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Fundamental Understanding on Selenium Electrochemistry:From Electrolytic Cell to Advanced Energy Storage

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Energy & Environmental Materials 2024年第3期7卷 236-256页

作者： jiguo tu Cheng Chang Jingxiu Wang Haiping Lei R.Vasant Kumar Mingyong Wang Shuqiang Jiao State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China School of Chemical Engineering The University of AdelaideAdelaideSA 5005Australia School of Metallurgical and Ecological Engineering University of Science and Technology BeijingBeijing 100083China Department of Materials Science and Metallurgy University of CambridgeCambridge CB30FSUK

Selenium(Se),as an important quasi-metal element,has attracted much attention in the fields of thin-film solar cells,electrocatalysts and energy storage applications,due to its unique physical and chemical ***,the electrochemical behavior of Se in different systems from electrolytic cell to battery are complex and not fully *** this article,we focus on the electrochemical processes of Se in aqueous solutions,molten salts and ionic liquid electrolytes,as well as the application of Se-containing materials in energy ***,the electrochemical behaviors of Se-containing species in different systems are comprehensively summarized to understand the complexity of the kinetic processes and guide the Se ***,the relationship between the deposition conditions and resulting structure and morphology of electrodeposited Se is discussed,so as to regulate the morphology and composition of the ***,the advanced energy storage applications of Se in thin-film solar cells and secondary batteries are reviewed,and the electrochemical reaction processes of Se are systematically comprehended in monovalent and multivalent metal-ion *** on understanding the fundamental electrochemistry mechanism,the future development directions of Se-containing materials are considered in view of the in-depth review of reaction kinetics and energy storage applications.

关键词： electrochemical behaviors electrodeposition electrolytes energy storage selenium

An efficient molten-salt electro-deoxidation strategy enabling fast-kinetics and long-life aluminum-selenium batteries

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SusMat 2024年第1期4卷 126-139页

作者： jiguo tu Zheng Huang Cheng Chang Haiping Lei Shuai Wang Shuqiang Jiao State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijingChina School of Chemistry Chemical Engineering and BiotechnologyNanyang Technological UniversitySingaporeSingapore School of Metallurgical and Ecological Engineering University of Science and Technology BeijingBeijingChina School of Electrical and Electronic Engineering Nanyang Technological UniversitySingaporeSingapore

Aluminum-selenium(Al-Se)batteries have been considered as one of the most promising energy storage systems owing to their high capacity,energy density,and cost effectiveness,but Se falls challenges in addressing the shuttle effect of soluble intermediate product and sluggish reaction kinetics in the solid-solid conversion process during ***,we propose an unprecedented design concept for fabricating uniform Se/C hollow microspheres with controllable morphologies through low-temperature electro-deoxidation in neutral NaCl-AlCl_(3) molten salt *** Se/C hollow microspheres are demonstrated to hold a favorable hollow structure for hosting Se,which can not only suppress the dissolution of soluble intermediate products into the electrolyte,thereby maintaining the structural integrity and maximizing Se utilization of the active material,but also promote the electrical/ionic conductivity,thus facilitating the rapid reaction kinetics during ***,the as-prepared Se/C hollow microspheres exhibit a high reversible capacity of 720.1 mAh g^(−1)at 500 mA g^(−1).Even at the high current density of 1000 mA g^(−1),Se/C delivers a high discharge capacity of 564.0 mAh g^(−1),long-term stability over 1100 cycles and high Coulombic efficiency of 98.6%.This present work provides valuable insights into short-process recovery of advanced Se-containingmaterials and value-added utilization for energy storage.

