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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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Metal-organic framework-derive d carbon-base d composites for electromagnetic wave absorption:Dimension design and morphology regulation

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Journal of materials Science & Technology 2023年第1期132卷 223-251页

作者： Yujie Ren Xin Wang jiaxin ma Qi Zheng Lianjun Wang Wan Jiang State Key Laboratory for Modification of Chemical Fibers and Polymer materials and College of materials Science and Engineering Donghua UniversityShanghai 201620China Institute of Functional materials Donghua UniversityShanghai 201620China Engineering Research Center of Advanced Glasses manufacturing Technology Ministry of EducationDonghua UniversityShanghai 201620China

Developing highly efficient microwave absorbing materials(maMs)to ameliorate the electromagnetic(EM)response and facilitate energy absorption is crucial in both the civil and military industries.Metal-organic framework(MOF)derived nanoporous carbon composites have emerged as advanced maMs ow-ing to their rich porosity,tunable compositions,facile functionalization,and morphology diversity.To-gether with the flourishing development of composition-tuning strategy,the rational dimension design and elaborate control over the architectures have also evolved into an effective approach to regulating their EM properties.Herein,we provide a comprehensive review of the recent advances in using di-mension and morphology modulation to adjust the microwave attenuation capacities for MOF-derived carbon composites.The underlying design rules and unique advantages for the maMs of various dimen-sions were discussed with the selection of representative work,providing general concepts and insight on how to efficiently tune the morphologies.Accordingly,the fundamental dimension-morphology-function relationship was also elucidated.Finally,the challenges and perspectives of dimension design and mor-phology control over MOF-derived maMs were also presented.

关键词： MOF-derived carbon composites Electromagnetic microwave absorption Dimension design Morphology regulation

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Kinetic regulation of MXene with water-in-LiCl electrolyte for high-voltage micro-supercapacitors

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National Science Review 2022年第7期9卷 97-105页

作者： Yuanyuan Zhu Shuanghao Zheng Pengfei Lu jiaxin ma Pratteek Das Feng Su Hui-Ming Cheng Zhong-Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian National Laboratory for Clean Energy Chinese Academy of Sciences University of Chinese Academy of Sciences Shenyang National Laboratory for materials Science Institute of Metal Research Chinese Academy of Sciences Faculty of materials Science and Engineering/Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced TechnologyChinese Academy of Sciences Shenzhen International Graduate School Tsinghua University

MXenes are one of the key materials for micro-super capacitors(MSCs),integrating miniaturized energy-storage components with microelectronics.However,the energy densities of MSCs are greatly hampered by MXenes’ narrow working potential window(typically≤0.6 V) in aqueous ele ctrolytes.Here,we report the fabrication of high-voltage MXene-MSCs through the efficient regulation of reaction kinetics in 2 D Ti3C2TxMXene microelectrodes using a water-in-LiCl(WIL,20 m LiCl) salt gel electrolyte.Importantly,the intrinsic energy-storage mechanism of MXene microelectrodes in WIL,which is totally different from traditional electrolytes(1 m LiCl),was revealed through in situ and ex situ characterizations.We validated that the suppression of MXene oxidation at high anodic potential occurred due to the high content of WIL regulating anion intercalation in MXene electrodes,which effectively broadened the voltage window of MXene-MSCs.Remarkably,the symmetric planar MXene-MSCs presented a record operating voltage of 1.6 V,resulting in an exceptionally high volumetric energy density of 31.7 mWh cm-3.With the ultra-high ionic conductivity(69.5 mS cm-1) and ultralow freezing point(-57℃) of the WIL gel electrolyte, our MSCs could be operated in a wide temperature range of-40 to 60℃,and worked for a long duration even at-40℃,demonstrative of its practicality in extreme environments.

