3+ ions in the transition-metal layer to synthesize Na0.67[Mn0.65Ni0.15Co0.15Al0.05]O2. As expected, the Al-substituted material demonstrates a greatly improved cycling stability with a 95.4% capacity retention over 50 cycles, possibly serving as a high capacity and stable cathode for Na-ion battery applications.
Co-reporter:L. M. Zhu, A. W. Lei, Y. L. Cao, X. P. Ai and H. X. Yang
Chemical Communications 2013 - vol. 49(Issue 6) pp:NaN569-569
Publication Date(Web):2012/11/23
DOI:10.1039/C2CC36622C
An all-organic rechargeable battery is realized by use of polyparaphenylene as both cathode- and anode-active material. This new battery can operate at a high voltage of 3.0 V with fairly high capacity, offering a renewable and cheaper alternative to conventional batteries.
Co-reporter:Limin Zhu, Yifei Shen, Mengying Sun, Jiangfeng Qian, Yuliang Cao, Xinping Ai and Hanxi Yang
Chemical Communications 2013 - vol. 49(Issue 97) pp:NaN11372-11372
Publication Date(Web):2013/10/16
DOI:10.1039/C3CC46642F
A Na-host cathode is developed by grafting the polypyrrole chains with ionizable sodium sulfonate. Due to the immobile p-doping of organic anions, the self-doped polymer can act as a Na-host for reversible Na insertion–extraction reaction, thus offering a low cost and renewable organic cathode for Na ion battery applications.
Co-reporter:Zhongxue Chen, Yuliang Cao, Jiangfeng Qian, Xinping Ai and Hanxi Yang
Journal of Materials Chemistry A 2010 - vol. 20(Issue 34) pp:NaN7271-7271
Publication Date(Web):2010/07/27
DOI:10.1039/C0JM00829J
A simple synthetic route was developed to obtain Sn-sandwiched composite nanoparticles by mechanical ball-milling ductile Sn particles with rigid SiC nanocores to form a SiC@Sn core-shell nanocomposite and then carbon-coating the SiC@Sn nanoparticles with graphite to produce the SiC@Sn@C nanoparticles. Such a novel nanostructure can effectively buffer the mechanical stress and prevent the aggregation of the Sn nanolayer and therefore improve the electrochemical utilization and cycling stability of electroactive Sn during Li-storage reaction. The Sn-sandwiched nanoparticles as-prepared exhibited a considerable high Li-storage capacity of ∼600 mA h g−1 and an excellent cycling stability with ∼90% capacity retention at 100 cycles, showing a prospect for practical lithium battery applications. In particular, the reported synthetic method is very simple, low-cost and pollution-free, enabling it to be readily adopted for large-scale production and also to be extended for other attractive lithium storage metals and alloys.
Co-reporter:Zhongxue Chen, Shen Qiu, Yuliang Cao, Xinping Ai, Kai Xie, Xiaobin Hong and Hanxi Yang
Journal of Materials Chemistry A 2012 - vol. 22(Issue 34) pp:NaN17772-17772
Publication Date(Web):2012/07/06
DOI:10.1039/C2JM33338D
Spinel LiNi0.5Mn1.5O4 has attracted extensive interest as an appealing cathode material of next generation lithium-ion batteries to meet the cost/performance requirements for electric vehicle applications and renewable electric energy storage. In this paper, we report, for the first time, a nanoflake-stacked LiNi0.5Mn1.5O4 spinel with oriented growth of the (001) planes synthesized via an in situ template route. The resultant LiNi0.5Mn1.5O4 cathode delivers an initial discharge capacity of 133.5 mA h g−1 at 1 C with capacity retention of 86% after 500 cycles. X-ray diffraction and transmission electron microscopy results suggest that the growth of (111) facets on the surfaces of the nanoflake-stacked LiNi0.5Mn1.5O4 spinel is significantly restricted, which helps to inhibit the dissolution of manganese from the lattice and ensure an excellent cycling stability. Moreover, the very thin nanoflakes and large interspaces between the nanoflakes are favorable for Li ion transportation, leading to a fast kinetics of the LiNi0.5Mn1.5O4 spinel. As a result, the material demonstrates a reversible capacity of 96 mA h g−1 even at 50 C rate, showing a feasible application for high-power lithium ion batteries. In particular, this study provides a synthetic strategy to fabricate insertion materials with a surface-oriented morphology and nanoflake-stacked structure for energy storage, fast-ion conductors and other applications.
Co-reporter:Wenwen Deng, Yifei Shen, Jiangfeng Qian and Hanxi Yang
Chemical Communications 2015 - vol. 51(Issue 24) pp:NaN5099-5099
Publication Date(Web):2015/02/17
DOI:10.1039/C5CC00073D
A redox-active and water-insoluble polyimide, poly-(naphthalene four formyl ethylenediamine), demonstrates a high capacity of 130 mA h g−1, a strong rate capability at 10 C rate and an excellent capacity retention of 91.2% over 1000 cycles, offering a low cost and environmentally benign anode for aqueous Na-ion batteries.
Co-reporter:Jiangfeng Qian, Dan Qiao, Xinping Ai, Yuliang Cao and Hanxi Yang
Chemical Communications 2012 - vol. 48(Issue 71) pp:NaN8933-8933
Publication Date(Web):2012/07/17
DOI:10.1039/C2CC34388F
An amorphous phosphorus/carbon nanocomposite demonstrates a reversible 3-Li storage capacity of 2355 mAh g−1 with an excellent capacity retention of 90% over 100 cycles and a superior power capability with 62% of its capacity realizable at a very high rate of 8000 mA g−1, possibly serving as a high capacity and high rate alternative anode for next-generation Li-ion batteries.
