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Unlocking the multi-electron transfer reaction in NASICON-type cathode materials

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Materials Futures 2023年第2期2卷 109-122页

作者： Yuan Liu Xiaohui Rong Fei Xie Yaxiang Lu Junmei Zhao Liquan Chen Yong-Sheng Hu Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190People’s Republic of China College of Materials Science and Optoelectronic Technology University of Chinese Academy of SciencesBeijing 100049People’s Republic of China Yangtze River Delta Physics Research Center Co.Ltd Liyang 213300People’s Republic of China huairou Division Institute of PhysicsChinese Academy of SciencesBeijing 101400People’s Republic of China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Biochemical EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijingPeople’s Republic of China

The growing concern about scarcity and large-scale applications of lithium resources has attracted efforts to realize cost-effective phosphate-based cathode materials for next-generation Na-ion batteries(NIBs).In previous work,a series of materials(such as Na_(4)Fe_(3)(PO_(4))_(2)(P_(2)O_(7)),Na_(3)VCr(PO_(4))_(3),Na_(4)VMn(PO_(4))3,Na_(3)MnTi(PO_(4))_(3),Na_(3)MnZr(PO_(4))3,etc)with∼120 mAh g^(-1) specific capacity and high operating potential has been proposed.However,the mass ratio of the total transition metal in the above compounds is only∼22 wt%,which means that one-electron transfer for each transition metal shows a limited capacity(the mass ratio of Fe is 35.4 wt%in LiFePO_(4)).Therefore,a multi-electron transfer reaction is necessary to catch up to or go beyond the electrochemical performance of LiFePO_(4).This review summarizes the reported NASICON-type and other phosphate-based cathode materials.On the basis of the aforementioned experimental results,we pinpoint the multi-electron behavior of transition metals and shed light on designing rules for developing high-capacity cathodes in NIBs.

关键词： NASICON Na-ion batteries cathode materials multi-electron transfer reactions

Modification of NASICON Electrolyte and Its Application in Real Na-Ion Cells

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Engineering 2022年第1期8卷 170-180页

作者： Qiangqiang Zhang Quan Zhou Yaxiang Lu Yuanjun Shao Yuruo Qi Xingguo Qi Guiming Zhong yong Yang Liquan Chen Yong-Sheng Hu Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and DevicesBeijing National Laboratory for Condensed Matter PhysicsInstitute of PhysicsChinese Academy of SciencesBeijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Xiamen Institute of Rare-Earth Materials Haixi InstitutesChinese Academy of SciencesXiamen 361021China State Key Laboratory of Physical Chemistry of Solid Surfaces&Department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China HiNa Battery Technology Co. Ltd.Liyang 213300China Yangtze River Delta Physics Research Center Co. Ltd.Liyang 213300China

The low ionic conductivity of solid-state electrolytes(SSEs)and the inferior interfacial reliability between SSEs and solid-state electrodes are two urgent challenges hindering the application of solid-state sodium batteries(SSSBs).Herein,sodium(Na)super ionic conductor(NASICON)-type SSEs with a nominal composition of Na_(3+2x)Zr_(2-x)MgxSi_(2)PO_(12) were synthesized using a facile two-step solid-state method,among which Na_(3.3)Zr_(1.85)Mg_(0.15)Si_(2)PO_(12)(x=0.15,NZSP-Mg_(0.15))showed the highest ionic conductivity of 3.54mS∙cm^(-1) at 25℃.By means of a thorough investigation,it was verified that the composition of the grain boundary plays a crucial role in determining the total ionic conductivity of NASICON.Furthermore,due to a lack of examination in the literature regarding whether NASICON can provide enough anodic electrochemical stability to enable high-voltage SSSBs,we first adopted a high-voltage Na_(3)(VOPO_(4))2F(NVOPF)cathode to verify its compatibility with the optimized NZSP-Mg_(0.15) SSE.By comparing the electrochemical performance of cells with different configurations(low-voltage cathode vs high-voltage cathode,liquid electrolytes vs SSEs),along with an X-ray photoelectron spectroscopy evaluation of the after-cycled NZSP-Mg_(0.15),it was demonstrated that the NASICON SSEs are not stable enough under high voltage,suggesting the importance of investigating the interface between the NASICON SSEs and high-voltage cathodes.Furthermore,by coating NZSP-Mg_(0.15) NASICON powder onto a polyethylene(PE)separator(PE@NASICON),a 2.42 A∙h non-aqueous Na-ion cell of carbon|PE@NASICON|NaNi_(2/9)Cu_(1/9)Fe_(1/3)Mn_(1/3)O_(2) was found to deliver an excellent cycling performance with an 88%capacity retention after 2000 cycles,thereby demonstrating the high reliability of SSEs with NASICON-coated separator.