关键词： MXene micro-supercapacitors water-in-LiCl aqueous high voltage wide temperature

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In Situ Fabrication of Superfine Perovskite Composite Nanofibers with Ultrahigh Stability by One‑Step Electrospinning Toward White Light‑Emitting Diode

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Advanced Fiber materials 2023年第1期5卷 183-197页

作者： Xiaobo Hu Yanqiao Xu Jiancheng Wang jiaxin ma Lianjun Wang Wan Jiang State Key Laboratory for Modification of Chemical Fibers and Polymer materials and College of materials Science and Engineering Donghua UniversityShanghai 201620People’s Republic of China Engineering Research Center of Advanced Glasses manufacturing Technology Ministry of EducationDonghua UniversityShanghai 201620People’s Republic of China National Engineering Research Center for Domestic and Building Ceramics Jingdezhen Ceramic UniversityJingdezhen 333000China

All-inorganic CsPbX_(3)(X=Cl,Br,I)perovskite nanocrystals(NCs)are emerging as promising candidate materials for optoelectronic devices due to their splendid optical and electrical properties.However,the intrinsic instability greatly limits their practical application.Herein,a feasible strategy is proposed for fabricating highly stable and luminescent CsPbBr_(3)@PVDF-HFP/PS nanofibers by combining one-step electrospinning method with 1H,1H,2H,2H-perfluorodecyltrimethoxysi-lane(PFDTMS)-assisted post-treatment.The bright-emitting CsPbBr_(3) NCs can be effectively encapsulated within polymer nanofibers,which exhibit ultrafine diameter of only 88.1±2.8 nm and high photoluminescence quantum yield(PLQY)of 87.9%via rationally optimizing the electrospinning parameters,concentration of perovskite precursors and ligands.Most importantly,the superhydrophobic surface structures of nanofibers are formed by the hydrolysis and condensation of PFDTMS under moist environment.Benefiting from the double effective protection of polymer matrices and hydrophobic PFDTMS oligomers against moisture erosion,the CsPbBr_(3)@PVDF-HFP/PS nanofibers present an obviously improved stability,which can retain 90%initial PL intensity after water immersion for 70 days.Furthermore,an efficient white light-emitting diode with wide color gamut covering 117%of National Television System Committee(NTSC)standard is successfully fabricated based on the composite nanofiber membranes,suggesting their promising prospect for solid-state lighting and display applications.

关键词： Perovskite nanocrystals Nanofibers Electrospinning Optical properties Stability

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Addressing the Chengjiang conundrum: A palaeoecological view on the rarity of hurdiid radiodonts in this most diverse early Cambrian Lagerstatte

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Geoscience Frontiers 2022年第6期13卷 1-15页

作者： Yu Wu Stephen Pates jiaxin ma Weiliang Lin Yuheng Wu Xingliang Zhang Dongjing Fu State Key Laboratory of Continental Dynamics Shaanxi Key Laboratory of Early Life and Environmentsand Department of GeologyNorthwest UniversityXi’an 710069China Department of Zoology University of CambridgeDowning StreetCambridge CB23EJUnited Kingdom

Over one hundred arthropod fossil species have been described from the famous Chengjiang Lagerst?tte(South China, Cambrian Stage 3, ca. 518 ma) including a diverse assemblage of radiodonts–a group containing Anomalocaris and its relatives. These iconic stem-group euarthropods include some of the largest animals of the time, and some are known from hundreds of specimens. A longstanding conundrum has been the rarity or absence of hurdiids from Cambrian Series 2 Lagerst?tten like Chengjiang. This is because radiodonts are generally common in such deposits and the oldest radiodont ever discovered is a hurdiid. Furthermore, this family displays the widest geographic and temporal ranges of all radiodont families, and the highest diversity. Here we document the first hurdiid frontal appendages from Chengjiang, which display unique features within the family and may provide insights for understanding the character evolution of hurdiid appendages. The palaeoenvironmental distribution of hurdiids suggests that the rarity of hurdiids in Chengjiang may be due to a preference for deeper water environments,and the later success of this family from the Wuliuan onwards may relate to their ability to tolerate cooler water temperatures than other radiodont families. The palaeogeographical, palaeoenvironmental, and stratigraphical patterns observed in hurdiids maybe caused in part by the limited distributions of Konservat-Lagerst?tten in the Cambrian as well.

