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2.4 V ultrahigh-voltage aqueous MXene-based asymmetric micro-supercapacitors with high volumetric energy density toward a self-sufficient integrated microsystem

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Fundamental Research 2024年第2期4卷 307-314页

作者： Yuanyuan Zhu Shuanghao Zheng jieqiong qin Jiaxin Ma Pratteek Das Feng Zhou Zhong-Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Shijingshan DistrictBeijing 100049China College of Science Henan Agricultural UniversityZhengzhou 450002China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023China Key Laboratory of Spin Electron and Nanomaterials of Anhui Higher Education Institutes Suzhou UniversitySuzhou 234000China

Two-dimensional MXenes are key high-capacitance electrode materials for micro-supercapacitors(MSCs)catering to integrated microsystems.However,the narrow electrochemical voltage windows of conventional aqueous electrolytes(≤1.23 V)and symmetric MXene MSCs(typically≤0.6 V)substantially limit their output voltage and energy density.Highly concentrated aqueous electrolytes exhibit lower water molecule activity,which inhibits water splitting and consequently widens the operating voltage window.Herein,we report ultrahigh-voltage aqueous planar asymmetric MSCs(AMSCs)based on a highly concentrated LiCl-gel quasi-solid-state electrolyte with MXene(Ti3C2Tx)as the negative electrode and MnO_(2) nanosheets as the positive electrode(MXene//MnO_(2)-AMSCs).The MXene//MnO_(2)-AMSCs exhibit a high voltage of up to 2.4 V,attaining an ultrahigh volumetric energy density of 53 mWh cm−3.Furthermore,the in-plane geometry and the quasi-solid-state electrolyte enabled excellent mechanical flexibility and performance uniformity in the serially/parallel connected packs of our AMSCs.Notably,the MXene//MnO_(2)-AMSC-based integrated microsystem,in conjunction with solar cells and consumer electronics,could efficiently realize simultaneous energy harvesting,storage,and conversion.The findings of this study provide insights for constructing high-voltage aqueous MXene-based AMSCs as safe and self-sufficient micropower sources in smart integrated microsystems.

关键词： Asymmetric micro-supercapacitors MXene MnO_(2) Aqueous electrolyte High voltage Integrated microsystem

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Hierarchically Structured Nb_(2)O_5 Microflowers with Enhanced Capacity and Fast-Charging Capability for Flexible Planar Sodium Ion Micro-Supercapacitors

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Nano-Micro Letters 2024年第4期16卷 97-109页

作者： Jiaxin Ma jieqiong qin Shuanghao Zheng Yinghua Fu Liping Chi Yaguang Li Cong Dong Bin Li Feifei Xing Haodong Shi Zhong‑Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences457 Zhongshan RoadDalian 116023People’s Republic of China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001People’s Republic of China College of Science Henan Agricultural UniversityNo.63 Agricultural RoadZhengzhou 450002People’s Republic of China Dalian National Laboratory for Clean Energy Chinese Academy of Sciences457 Zhongshan RoadDalian 116023People’s Republic of China University of Chinese Academy of Sciences 19A Yuquan RoadShijingshan DistrictBeijing 100049People’s Republic of China Hebei Key Lab of Optic‑Electronic Information and Materials The College of Physics Science and TechnologyInstitute of Life Science and Green DevelopmentHebei UniversityBaoding 071002People’s Republic of China

Planar Na ion micro-supercapacitors(NIMSCs) that offer both high energy density and power density are deemed to a promising class of miniaturized power sources for wearable and portable microelectron-ics. Nevertheless, the development of NIMSCs are hugely impeded by the low capacity and sluggish Na ion kinetics in the negative electrode.Herein, we demonstrate a novel carbon-coated Nb_(2)O_5 microflower with a hierarchical structure composed of vertically intercrossed and porous nanosheets, boosting Na ion storage performance. The unique structural merits, including uniform carbon coating, ultrathin nanosheets and abun-dant pores, endow the Nb_(2)O_5 microflower with highly reversible Na ion storage capacity of 245 mAh g^(-1) at 0.25 C and excellent rate capability.Benefiting from high capacity and fast charging of Nb_(2)O_5 microflower, the planar NIMSCs consisted of Nb_(2)O_5 negative electrode and activated car-bon positive electrode deliver high areal energy density of 60.7 μWh cm^(-2),considerable voltage window of 3.5 V and extraordinary cyclability. Therefore, this work exploits a structural design strategy towards electrode materials for application in NIMSCs, holding great promise for flexible microelectronics.

