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Manipulation of Na_(3)V_(2)(PO_(4))_(2)F_(3) via aluminum doping to alter local electron states toward an advanced cathode for sodiumion batteries

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Rare Metals 2024年第9期43卷 4253-4262页

作者： Shi-Min wang Jin-qi li li Xu Meng-Jiao Sun Wen-Jin Huang qing liu Fu-tong Ren Yong-Jiang Sun ling-Yan Duan Hang Ma Hong Guo International Joint Research Center for Advanced Energy Materials of Yunnan Province Yunnan Key Laboratory of Carbon Neutrality and Green Low-Carbon TechnologiesSchool of Materials and EnergyYunnan UniversityKunming 650091China college of environmental and chemical engineering Metallurgy CollegeKunming 650033China R&D Center Yunnan Yuntianhua Co.LtdKunming 650228China Southwest United Graduate School Kunming 650091China

With its unique 3D skeleton structure and exceptional cyclic stability,the Na^(+)superionic conducto(NASICON)-type Na_(3)V_(2)(PO_(4))_(2)F_(3)(NVPF)has been con sidered as a competitive cathode material for advanced Na ion ***,the release of fluorine during th heat treatment leads to the formation of an additional phas Na_(3)V_(2)(PO_(4))_(3)(NVP),which results in a low-voltage plateau and compromises the energy ***,we modulat the local electronic states of the V site by aluminum sub stitution to strengthen the stability of *** results confirm that the aluminum introduction not only changes the loca electron states of V sites,significantly reducing the for mation of NVP by-product from 6.71 wt%to 1.01 wt%but also effectively reduces the band gap,improving th electronic conductivity of *** optimized Na_(3)V_(1.9)Al_(0.1)(PO_(4))_(2)F_(3)exhibits higher energy density of 340 Wh·kg^(-1)and excellent rate performance of 106.7 mAh·g^(-1)at 10C compared with the pristine cathode.

关键词： Sodium-ion energy storage batteries Cathode NASICON Doping Electrochemistry

大气NR-PM_(1)特性的多尺度演变及其影响机制

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中国环境科学 2024年第9期44卷 4737-4753页

作者：田健韩力慧兰童齐超楠肖茜王海燕北京工业大学环境科学与工程学院区域大气复合污染防治北京市重点实验室北京100124

通过采用气溶胶化学组分在线监测质谱仪(ACSM)实时监测了北京市东南城区2021年12月至2022年11月大气非难熔亚微米颗粒物NR-PM_(1)及其组分有机物(Org)、硫酸盐(SO_(4)^(2-))、硝酸盐(NO_(3)^(-))、铵盐(NH_(4)^(+))和氯化物(Cl^(-))浓度... 详细信息

通过采用气溶胶化学组分在线监测质谱仪(ACSM)实时监测了北京市东南城区2021年12月至2022年11月大气非难熔亚微米颗粒物NR-PM_(1)及其组分有机物(Org)、硫酸盐(SO_(4)^(2-))、硝酸盐(NO_(3)^(-))、铵盐(NH_(4)^(+))和氯化物(Cl^(-))浓度,分析研究了NR-PM_(1)及其组分不同时间尺度,特别是污染期间的变化特征,以及影响二次硫酸盐和硝酸盐形成的重要因素.同时,结合正交矩阵因子分析法(PMF)和后向轨迹聚类分析法分别探究了有机气溶胶(OA)不同时段物种的变化特征,以及不同时段气团长距离传输对NR-PM_(1)及其组分的影响机制.结果表明,研究期间NR-PM_(1)年均质量浓度为(7.60±10.35)μg/m^(3),低于2016年以来相应的年均值,并呈现出逐年下降的趋势,不同季节其平均浓度呈现出秋季>春季>冬季>夏季的季节变化特征,不同季节其日变化均呈现出夜间高于白天的特征.NR-PM_(1)物种年均质量浓度呈现出Org>NO_(3)^(-)>NH_(4)^(+)~SO_(4)^(2-)>Cl^(-)的特征,其中Org对NR-PM_(1)的贡献最大,约为41.16%,其后依次为硝酸盐33.05%,铵盐12.47%,硫酸盐11.99%,氯化物最小,约为1.33%.不同季节NR-PM_(1)组分浓度的昼夜变化均较小,NR-PM_(1)及其组分在霾污染天的平均浓度均大于臭氧污染天和清洁天.大气中碱性NH_3的存在以及霾污染天的气象条件更有利于气态前体物的二次转化.不同季节OA物种有所不同,冬季、春季和秋季的二次有机气溶胶(SOA)是OA的主要组分,而夏季一次有机气溶胶(POA)是OA的主要组分,霾污染天和臭氧污染天OA均主要受二次有机物生成的影响.不同季节气团传输途径有所不同,值得注意的是霾污染天主要受东南方向和南方向短距离气团输送的影响,且NO_(3)^(-)对NR-PM_(1)的贡献较大.O_(3)污染天主要受南方向的短距离气团输送的影响,而清洁天以西北方向长距离气团输送为主.