关键词： Radiodonta Hurdiidae Panarthropoda Palaeobiogeography Palaeoenvironment Chengjiang Lagerstatte

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Advancing MXene-based integrated microsystems with microsupercapacitors and/or sensors:Rational design,key progress,and challenging perspectives

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Journal of materiomics 2023年第6期9卷 1242-1262页

作者： Jin Jia Yuanyuan Zhu Pratteek Das jiaxin ma Sen Wang Guang Zhu Zhong-Shuai Wu Key Laboratory of Spin Electron and Nanomaterials of Anhui Higher Education Institutes Suzhou UniversitySuzhou 234000China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Shijingshan DistrictBeijing 100049China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023China

The escalating demand for micro/nano-sized devices,such as micro/nano-robots,intelligent portable/wearable microsystems,and implantable medical microdevices,necessitates the expeditious development of integrated microsystems incorporating energy conversion,storage,and consumption.Critical bottlenecks in microscale energy storage/sensors and their integrated systems are being addressed by exploring new technologies and new materials,e.g.,MXene,holding great potential for developing lightweight and deformable integrated microdevices.This review summarizes the latest progress and milestones in the realization of MXene-based micro-supercapacitors(MSCs)and sensor arrays,and thus discusses the design fundamentals and key advancements of MXene-based energy conversion-storageconsumption integrated microsystems.Finally,we outline the key challenges in fabricating MXenebased MSCs/sensors and their self-powered integrated microsystems,which is crucial for their practical applications.Particularly,we illuminate viable solutions to such unsolved issues and highlight the exciting opportunities.

关键词： MXene Micro-supercapacitors Sensors Self-powered Integrated microsystem

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High-Performance and Flexible Co-Planar Integrated Microsystem of Carbon-Based All-Solid-State Micro-Supercapacitor and Real-Time Temperature Sensor

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Energy & Environmental materials 2023年第6期6卷 291-296页

作者： Dongming Liu jiaxin ma Shuanghao Zheng Wenlong Shao Tianpeng Zhang Siyang Liu Xigao Jian Zhongshuai Wu Fangyuan Hu School of materials Science and Engineering State Key Laboratory of Fine ChemicalsSchool of Polymer MaterialsDalian University of TechnologyDalian 116024China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023China

With the rapid development of flexible and portable microelectronics,the extreme demand for miniaturized,mechanically flexible,and integrated microsystems are strongly stimulated.Here,biomass-derived carbons(BDCs)are prepared by KOH activation using Qamgur precursor,exhibiting three-dimensional(3D)hierarchical porous structure.Benefiting from unobstructed 3D hierarchical porous structure,BDCs provide an excellent specific capacitance of 433 F g^(-1)and prominent cyclability without capacitance degradation after 50000 cycles at 50 A g^(-1).Furthermore,BDC-based planar micro-supercapacitors(MSCs)without metal collector,prepared by mask-assisted coating,exhibit outstanding areal-specific capacitance of 84 mF cm^(-2)and areal energy density of 10.6μWh cm^(-2),exceeding most of the previous carbon-based MSCs.Impressively,the MSCs disclose extraordinary flexibility with capacitance retention of almost 100%under extreme bending state.More importantly,a flexible planar integrated system composed of the MSC and temperature sensor is assembled to efficiently monitor the temperature variation,providing a feasible route for flexible MSC-based functional micro-devices.