关键词： Nb_(2)O_5 nanosheets Microflowers Sodium ion micro-supercapacitors Flexibility Energy storage

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Recent advances and key opportunities on in-plane micro-supercapacitors:From functional microdevices to smart integrated microsystems

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Journal of Energy Chemistry 2023年第6期81卷 410-431,I0010页

作者： jieqiong qin Hongtao Zhang Zhi Yang Xiao Wang Pratteek Das Feng Zhou Zhong-Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina College of Science Henan Agricultural UniversityZhengzhou 450002HenanChina Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023LiaoningChina

The popularization of portable,implantable and wearable microelectronics has greatly stimulated the rapid development of high-power planar micro-supercapacitors(PMSCs).Particularly,the introduction of new functionalities(e.g.,high voltage,flexibility,stretchability,self-healing,electrochromism and photo/thermal response)to PMSCs is essential for building multifunctional PMSCs and their smart selfpowered integrated microsystems.In this review,we summarized the latest advances in PMSCs from various functional microdevices to their smart integrated microsystems.Primarily,the functionalities of PMSCs are characterized by three major factors to emphasize their electrochemical behavior and unique scope of application.These include but are not limited to high-voltage outputs(realized through asymmetric configuration,novel electrolyte and modular integration),mechanical resilience that includes various feats of flexibility or stretchability,and response to stimuli(self-healing,electrochromic,photo-responsive,or thermal-responsive properties).Furthermore,three representative integrated microsystems including energy harvester-PMSC,PMSC-energy consumption,and all-in-one selfpowered microsystems are elaborately overviewed to understand the emerging intelligent interaction models.Finally,the key perspectives,challenges and opportunities of PMSCs for powering smart microelectronics are proposed in brief.

关键词： Micro-supercapacitors In-plane Functionalization Integrated microsystem Energy storage

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Two‑Dimensional Mesoporous Materials for Energy Storage and Conversion:Current Status,Chemical Synthesis and Challenging Perspectives

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Electrochemical Energy Reviews 2023年第1期6卷 614-650页

作者： jieqiong qin Zhi Yang Feifei Xing Liangzhu Zhang Hongtao Zhang Zhong‑Shuai Wu College of Science Henan Agricultural University63 Agricultural RoadZhengzhou 450002HenanChina State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences457 Zhongshan RoadDalian 116023LiaoningChina University of Chinese Academy of Sciences 19 A Yuquan RoadShijingshan DistrictBeijing 100049China

Two-dimensional(2D)mesoporous materials(2DMMs),defined as 2D nanosheets with randomly dispersed or orderly aligned mesopores of 2–50 nm,can synergistically combine the fascinating merits of 2D materials and mesoporous mate-rials,while overcoming their intrinsic shortcomings,e.g.,easy self-stacking of 2D materials and long ion transport paths in bulk mesoporous materials.These unique features enable fast ion diffusion,large specific surface area,and enriched adsorption/reaction sites,thus offering a promising solution for designing high-performance electrode/catalyst materials for next-generation energy storage and conversion devices(ESCDs).Herein,we review recent advances of state-of-the-art 2DMMs for high-efficiency ESCDs,focusing on two different configurations of in-plane mesoporous nanosheets and sandwich-like mesoporous heterostructures.Firstly,a brief introduction is given to highlighting the structural advantages(e.g.,tailored chemical composition,sheet configuration,and mesopore geometry)and key roles(e.g.,active materials and functional additives)of 2DMMs for high-performance ESCDs.Secondly,the chemical synthesis strategies of 2DMMs are summarized,including template-free,2D-template,mesopore-template,and 2D mesopore dual-template methods.Thirdly,the wide applications of 2DMMs in advanced supercapacitors,rechargeable batteries,and electrocatalysis are discussed,enlightening their intrinsic structure–property relationships.Finally,the future challenges and perspectives of 2DMMs in energy-related fields are presented.

关键词： 2D materials Mesopores Nanosheets Energy storage Energy conversion

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Lignin derived hierarchical porous carbon with extremely suppressed polyselenide shuttling for high-capacity and long-cycle-life lithium-selenium batteries

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Journal of Energy Chemistry 2021年第4期30卷 476-483页

作者： Pengfei Lu Fangyan Liu Feng Zhou jieqiong qin Haodong Shi Zhong-Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Shijingshan DistrictBeijing 100049China