关键词： NR-PM_(1) 理化特性多尺度演变影响因素

A facial strategy to efficiently improve catalytic performance of CoFe_(2)O_(4) to peroxymonosulfate

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Journal of environmental Sciences 2022年第6期34卷 1-13页

作者： lili Gao Jieqiong Deng tong li Kai qi Jiandong Zhang Qun Yi college of environmental Science and engineering Taiyuan University of TechnologyTaiyuan 030024China college of Biomedical engineering Taiyuan University of TechnologyTaiyuan 030024China

Cobalt iron spinel(CoFe_(2)O_(4)) has been considered as a good heterogeneous catalysis to peroxymonosulfate(PMS) in the degradation of persistent organic pollutants due to its magnetic properties and good chemical stability. However, its catalytic activity needs to be further improved. Here, a facial strategy, “in-situ substitution”, was adopted to modify CoFe_(2)O_(4) to improve its catalytic performance just by suitably increasing the Co/Fe ratio in synthesis process. Compared with CoFe_(2)O_(4), the newly synthesized Co_(1.5)Fe_(1.5)O_(4), could not only significantly improve the degradation efficiency of phenol, from 50.69 to 93.6%, but also exhibited more effective mineralization ability and higher PMS utilization. The activation energy advantage for phenol degradation using Co_(1.5)Fe_(1.5)O_(4)was only 44.2 k J/mol, much lower than that with CoFe_(2)O_(4)(127.3 k J/mol). A series of related representations of CoFe_(2)O_(4) and Co_(1.5)Fe_(1.5)O_(4) were compared to explore the possible reasons for the outstanding catalytic activity of Co_(1.5)Fe_(1.5)O_(4). Results showed that Co_(1.5)Fe_(1.5)O_(4)as well represented spinel crystal as CoFe_(2)O_(4)and the excess cobalt just partially replaced the position of iron without changing the original structure. Co_(1.5)Fe_(1.5)O_(4) had smaller particle size(8.7 nm), larger specific surface area(126.3 m^(2)/g), which was more favorable for exposure of active sites. Apart from the superior physical properties, more importantly, more reactive centers Co(Ⅱ) and surface hydroxyl compounds generated on Co_(1.5)Fe_(1.5)O_(4), which might be the major reason. Furthermore, Co_(1.5)Fe_(1.5)O_(4) behaved good paramagnetism, wide range of pH suitability and strong resistance to salt interference, making it a new prospect in environmental application.

关键词： CoFe_(2)O_(4) Co_(1.5)Fe_(1.5)O_(4) In-situ substitution Peroxymonosulfate(PMS) Advanced oxidation processes(AOPs)

中国典型城市大气降水离子特性、来源及其对环境的影响

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中国环境科学 2024年第10期44卷 5329-5343页

作者：肖茜韩力慧齐超楠田健兰童王海燕郑爱华郭敬华北京工业大学环境科学与工程学院北京100124 区域大气复合污染防治北京市重点实验室北京100124 北京师范大学分析测试中心北京100875

基于采样数据和东亚酸沉降监测网数据,对2019年华北、西北、西南、华东和华南地区典型代表城市的大气降水化学组分、酸度及其成因、湿沉降量和污染来源进行了研究,评估了降水对环境的生态效应.结果表明,离子总浓度在季节上表现为旱季明... 详细信息