Co-reporter:Zhongxue Chen, Shen Qiu, Yuliang Cao, Jiangfeng Qian, Xinping Ai, Kai Xie, Xiaobin Hong and Hanxi Yang
Journal of Materials Chemistry A 2013 - vol. 1(Issue 16) pp:NaN4992-4992
Publication Date(Web):2013/02/12
DOI:10.1039/C3TA00611E
A hierarchical porous Li2FeSiO4/C composite was prepared using an in situ template synthesis by tetraconstituent co-assembly of resols, nitrates, silica oligomers, and a triblock copolymer surfactant. The structural and electrochemical characterizations revealed that the Li2FeSiO4/C composite has a hierarchical micro-, meso- and macro-porous structure, in which macrosized pores provide abundant electrolyte channels for fast ionic transport, while the microporous network offers large accessible electrochemically active areas for the Li insertion reaction. The Li2FeSiO4/C composite demonstrates a very high capacity of 254 mA h g−1 at room temperature with excellent cycling stability and rate capability, corresponding to 77.5% utilization of its theoretical 2 Li storage capacity. The results from this study suggest a feasible approach to improve dramatically the electrochemical utilization and cyclability of the kinetically sluggish intercalation compounds by creating an electrochemically favorable porous structure and the synthetic strategy described in this work may be extended to fabricate other types of porous multifunctional materials for energy storage, catalysis and other applications.
Co-reporter:Jiangfeng Qian, Yao Chen, Lin Wu, Yuliang Cao, Xinping Ai and Hanxi Yang
Chemical Communications 2012 - vol. 48(Issue 56) pp:NaN7072-7072
Publication Date(Web):2012/05/29
DOI:10.1039/C2CC32730A
A Sb/C nanocomposite was synthesized and found to deliver a reversible 3 Na storage capacity of 610 mA h g−1, a strong rate capability at a very high current of 2000 mA g−1 and a long-term cycling stability with 94% capacity retention over 100 cycles, offering practical feasibility as a high capacity and cycling-stable anode for room temperature Na-ion batteries.
Co-reporter:Xianyong Wu, Wenwen Deng, Jiangfeng Qian, Yuliang Cao, Xinping Ai and Hanxi Yang
Journal of Materials Chemistry A 2013 - vol. 1(Issue 35) pp:NaN10134-10134
Publication Date(Web):2013/06/21
DOI:10.1039/C3TA12036H
Prussian blue analogues are actively explored as low cost and high capacity cathodes for Na ion batteries; however, their applications are hindered by low capacity utilization and poor cyclability of these compounds. Here we show that this problem can be solved by controlling the purity and crystallinity of the Prussian blue lattices. As a model compound, single-crystal FeIIIFeIII(CN)6 nanoparticles are synthesized and found to have a sufficiently high capacity of 120 mA h g−1, an exceptional rate capability at 20 C and superior cyclability with 87% capacity retention over 500 cycles, showing great promise for Na ion battery applications. More significantly, these results provide a new insight into the intercalation chemistry of Prussian blue analogues and open new perspectives to develop Na storage cathodes for widespread applications of electric energy storage.
Co-reporter:Fei Xu, Hongtao Wang, Jianghui Lin, Xiao Luo, Shun-an Cao and Hanxi Yang
Journal of Materials Chemistry A 2016 - vol. 4(Issue 29) pp:NaN11497-11497
Publication Date(Web):2016/06/30
DOI:10.1039/C6TA03956A
Redox-active organic imides are potential alternatives to transition-metal based cathodes for material-sustainable and environmentally friendly Na-ion batteries; however, their poor cyclability remains a challenge for battery applications. To address this issue, we use a redox-active anthraquinone to link the small carbonyl molecules to obtain a conjugated polymer with multiple redox-active centers. Herein, we synthesize four cathode-active poly(anthraquinonyl imide)s (PAQIs) from pyromellitic dianhydride (or 1,4,5,8-naphthalenetetracarboxylic dianhydride) and 1,4-diaminoanthraquinone (or 1,5-diaminoanthraquinone). The as-prepared PAQI materials exhibit a high reversible capacity of 190 mA h g−1 and a stable cyclability with 93% capacity retention over 150 cycles, suggesting a possible use of these organic cathode materials for high capacity Na-ion batteries.
Co-reporter:Ya Xiong, Jiangfeng Qian, Yuliang Cao, Xinping Ai and Hanxi Yang
Journal of Materials Chemistry A 2016 - vol. 4(Issue 29) pp:NaN11356-11356
Publication Date(Web):2016/06/22
DOI:10.1039/C6TA04402F
Anatase TiO2 has low-cost and potentially high capacity as a Na-storage anode, but its low capacity utilization and poor rate capability remain a challenge for practical battery applications. To address this issue, we synthesized graphene-supported TiO2 nanospheres through a facile hydrothermal process, aiming at enhancing the electrochemical capacity and kinetics of this material. The porous TiO2 nanospheres offer abundant electrochemically active surface sites and ionic channels, enabling high utilization of the TiO2 nanoparticles, meanwhile the rGO matrices provide high electronic conduction and prevent the aggregation of the TiO2 nanoparticles during repeated cycles. The as-prepared rGO–TiO2 electrode demonstrates a high capacity of 300 mA h g−1 and a cycling stability with a capacity retention of 208 mA h g−1 over 300 cycles. Also, this rGO–TiO2 electrode exhibits a high rate capability of 123.1 mA h g−1 at a very high rate of 4.0 A g−1. The structural design and synthesis route described in this work may provide an effective approach to promote the electrochemical performance of Na-insertion materials for high-rate and high capacity Na-ion batteries.