关键词： aluminum-ion batteries hollow Se/C microspheres long-term cycling stability lowtemperature electro-deoxidation NaCl-AlCl_(3)molten salt

镀锌废酸液溶剂萃取分离与资源化回收锌铁的研究进展

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中国有色金属学报 2024年第7期34卷 2383-2398页

作者：冯鑫初国君汪涵石晓磊涂继国北京科技大学绿色低碳钢铁冶金全国重点实验室北京100083 吉林华信新型结构科技有限公司吉林132300 北京科技大学绿色低碳冶炼与资源综合利用联合实验室北京100083

镀锌废酸液含有高浓度亚铁盐、锌盐和残余酸,同时具有酸性强、腐蚀性强以及不易处理等特点。若对镀锌废酸液不能进行有效处理并直接排放,将对周围环境造成显著破坏,并导致严重的资源浪费。溶剂萃取法是一种极具应用潜力的镀锌废酸液处... 详细信息

镀锌废酸液含有高浓度亚铁盐、锌盐和残余酸,同时具有酸性强、腐蚀性强以及不易处理等特点。若对镀锌废酸液不能进行有效处理并直接排放,将对周围环境造成显著破坏,并导致严重的资源浪费。溶剂萃取法是一种极具应用潜力的镀锌废酸液处理方法,具有高选择性、多功能性和产品纯度高的特点,特别是在处理含锌离子废液方面具有显著优势。本文全面总结了不同酸碱萃取剂条件下处理镀锌废酸液的萃取机理及影响因素,并对镀锌废酸液中高附加值成分的回收进行了系统阐述。此外,总结了溶剂萃取法资源化回收镀锌废酸液的发展现状,并展望了锌、铁高效分离与回收的未来研究方向,为相关技术产业化提供重要的理论依据,并促进镀锌废酸液的可持续处理与资源化利用。

关键词：镀锌废酸溶剂萃取萃取机制锌铁分离高值产品回收

Hierarchical N-doped porous carbon hosts for stabilizing tellurium in promoting Al-Te batteries

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Journal of Energy Chemistry 2021年第6期30卷 378-385,I0009页

作者： Xuefeng Zhang Mingyong Wang jiguo tu Shuqiang Jiao State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China

Aluminum batteries are attractive in electrochemical energy storage due to high energy density and lowcost aluminum,while the energy density is limited for the lack of favorable positive electrode materials to match aluminum negative *** positive electrode is intrinsically electrically conductive among chalcogen and holds high theoretical specific capacity(1260.27 mAh g^(-1)) and discharge voltage plateau(~1,5 V).However,the chemical and electrochemical dissolution of Te active materials results in the low material utilization and poor cycling *** enhance the electrochemical performance,herein a nitrogen doped porous carbon(N-PC) is derived from zeolite imidazolate framework(ZIF-67)as an effective tellurium host to suppress the undesired shuttle *** order to inhibit the volume expansion of N-PC during the charge/discharge process,the reduced graphene oxide(rGO) nanosheets are introduced to form a stable host materials(N-PC-rGO) for stabilizing *** physical encapsulation and chemical confinement to soluble tellurium species are achieved.N-PC-rGO-Te positive electrode exhibits an improved initial specific capacity and long-term cycling performance at a current density of 500 mA g^(-1)(initial specific capacity:935.5 mAh g^(-1);after 150 cycles:467.5 mAh g^(-1)), highlighting a promising design strategy for inhibiting chemical and electrochemical dissolution of Te.

关键词： Porous carbon Tellurium Positive electrode Aluminum-ion battery Chalcogen

3D skeleton nanostructured Ni_3S_2/Ni foam@RGO composite anode for high-performance dual-ion battery

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Journal of Energy Chemistry 2019年第1期28卷 144-150页

作者： Shuai Wang jiguo tu Jiusan Xiao Jun Zhu Shuqiang Jiao State Key Laboratory of Advanced Metallurgy University of Science and Technology Beijing

The growing global demands of safe, low-cost and high working voltage energy storage devices trigger strong interests in novel battery concepts beyond state-of-art lithium-ion battery. Herein, a dualion battery based on nanostructured Ni_3S_2/Ni foam@RGO(NSNR) composite anode is developed, utilizing graphite as cathode material and LiPF6-VC-based solvent as electrolyte. The battery operates at high working voltage of 4.2–4.5 V, with superior discharge capacity of ～90 m A h g^(-1) at 100 mA g^(-1), outstanding rate performance, and long-term cycling stability over 500 cycles with discharge capacity retention of ～85.6%. Moreover, the composite simultaneously acts as the anode material and the current collector, and the corrosion phenomenon can be greatly reduced compared to metallic Al anode. Thus, this work represents a significant step forward for practical safe, low-cost and high working voltage dual-ion batteries,showing attractive potential for future energy storage application.