Lithium-selenium(Li-Se)batteries have attracted considerable attentions for next-generation energy storage systems owing to high volumetric capacity of 3265 m Ah cm^(-3) and excellent electronic conductivity(~10^(-5)S cm^(-1))of selenium.However,the shuttling effect and capacity fading prevent their wide applications.Herein we report a low-cost strategy for scalable fabrication of lignin derived hierarchical porous carbon(LHPC)as a new high-loading Se host for high-capacity and long-term cycling Li-Se batteries in carbonate electrolyte.The resulting LHPC exhibits three-dimensional(3D)hierarchically porous structure,high specific surface area of 1696 m^(2) g^(-1),and hetero-atom doping(O,S),which can effectively confine the Se particles into the micropores,and meanwhile,offer effective chemical binding sites for selenides from hetero-atoms(O,S).As a result,our Li-Se batteries based on Se@LHPC demonstrate high capacity of 450 m Ah g^(-1) at 0.5 C after 500 cycles,with a low capacity fading rate of only 0.027%.The theoretical simulation confirmed the strong affinity of selenides on the O and S sites of LHPC effectively mitigating the Se losing.Therefore,our strategy of using lignin as the low-cost precursor of hierarchically porous carbon for high-loading Se host offers new opportunities for high-capacity and long-life Li-Se batteries.

关键词： Lignin Hierarchical porous carbon Lithium selenium battery Long cycling stability Energy storage

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Scalable fabrication of printed Zn//MnO2 planar micro-batteries with high volumetric energy density and exceptional safety

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National Science Review 2020年第1期7卷 64-72页

作者： Xiao Wang Shuanghao Zheng Feng Zhou jieqiong qin Xiaoyu Shi Sen Wang Chenglin Sun Xinhe Bao Zhong-Shuai Wu Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences Department of Chemical Physics University of Science and Technology of China State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences

The rapid development of printed and microscale electronics imminently requires compatible micro-batteries(MBs) with high performance, applicable scalability, and exceptional safety, but faces great challenges from the ever-reported stacked geometry. Herein the first printed planar prototype of aqueous-based, high-safety Zn//MnOMBs, with outstanding performance, aesthetic diversity, flexibility and modularization, is demonstrated, based on interdigital patterns of Zn ink as anode and MnOink as cathode, with high-conducting graphene ink as a metal-free current collector, fabricated by an industrially scalable screen-printing technique. The planar separator-free Zn//MnOMBs, tested in neutral aqueous electrolyte, deliver a high volumetric capacity of 19.3 mAh/cm~3(corresponding to 393 mAh/g) at 7.5 mA/cm~3, and notable volumetric energy density of 17.3 mWh/cm~3, outperforming lithium thin-film batteries(≤10 mWh/cm~3). Furthermore, our Zn//MnOMBs present long-term cyclability having a high capacity retention of 83.9% after 1300 cycles at 5 C, which is superior to stacked Zn//MnObatteries previously reported. Also, Zn//MnOplanar MBs exhibit exceptional flexibility without observable capacity decay under serious deformation, and remarkably serial and parallel integration of constructing bipolar cells with high voltage and capacity output. Therefore, low-cost, environmentally benign Zn//MnOMBs with in-plane geometry possess huge potential as high-energy, safe, scalable and flexible microscale power sources for direction integration with printed electronics.

关键词： low cost printed planar Zn//MnO2 micro-batteries metal-free current collectors

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2D hierarchical yolk-shell heterostructures as advanced host-interlayer integrated electrode for enhanced Li-S batteries

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Journal of Energy Chemistry 2019年第9期28卷 64-73页

作者： Yanfeng Dong Pengfei Lu Haodong Shi jieqiong qin Jian Chen Wencai Ren Hui-Ming Cheng Zhong-Shuai Wu Department of Chemistry College of Sciences Northeastern UniversityShenyang 110819 Liaoning China Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023 Liaoning China University of Chinese Academy of Sciences Beijing 100049 China Shenyang National Laboratory for Materials Science Institute of Metal Research Chinese Academy of Sciences Shenyang 110016 Liaoning China Tsinghua-Berkeley Shenzhen Institute Shenzhen 518055 Guangdong China

Lithium sulfur(Li-S)batteries hold great promising for high-energy-density batteries,but appear rapid capacity fading due to the lack of overall and elaborated design of both sulfur host and interlayer.Herein,we developed a novel two-dimensional(2D)hierarchical yolk-shell heterostructure,constructed by a graphene yolk,2D void and outer shell of vertically aligned carbon-mediated MoS2 nanosheets(G@void@MoS2/C),as advanced host-interlayer integrated electrode for Li-S batteries.Notably,the 2D void,with a typical thickness of^80 nm,provided suitable space for loading and confining nano sulfur,and vertically aligned ultrathin MoS2 nanosheets guaranteed enriched catalytically active sites to effectively promote the transition of soluble polysulfides.The conductive graphene yolk and carbon mediated shell sufficiently accelerated electron transport.Therefore,the integrated electrode of G@void@MoS2/C not only exceptionally confined the sulfur/polysulfides in 2D yolk-shell heterostructures,but also achieved catalytic transition of the residual polysulfides dissolved in electrolyte to solid Li2S2/Li2S,both of which synergistically achieved an extremely low capacity fading rate of 0.05%per cycle over 1000 times at 2C,outperforming most reported Mo based cathodes and interlayers for Li-S batteries.2D hierarchical yolkshell heterostructures developed here may shed new insight on elaborated design of integrated electrodes for Li-S batteries.