关键词： 3D hierarchical porous carbon biomass-derived carbon integrated microsystem micro-supercapacitors temperature sensor

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Assembly of N-and P-functionalized carbon nanostructures derived from precursor-defined ternary copolymers for high-capacity lithiumion batteries

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Chinese Journal of Chemical Engineering 2023年第1期53卷 280-288页

作者： Luyao Guo Mengru Wang Ronghe Lin jiaxin ma Shuanghao Zheng Xiaoling Mou Jun Zhang Zhong-Shuai Wu Yunjie Ding Hangzhou Institute of Advanced Studies Zhejiang Normal UniversityHangzhou 311231China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Yuquan Road 19AShijingshan DistrictBeijing 100049China College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesZhongshan Road 457Dalian 116023China

Synthesis of new carbon nanostructures with tunable properties is vital for precisely regulating electrochemical performance in the wide applications.Herein,we report a novel approach for the oxidative polymerization of N-and P-bearing copolymers from the self-assembly of three different monomers(aniline,pyrrole,and phytic acid),and further prepare the respective carbon nanostructures with relatively consistent N dopant(6.2%–8.0%,atom)and varying P concentrations(0.4%–2.8%,atom)via controllable pyrolysis.The impacts of phytic acid addition on the compositional,structural,and morphological evolution of the copolymers and the resulting nanocarbons are well studied through a spectrum of characterizations including N2 sorption,Fourier transform infrared spectroscopy,gel permeation chromatograph,scanning/transmission electron microscopy,and X-ray photoelectron spectroscopy.Gradual fragmentation of the nanosphere structures is evidenced with increasing addition of phytic acid,leading to different nanostructures from hollow nanospheres to 3D aggregates.Nanocarbons decorated with N and P dopants from pyrolysis are further utilized as anode materials in lithium-ion batteries,demonstrating enhanced electrochemical performance,i.e.,a reversible capacity of 380 mahg^(-1)at 2 Ag^(-1)for NPC-0.5 during 200 cycles.The superior performance originates from the balanced porosity,and appropriate concentrations of P and pyrrolic N,thus pointing the direction for designing high-performance anode materials.

关键词： Carbon nanospheres Doping Lithium-ion batteries Polymers Porosity

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Monolithic integrated micro-supercapacitors with ultra-high systemic volumetric performance and areal output voltage

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National Science Review 2023年第3期10卷 169-177页

作者： Sen Wang Linmei Li Shuanghao Zheng Pratteek Das Xiaoyu Shi jiaxin ma Yu Liu Yuanyuan Zhu Yao Lu Zhong-Shuai Wu Hui-Ming Cheng State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Department of Biotechnology Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian National Laboratory for Clean Energy Chinese Academy of Sciences University of Chinese Academy of Sciences Faculty of materials Science and Engineering Institute of Technology for Carbon NeutralityShenzhen Institute of Advanced TechnologyChinese Academy of Sciences Shenyang National Laboratory for materials Science Institute of Metal Research Chinese Academy of Sciences Advanced Technology Institute University of Surrey

Monolithic integrated micro-supercapacitors(MIMSCs) with high systemic performance and cell-number density are important for miniaturized electronics to empower the Internet of Things.However,fabrication of customizable MIMSCs in an extremely small space remains a huge challenge considering key factors such as materials selection,electrolyte confinement,microfabrication and device-performance uniformity.Here,we develop a universal and large-throughput microfabrication strategy to address all these issues by combining multistep lithographic patterning,spray printing of MXene micro electrodes and controllable 3D printing of gel electrolytes.We achieve the monolithic integration of electrochemically isolated micro-supercapacitors in close proximity by leveraging high-resolution micropatterning techniques for micro electrode deposition and 3D printing for precise electrolyte deposition.Notably,the MIMSCs obtained demonstrate a high areal-number density of 28 cells cm-2(340 cells on 3.5 × 3.5 cm2),a record areal output voltage of 75.6 V cm-2,an acceptable systemic volumetric energy density of 9.8 mWh cm-3and an unprecedentedly high capacitance retention of 92% after 4000 cycles at an extremely high output voltage of 162 V.This work paves the way for monolithic integrated and microscopic energy-storage assemblies for powering future microele ctronics.

关键词： monolithic integrated micro-supercapacitors areal output voltage lithography MXene

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