基于采样数据和东亚酸沉降监测网数据,对2019年华北、西北、西南、华东和华南地区典型代表城市的大气降水化学组分、酸度及其成因、湿沉降量和污染来源进行了研究,评估了降水对环境的生态效应.结果表明,离子总浓度在季节上表现为旱季明显大于雨季,空间分布特征为:北京(706.87μeq/L)>西安(369.26μeq/L)>重庆(265.17μeq/L)>厦门(244.54μeq/L)>珠海(134.31μeq/L)>五指山(81.88μeq/L).NH_(4)^(+)、Ca^(2+)、SO_(4)^(2-)和NO_(3)^(-)是内陆城市降水中最主要的离子成分,而Cl^(-)和Na^(+)在沿海城市中占比较大.华北城市降水主要呈中性,酸雨事件仅占全年降水事件的2.3%;西北城市降水呈弱碱性,没有出现酸雨事件;而西南城市酸雨问题严重,城区站点和乡郊站点酸雨频率分别为30.3%和80.3%,且季节变化明显;华东城市城区站点降水主要呈中性,偏远地区站点酸雨问题严重,全年酸雨率高达99%;华南城市夏季降水主要呈中性,其余季节均为酸性,全年酸雨事件占总降水的62.2%.中和能力分析表明酸雨问题严重的地区,主要是由降水中碱性成分不足导致的.受降雨量影响,各城市氮和硫湿沉降量在季节上表现为雨季大于旱季,并且在雨季对生态环境有重要的促进作用.中国氮和硫湿沉降量均呈现出从东部向西部、沿海向内陆递减的空间分布特征.不同城市降水离子来源及贡献差异较显著,尤其是酸雨问题严重的城市,其以Ca^(2+)和Mg^(2+)为主的扬尘源贡献小于以SO_(4)^(2-)和NO_(3)^(-)为主的二次源贡献.

关键词：大气降水水溶性离子酸度成因湿沉降量来源解析

Efficient degradation of Rhodamine B by magnetically recoverable Fe_(3)O_(4)-modified ternary CoFeCu-layered double hydroxides via activating peroxymonosulfate

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Journal of environmental Sciences 2021年第10期33卷 188-200页

作者： tong li Xiange Du Jieqiong Deng Kai qi Jiandong Zhang lili Gao Xiuping Yue college of environmental Science and engineering Taiyuan University of TechnologyShanxi 030024China Department of Biological and Pharmaceutical engineering College of Biomedical EngineeringUniversity of TechnologyShanxi 030024China

Environment-friendly nano-catalysts capable of activating peroxymonosulfate(PMS)have received increasing attention ***,traditional nano-catalysts are generally well dispersed and difficult to be separated from reaction system,so it is particularly important to develop nano-catalysts with both good catalytic activity and excellent recycling *** this work,magnetically recoverable Fe_(3)O_(4)-modified ternary CoFeCu-layered double hydroxides(Fe_(3)O_(4)/CoFeCu-LDHs)was prepared by a simple co-precipitation method and initially applied to activate PMS for the degradation of Rhodamine B(Rh B).X-ray diffraction(XRD),fourier transform infrared spectrometer(FT-IR),scanning electron microscope(SEM),transmission electron microscopy(TEM),Brunauer-Emmett-Teller method(BET),and vibrating sample magnetometer(VSM)were applied to characterize morphology,structure,specific surface area and *** addition,the effects of several key parameters were *** Fe_(3)O_(4)/CoFeCu-LDHs exhibited high catalytic activity,and Rh B degradation efficiency could reach 100%within 20 min by adding 0.2 g/L of catalyst and 1 mmol/L of PMS into 50 mg/L of Rh B solution under a wide pH condition(3.0-7.0).Notably,the Fe_(3)O_(4)/CoFeCu-LDHs showed good super-paramagnetism and excellent stability,which could be effectively and quickly recovered under magnetic condition,and the degradation efficiency after ten cycles could still maintain 98.95%.Both radicals quenching tests and electron spin resonance(ESR)identified both HO·and SO_(4)^(·-) were involved and SO_(4)^(·-) played a dominant role on the RhB ***,the chemical states of the sample’s surface elements were measured by X-ray photoelectron spectroscopy(XPS),and the possible activation mechanism in Fe_(3)O_(4)/CoFeCu-LDHs/PMS system was proposed according to comprehensive analysis.

关键词： Advanced catalytic oxidation Fe_(3)O_(4)/CoFeCu-LDHs Peroxymonosulfate Rhodamine B(RhB) High degradation efficiency Heterogeneous catalyst

用于li-CO_(2)电池的阴极催化剂:发展及挑战

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储能科学与技术 2024年第10期13卷 3453-3466页

作者：王雨锟李雪莲雷普英齐凯高丽丽王转培杨晓伟太原理工大学环境科学与工程学院山西晋中030600 山西省重点实验室大气复合污染识别与控制山西太原030024 山西中科华能科技有限公司山西太原030032 河南大学能源科学与技术学院河南郑州450046 上海交通大学化学化工学院上海200240

在能源危机与温室效应日益加剧的形势下,li-CO_(2)电池作为一种兼具高效储能与CO_(2)气体利用的新型器件,具有重大的研究意义。鉴于电池涉及多相反应,电子传递与物质转移主要发生于阴极,因此,li-CO_(2)电池阴极催化剂的设计与制备显得... 详细信息