关键词： MoS2 Graphene Yolk shell 2D heterostructure Lithium sulfur batteries

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Simplified fabrication of high areal capacitance all-solid-state micro-supercapacitors based on graphene and MnO_2 nanosheets

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Chinese Chemical Letters 2018年第4期29卷 582-586页

作者： jieqiong qin Zhong-Shuai Wu Feng Zhou Yanfeng Dong Han Xiao Shuanghao Zheng Sen Wang Xiaoyu Shi Haibo Huang Chenglin Sun Xinhe Bao Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China University of Chinese Academy of Sciences Beijing 100049 China Department of Chemical Physics University of Science and Technology of China Hefei 230026 China

All-solid-state micro-supercapacitors are acknowledged as a very promising class of microscale energy storage devices for directly integrating portable and wearable electronics. However, the improvement of electrochemical performance from materials to devices still remains tremendous challenges. Here, we demonstrate a novel and universal mask-assisted filtration technology for the simplified fabrication of all-solid-state planar micro-supercapacitors（MSCs） based on interdigital patterns of 2D pseudocapacitive MnO2 nanosheets and electrochemically exfoliated graphene film as both electrode and current collector, and polyvinyl alcohol/Li Cl gel as electrolyte. Remarkably, the resulting MSCs exhibit outstanding areal capacitance of ～355 m F/cm^2, which is among the highest values reported in the state-of-the-art MSCs. Meanwhile, MSCs possess exceptionally mechanical flexibility as high as ～92% of initial capacitance even at a highly bending angle of 180°, excellent cyclability with a capacitance retention of 95% after 3000 cycles, and impressive serial or parallel integration for modulating the voltage or capacitance. Therefore, our proposed strategy of simplified construction of MSCs will pave the ways for utilizing graphene and analogous pseudocapactive nanosheets in high-performance MSCs.

关键词： MnO2 nanosheets Graphene All-solid-state Planar Micro-supercapacitors Energy storage

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农林院校工科类专业大学化学课程的教学改革探索

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化工设计通讯 2024年第5期50卷 81-83,87页

作者：秦洁琼韩丹丹刘国星武晓霞郑昕河南农业大学理学院河南郑州450002

大学化学是高等农林院校工科类专业的基础课程之一,对专业课程的学习起承先启后的作用。针对该专业的学科特点,发现目前存在教学内容与专业的联系少,教学模式与专业适配度低,以及实验环节与理论知识结合度不够等情况。为此,提出重视绪论... 详细信息

大学化学是高等农林院校工科类专业的基础课程之一,对专业课程的学习起承先启后的作用。针对该专业的学科特点,发现目前存在教学内容与专业的联系少,教学模式与专业适配度低,以及实验环节与理论知识结合度不够等情况。为此,提出重视绪论,引入专业相关案例;结合专业,优化教学内容;面向专业,改革教学模式和方法;理论联系实际,加强实验创新等改革策略,以期望提高大学化学课程的教学效果和相关专业学生的综合素养。

关键词：农林院校工科类大学化学现状分析教学改革

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从字用看秦“书同文”的具体规定

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语言科学 2023年第3期22卷 306-316页

作者：李洁琼清华大学出土文献研究与保护中心北京100084

从里耶秦简8-461号木牍摘录的部分“书同文”内容看,秦“书同文”内容丰富而广泛,但无论是传世文献还是出土文献,都没有秦“书同文”完整规定的记录。语言文字的发展如果是自然演化,必然存在新旧共用的阶段,而如果是人为规定,则不会存... 详细信息

从里耶秦简8-461号木牍摘录的部分“书同文”内容看,秦“书同文”内容丰富而广泛,但无论是传世文献还是出土文献,都没有秦“书同文”完整规定的记录。语言文字的发展如果是自然演化,必然存在新旧共用的阶段,而如果是人为规定,则不会存在共用阶段,依据这一规律,可以通过“书同文”前后秦出土文献语言文字的对比,推断“书同文”的未有明确记载的内容。“胃”“谓”分用、“直”“置”分用、“丈”“杖”分用等当属“书同文”规定。

关键词： “书同文” 汉字发展史汉语词汇史用字

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