关键词： Solid-state electrolytes Solid-state sodium batteries NASICON Interface Separator Coating

High-temperature treatment induced carbon anode with ultrahigh Na storage capacity at low-voltage plateau

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Science Bulletin 2018年第17期63卷 1125-1129页

作者： Chenglong Zhao Qidi Wang Yaxiang Lu Baohua Li Liquan Chen Yong-Sheng Hu Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and Devices Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China School of Physical Sciences University of Chinese Academy of Sciences Beijing 100049 China Division of Energy and Environment Engineering Laboratory for the Next Generation Power and Energy Storage Batteries Graduate School at Shenzhen Tsinghua Universty Shenzhen 518055 Chino School of Materials Science and Engineering Tsinghua University Beijing 100084 China

Sodium-ion batteries(NIBs) show great prospect on the energy storage applications benefiting from their low cost and the abundant Na resources despite the expected lower energy density compared with lithium-ion batteries(LIBs). To further enhance the competitive advantage, especially in energy density,developing the high-capacity carbon anode materials can be one of the effective approaches to realize this goal. Herein, we report a novel carbon anode made from charcoal with a high capacity of ~400 m Ah g^(-1), wherein about 85%(>330 mAh g^(-1)) of its total capacity is derived from the long plateau region below ~0.1 V, which differs from those of typical hard carbon materials(~300 m Ah g^(-1)) in NIBs but is similar to the graphite anode in LIBs. When coupled with air-stable Na_(0.9)Cu_(0.22)e_(0.30)Mn_(0.48)O_2 oxide cathode, a high-energy density of ~240 Wh kg^(-1) is achieved with good rate capability and cycling stability. The discovery of this promising carbon anode is expected to further improve the energy density of NIBs towards large-scale electrical energy storage.

关键词：碳阳极材料存储能力高原 Na 低电压高温度 cyclin 钠离子电池

Intrinsic effects of precursor functional groups on the Na storage performance in carbon anodes

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Nano Research 2023年第11期16卷 12579-12586页

作者： Xiaohan Tang Fei Xie Yaxiang Lu Zhao Chen Xiangfei Li Hong Li Xuejie huang Liquan Chen Yuanjiang Pan Yong-Sheng Hu Department of Chemistry Zhejiang UniversityHangzhou 310027China Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and DevicesBeijing National Laboratory for Condensed Matter PhysicsInstitute of PhysicsChinese Academy of SciencesBeijing 100190China huairou Division Institute of PhysicsChinese Academy of SciencesBeijing 101400China Yangtze River Delta Physics Research Center Co. Ltd.Liyang 213300China College of Materials Science and Optoelectronic Technology University of Chinese Academy of SciencesBeijing 100049China

The oxygen-containing functional groups in disordered carbon anodes have been widely reported to influence the Na storage performance.However,the effect of original oxygen-containing groups in the precursors on the final structures and electrochemical performance is rarely studied.Herein,we used the anthraquinone derivatives with different oxygen-containing functional groups as precursors to make the disordered carbon anodes for Na-ion batteries(NIBs).Through comprehensive structural and electrochemical analyses,we found that the different types of functional groups in carbon precursors directly affect the cross-linking process during carbonization.The original precursors containing enough inter-chain oxygen or oxygen-containing functional groups with unsaturated bonds unattached to the ring are beneficial for the oxygen atoms to remain or cross-link in structure to result in more C–O–C group,forming nanovoids and disordered structure,which then determine the high performance of the carbon anodes in NIBs.This work highlights the importance of the type/content of functional groups in precursor and provides guidance for the future design of carbon anodes in NIBs from the perspective of precursor selection.

关键词： disordered carbon precursor oxygen-contained functional group Na-ion batteries

Na-ion batteries:from fundamental research to industrial exploration

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Na-ion batteries:from fundamental research to industrial exp...

Disordered carbon anodes for Na-ion batteries—quo vadis?

中国化学会第三届中国能源材料化学研讨会

作者： Yong-Sheng Hu Institute of Physics Chinese Academy of Sciences

Na-ion batteries have been recently reconsidered for storing the electricity from renewable energy and minielectric vehicles due to the abundant sodium resources and low cost.Furthermore,we can use Na ions as the charge carrier to explore new chemistry and new materials to further decrease the cost.For example,Na cannot form the alloy with Al,

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Science China Chemistry 2021年第10期64卷 1679-1692页

作者： Fei Xie Zhen Xu Zhenyu Guo Yaxiang Lu Liquan Chen Maria-Magdalena Titirici Yong-Sheng Hu Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and DevicesBeijing National Laboratory for Condensed Matter PhysicsInstitute of PhysicsChinese Academy of SciencesBeijing 100190China Department of Chemical Engineering Imperial College LondonLondon SW72AZUK

Na-ion batteries(NIBs)are gradually attracting much attention as an alternative to lead-acid batteries and supplement to Li-ion batteries(LIBs)owing to the abundant Na resources and excellent cost-effectiveness.Since the most commonly used graphite as an anode material in LIBs cannot be inherently used in NIBs,tremendous efforts have been made to advance the fundamental understanding and design of suitable anode materials for NIBs,including the improvement of Na storage capacity and the study on Na storage mechanisms.According to all these studies,disordered carbons are now the most promising anode candidates for NIBs.In this review,we discuss the current challenges and remaining problems to be solved in the area of disordered carbon anode materials for NIBs and provide future insights and research directions.