在能源危机与温室效应日益加剧的形势下,li-CO_(2)电池作为一种兼具高效储能与CO_(2)气体利用的新型器件,具有重大的研究意义。鉴于电池涉及多相反应,电子传递与物质转移主要发生于阴极,因此,li-CO_(2)电池阴极催化剂的设计与制备显得尤为重要。本文探讨了li-CO_(2)电池作为新型储能器件的优势,基于li-CO_(2)电池充放电反应机理的发展历程,深入探讨了目前其面临的关键挑战,如充放电电位差较大,容量衰减快和循环稳定性差等问题,将解决方案聚焦于阴极催化剂的研发,提出高效催化剂应该满足的核心条件。总结了近年来碳基非金属,贵金属和过渡金属等传统催化剂在li-CO_(2)电池领域的应用情况,并深入分析了各类催化剂的优势与不足;本文重点介绍了新兴的单原子催化剂与氧化还原介质研究进展,通过结构表征和理论计算证明其在li-CO_(2)电池领域展现出卓越的催化性能;本文深入剖析了li-CO_(2)电池进一步发展所面临的关键问题与严峻挑战,并对单原子催化剂未来的研究方向进行了展望,旨在为推动li-CO_(2)电池技术的不断进步提供有益的参考与借鉴。

关键词： li-CO_(2)电池反应机理正极单原子催化剂

Manipulating dielectric property of polymer coatings toward highretention-rate lithium metal full batteries under harsh critical conditions

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Nano Research 2023年第7期16卷 9240-9249页

作者： qi Kang Zechao Zhuang Yong li Yinze Zuo Jian wang Yijie liu Chaoqun Shi Jie Chen Hongfei li Pingkai Jiang Xingyi Huang Department of Polymer Science and engineering Shanghai Key Laboratory of Electrical Insulation and Thermal AgeingSchool of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China Department of Chemistry Tsinghua UniversityBeijing 100084China Institute of Applied and Physical Chemistry and Center for environmental Research and Sustainable Technology University of BremenBremen 28359Germany Institute for Sustainable Energy/college of Sciences Shanghai UniversityShanghai 200444China Helmholtz Institute Ulm(HIU) Ulm D89081Germany School of Electrical engineering Xi’an Jiaotong UniversityXi’an 710049China

lithium(li)metal batteries(LMBs)can potentially deliver much higher energy density but remain plagued by uncontrollable li plating with dendrite growth,unstable interfaces,and highly abundant excess li(>50 mAh·cm^(-2)).Herein,different from the artificial layer or three-dimensional(3D)matrix host constructions,various dielectric polymers are initially well-comprehensively investigated from experimental characterizations to theoretical simulation to evaluate their functions in modulating li ion *** a proof of concept,a 3D interwoven high dielectric functional polymer(HDFP)nanofiber network with polar C-F dipole moments electrospun on copper(Cu)foil is designed,realizing uniform and controllable li deposition capacity up to 5.0 mAh·cm^(-2),thereby enabling stable li plating/stripping cycling over 1400 h at 1.0 mA·cm^(-2).More importantly,under the highcathode loading(~3.1 mAh·cm^(-2))and only 0.6×excess li(N/P ratio of 1.6),the full cells retain capacity retention of 97.4%after 200 cycles at 3.36 mA·cm^(-2)and achieve high energy density(297.7 Wh·kg^(-1)at cell-level)under lean electrolyte conditions(15μL),much better than ever-reported *** work provides a new direction for designing high dielectric polymer coating toward high-retention-rate practical li full batteries.

关键词： high dielectric functional polymer nanofiber li metal full cell low N/P ratio high-retention capacity

The Main Progress of Perovskite Solar Cells in 2020-2021

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Nano-Micro Letters 2021年第10期13卷 113-130页