关键词： Dual-ion battery Nanostructured Ni3S2/Ni foam@RGO composite High working voltage Long-term cycling

MOF-based quasi-solid-state electrolyte for long-life Al-Se battery

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Journal of Energy Chemistry 2023年第11期86卷 237-245,I0006页

作者： Haiping Lei jiguo tu Suqin Li Jiacheng Wang Zheng Huang Zhijing Yu Shuqiang Jiao State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China School of Metallurgical and Ecological Engineering University of Science and Technology BeijingBeijing 100083China

Aluminum-selenium(Al-Se)batteries,which possess a high theoretical specific capacity of 1357 mA h g^(-1),represent a promising energy storage ***,they suffer from significant attenuation of capacity and low cycle life due to the shuttle *** mitigate the shuttle effect induced by soluble selenium chloroaluminate compound that tends to migrate towards the negative electrode,a quasi-solid-state Al-Se battery was fabricated through the synthesis of a multi-aperture structure quasisolid-state electrolyte(MOF@GPE)based on metal-organic framework(MOF)material and gel-polymer electrolyte(GPE).The high ionic conductivity(1.13×10^(-3)S cm^(-1))of MOF@GPE at room temperature,coupled with its wide electrochemical stability window(2.45 V),can facilitate ion transport kinetics and enhance the electrochemical performance of Al-Se *** MOF@GPE-based quasi-solidstate Al-Se batteries exhibit outstanding long-life cycling stability,delivering a high specific discharge capacity of 548 mA h g^(-1)with a maintained discharge specific capacity of 345 mA h g^(-1)after 500 cycles at a current density of 200 mA g^(-1).The stable ion transmission and high ion transport kinetics in MOF@GPE can be attributed to the stable structure and permeable channel of MOF,which effectively captures the soluble selenium chloroaluminate compound and further restrains the shuttle effect,resulting in improved cycling performance.

关键词： Aluminum selenium batteries MOF Quasi-solid-state electrolyte Shuttle effect Transport kinetics

Al homogeneous deposition induced by N-containing functional groups for enhanced cycling stability of Al-ion battery negative electrode

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Nano Research 2021年第3期14卷 646-653页

作者： Handong Jiao Shuqiang Jiao Wei-Li Song Xiang Xiao Dongmei She Na Li Haosen Chen jiguo tu Mingyong Wang Daining Fang Institute of Advanced Structure Technology Beijing Institute of TechnologyBeijing100081China State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing100083China

Rechargeable Al-ion batteries(AIBs)are considered as one of the most fascinating energy storage systems due to abundant Al resource and low ***,the cycling stability is subjected to critical problems for using Al foil as negative electrode,including Al dendrites,corrosion and *** addressing these problems,here a lightweight self-supporting N-doped carbon rod array(NCRA)is demonstrated for a long-life negative electrode in *** analysis and first-principle calculations reveal the storage mechanism involving the induced deposition of N-containing function groups to Al as well as the ideal skeleton of the NCRA matrix for Al plating/stripping,which is favorable for regulating Al nucleation and suppressing dendrites *** with the Al foil,the NCRA exhibits lower areal mass density(∼72%of Al foil),smaller thickness(40%of Al foil),but much longer cycle life(>4 times of Al foil).Benefiting from the remarkable stability of the array structure,symmetric cells show excellent cycling stability with small voltage hysteresis(∼80 mV)and meanwhile there are no corrosion and pulverization problems even after cycled for 120 ***,full cells also manifest long lifespan(1,500 cycles)and increased Coulombic efficiency(100±1%).