关键词： disordered carbon anode Na-ion batteries

Nano-sized carboxylates as anode materials for rechargeable lithium-ion batteries

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Journal of Energy Chemistry 2014年第3期23卷 269-273页

作者： Xiaoyan Wu Jie Ma Yong-Sheng Hu Hong Li Liquan Chen Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of Sciences

Nano-sized caiboxylales Na2C7H3NO4 and Na2C6H2N2O4 were prepared and investigated as anode materials for lithium-ion batteries.Both carboxylates exhibit high reversible capacities around 190 mAh/g above a cut-off voltage of 0.8 V vs.Li＋/Li.potentially improving the safety of the batteries.In addition,good rate performance and long cycle life of these carboxylates make them promising candidates as anode materials for lithium-ion batteries.

关键词： carboxylates Na2C7H3NO4 Na2C6H2N2O4 anode lithium-ion batteries

Chinese Internet Searches Provide Inaccurate and Misleading Information to Epilepsy Patients

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Chinese Medical Journal 2015年第24期128卷 3324-3328页

作者： Jian-Ming Liu Ru-Xiang Xu Yong-Sheng Hu Lian-Kun Ren hui Qiao hu Ding Zhi-Liang Liu Affiliated Bayi Brain Hospital Bayi Clinical College Southern Medical University Beijing 100700 China Department of Function Neurosurgery Beijing Xuanwu Hospital Beijing 100053 China Department of Neurology China-Japan Friendship Hospital Beijing 100029 China Department of Neuroelectrophysiology Beijing Tiantan Hospital Beijing 100050 China

Background： Most patients with epilepsy want to learn as much as possible about the disease, and many have turned to the internet for information. Patients are likely to use information obtained from the internet to control their epilepsy, but little is known about the accuracy of this information. In this survey, we have assessed the feasibility and usability ofinternet-based interventions for the treatment of epilepsy. Methods： Data were collected from an internet search. Different search terms were used to obtain general information on epilepsy together with information about medication, types of epilepsy, treatment, women＇s health, and other information. The accuracy of the information was evaluated by a group of experts. Results： A total of 1320 web pages were assessed. The majority were websites related to health. A large number （80.2%） of web pages contained content related to the search term. A significant number of web pages 450/1058 （42.5%） claimed to provide information from a credible source： however, only 206/1058 （19.5%） of the information was accurate and complete; 326/1058 （30.8%） was accurate but incomplete; 328/1058 （31.0%） was correct but nonstandard, and 198/1058 （18.8%） was inaccurate. The authenticity of the information was not significantly different between the two search engines （x^2 = 0.009, P - 0.924）. No significant difference was observed in the information obtained from a specialist or nonspecialist source （x^2 = 7.538, P- 0.057）. There was also no correlation between the quality of the information and the priority （x^2 = 6.880, P = 0,076）. Conclusions： Searching for information about epilepsy on the internet is convenient, but the information provided is not reliable. Too much information is inaccurate or for advertisement purposes, and it is difficult for patients to find the useful information. Turning to the internet for medical knowledge may be harmful. Physicians should be aware that their patients may search for information on the internet and guide them to safe, reputable web

关键词： Epilepsy Health Information Internet Self-management

Hard carbon derived from rice husk as low cost negative electrodes in Na-ion batteries

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Journal of Energy Chemistry 2019年第2期28卷 17-22页

作者： Maria K.Rybarczyk Yunming Li Mo Qiao Yong-Sheng Hu Maria-Magdalena Titirici Marek Lieder Gdansk University of Technology Chemical Faculty Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and DevicesNational Laboratory for Condensed Matter PhysicsInstitute of PhysicsChinese Academy of Sciences Queen Mary University London School of Materials Science & Engineering

Here,we report the synthesis of hard carbon materials(RH) made from natural rice husk through a single pyrolysis process and their application as an anode in sodium-ion batteries.The studies show that the electrochemical properties of RHs are affected by the treatment temperatures,which determine the materials morphology,in particular,their degree of graphitization and extent of continuous channels(nanovoids).The latter are accessible to sodium ions and significantly contribute to charge storage capacity of the produced anodes.The RHs obtained at 1600 °C deliver the highest reversible capacity of276 mAh g^(-1) mainly due to insertion of sodium ions into the nanovoids.This work deepens the basic understanding of the influence of the carbonization temperature on the sodium storage mechanism.

关键词： Nanovoids in rice husk Sustainable energy storage Na-ion batteries