作者： Tianhao Wu zhenzhen qin Yanbo wang Yongzhen Wu Wei Chen Shufang Zhang Molang Cai Songyuan Dai Jing Zhang Jian liu Zhongmin Zhou Xiao liu Hiroshi Segawa Hairen Tan Qunwei Tang Junfeng Fang Yaowen li liming Ding Zhijun ning Yabing qi Yiqiang Zhang liyuan Han State Key Laboratory of Metal Matrix Composites School of Material Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240People’s Republic of China Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Centre Shanghai Key Laboratory of Functional Materials ChemistryJoint International Research Laboratory of Precision Chemistry and Molecular EngineeringSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyMeilong Road 130Shanghai 200237People’s Republic of China Wuhan National Laboratory for Optoelectronics Huazhong University of Science and TechnologyLuoyu Road 1037Wuhan 430074People’s Republic of China college of Materials Science and engineering Nanjing University of Science and TechnologyNanjing 210094People’s Republic of China Beijing Key Laboratory of Novel Thin-Film Solar Cells and State Key Laboratory of Alternate Electrical Power System With Renewable Energy Sources North China Electric Power UniversityBeijing 102206People’s Republic of China Department of Microelectronic Science and engineering Ningbo UniversityZhejiang 315211People’s Republic of China college of chemical engineering Jiangsu Key Lab of Biomass-Based Green Fuels and ChemicalsNanjing Forestry UniversityNanjing 210037People’s Republic of China college of Chemistry and Molecular engineering Qingdao University of Science and TechnologyQingdao 266042People’s Republic of China Special Division of environmental and Energy Science Komaba Organization for Educational Excellence(KOMEX)College of Arts and SciencesUniversity of TokyoTokyo 153-8902Japan National Laboratory of Solid State Microstructures Jiangsu Key Laboratory of Artificial Functional MaterialsCollege of Engineering and Applied SciencesNanjing UniversityNanjing 210093People’s Republic of China college of Information Science and Technology Jinan UniversityGuangzhou 510632People’s Republic of China School of Physics and Electronic Science Engineering Research Center of Nan

Perovskite solar cells(PSCs)emerging as a promising photovoltaic technology with high efficiency and low manufacturing cost have attracted the attention from all over the *** the efficiency and stability of PSCs have increased steadily in recent years,and the research on reducing lead leakage and developing eco-friendly lead-free perovskites pushes forward the commercialization of PSCs step by *** review summarizes the main progress of PSCs in 2020 and 2021 from the aspects of efficiency,stability,perovskite-based tandem devices,and lead-free ***,a brief discussion on the development of PSC modules and its challenges toward practical application is provided.

关键词： Perovskite solar cells Stability Solar module Perovskite-based tandem devices Lead-free perovskite

Improving stability of MXenes

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Nano Research 2022年第7期15卷 6551-6567页

作者： Jizhou Jiang Saishuai Bai Jing Zou Song liu Jyh-Ping Hsu Neng li Guoyin Zhu Zechao Zhuang qi Kang Yizhou Zhang School of environmental Ecology and Biological engineering School of Chemistry and Environmental EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationWuhan Institute of TechnologyWuhan 430205China Key Laboratory of Rare Mineral Ministry of Natural ResourcesGeological Experimental Testing Center of Hubei ProvinceWuhan 430034China Institute of chemical Biology and Nanomedicine(ICBN) State Key Laboratory of Chemo/Biosensing and ChemometricsCollege of Chemistry and Chemical EngineeringCollege of BiologyHunan UniversityChangsha 410082China Department of chemical engineering “National Taiwan University”Taipei 10617TaiwanChina State Key Laboratory of Silicate Materials for Architectures Wuhan University of TechnologyWuhan 430070China Institute of Advanced Materials and Flexible Electronics(IAMFE) School of Chemistry and Materials ScienceNanjing University of Information Science&TechnologyNanjing 210044China Department of Chemistry Tsinghua UniversityBeijing 100084China Department of Polymer Science and engineering Shanghai Key Laboratory of Electrical Insulation and Thermal AgeingShanghai Jiao Tong UniversityShanghai 200240China

Due to their superior hydrophilicity and conductivity,ultra-high volumetric capacitance,and rich surface-chemistry properties,MXenes exhibit unique and excellent performance in catalysis,energy storage,electromagnetic shielding,and life *** they are derived from ceramics(MAX phase)through etching,one of the challenges in MXenes preparation is the inevitable exposure of metal atoms on their surface and embedding of anions and *** the as-obtained MXenes are always in a thermodynamically metastable state,they tend to react with trace oxygen or oxygen-containing groups to form metal oxides or degrade,leading to sharply declined activity and impaired ***,improving the stability of MXenesbased materials is of practical significance in relevant ***,there lacks a comprehensive review in the literature on relevant *** help promote the wide applications of MXenes,we review from the following aspects:(i)insights into the factors affecting the stability of MXenes-based materials,including oxidation of MXenes flakes,stability of MXenes colloidal solutions,and swelling and degradation of MXenes thin-film,(ii)strategies for enhancing the stability of MXenes-based materials by optimizing MAX phase synthesis and modifying the MXenes preparation,and(iii)techniques for further increasing the stability of freshly prepared MXenes-based materials via controlling the storage conditions,and forming shielding on the surface and/or edge of MXenes ***,some outlooks are proposed on the future developments and challenges of highly active and stable *** aim to provide guidance for the design,preparation,and applications of MXenes-based materials with excellent stability and activity.

关键词： MXenes stability oxidation swelling and degradation shielding strategies