关键词： Al-ion batteries Al homogeneous deposition negative electrode lightweight long cycle life

表面活性剂PEG6000对二元络合体系化学沉积铜的影响

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材料研究学报 2019年第9期33卷 666-672页

作者：卢建红邓小梅阎建辉涂继国王明涌焦树强北京科技大学钢铁冶金新技术国家重点实验室北京100083 北京化工大学常州先进材料研究院常州213164 湖南理工学院化学化工学院岳阳414006

研究了表面活性剂聚乙二醇6000对乙二胺四乙酸(EDTA)/四羟丙基乙二胺(THPED)二元络合体系化学镀铜的过程和化学镀铜表面结构的影响。混合电位-时间测试结果表明,化学沉积过程分为三个区:诱发区、过渡区和稳定区。PEG6000使体系的混合电... 详细信息

研究了表面活性剂聚乙二醇6000对乙二胺四乙酸(EDTA)/四羟丙基乙二胺(THPED)二元络合体系化学镀铜的过程和化学镀铜表面结构的影响。混合电位-时间测试结果表明,化学沉积过程分为三个区:诱发区、过渡区和稳定区。PEG6000使体系的混合电位负移趋势放缓,与表面活性剂在铜表面的吸附阻滞了对带电荷离子的吸附有关。线性扫描测试结果表明,阴极还原反应为控制步骤,PEG6000的吸附减缓了阴极还原反应,还原峰电流密度下降了约40%;铜化学沉积速率随着PEG6000浓度的提高呈线性下降趋势。SEM、EDS和XRD表征结果表明,化学镀铜的纯度较高,加入PEG6000使镀层呈现出明显的(220)晶面择优取向,且晶粒尺寸由77.7 nm减小到50.0 nm,有细化晶粒的作用。

关键词：材料表面与界面化学镀铜表面活性剂聚乙二醇6000 混合电位晶面择优取向

2,2′-联吡啶对化学铜二元络合剂体系沉积过程的影响

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材料导报 2020年第S2期34卷 539-542,548页

二元络合剂化学镀铜体系相较于一元络合体系,因增大了对沉积反应的调控空间而备受关注,稳定剂是二元体系的重要组分之一,当前关于稳定剂在二元络合体系中的作用规律系统性研究较少。本研究以2,2′-联吡啶为乙二胺四乙酸(EDTA)/四羟丙基... 详细信息

二元络合剂化学镀铜体系相较于一元络合体系,因增大了对沉积反应的调控空间而备受关注,稳定剂是二元体系的重要组分之一,当前关于稳定剂在二元络合体系中的作用规律系统性研究较少。本研究以2,2′-联吡啶为乙二胺四乙酸(EDTA)/四羟丙基乙二胺(THPED)化学镀铜二元络合体系为稳定剂,测试了体系的电化学特征和镀层结构的变化规律。基于活性离子的吸附差异,化学镀铜的二元络合体系混合电位分为诱导、过渡和稳定三个反应过程,发现2,2′-联吡啶使体系的混合电位值负向移动的趋势放缓。线性伏安法扫描数据表明,由于2,2′-联吡啶在反应电极表面的吸附,减缓了铜络离子的阴极还原反应,还原峰电流密度下降了34.3%,沉积反应受阴极还原步骤控制;镀层的沉积速率随2,2′-联吡啶浓度增加显著下降,同时由于强络合作用抑制了Cu+氧化,起到了稳定镀液的作用。通过SEM、EDS和XRD揭示,加入了2,2′-联吡啶后二元体系所制备的化学镀层呈均匀致密的菱形颗粒状,晶界面清晰分明,具有较高的纯度,以及明显的(220)晶面择优取向趋势,这与2,2′-联吡啶定向吸附在(111)、(200)生成方向抑制这二类晶面的生长,而在(220)生长方向吸附微弱从而抑制较少有关。

关键词： 2,2′-联吡啶化学镀铜混合电位晶面择优取向定向吸附