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Dielectric-ion-conductive ZnNb2O6 layer enabling rapid desolvation and diffusion for dendrite-free Zn metal batteries

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Journal of energy Chemistry 2025年第1期100卷 693-701页

作者： Haifeng Yang Jian Wang Panpan Zhang Xiaomin Cheng Qinghua Guan Jing Dong Bixian Chen Lujie Jia Jing Zhang Yongzheng Zhang Yunjian Liu Hongzhen Lin School of materials Science and engineering Jiangsu University i-lab & CAS key laboratory of Nanophotonic materials and Devices Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences Helmholtz Institute Ulm (HIU) Karlsruhe Institute of Technology (KIT) School of materials Science and engineering Xi'an University of Technology State key laboratory of chemical engineering East China University of Science and Technology

Rechargeable aqueous zinc-metal batteries （AZMBs） are promising candidates for large-scale energy storage systems due to their low cost and high ***,their performance and sustainability are significantly hindered by the sluggish desolvation kinetics at the electrode/electrolyte interface and the corresponding hydrogen evolution reaction where active water molecules tightly participate in the Zn（H2O）62+solvation ***,learnt from self-generated solid electrolyte interphase （SEI） in anodes,the dielectric but ion-conductive zinc niobate nanoparticles artificial layer is constructed on metallic Zn surface （ZNB@Zn）,acting as a rapid desolvation *** zincophilic and dielectric-conductive properties of ZNB layer accelerate interfacial desolvation/diffusion and suppress surface corrosion or dendrite formation,achieving uniform Zn plating/stripping behavior,as confirmed by electronic/optical microscopies and interface spectroscopical measurements together with theoretical ***,the as-prepared ZNB@Zn electrode exhibits excellent cycling stability of over 2000 h and robust reversibility （99.54%） even under high current density and depth of discharge ***,the assembled ZNB@Zn-based full cell displays high capacity-retention rate of 80.21%after 3000 cycles at 5 A g-1and outstanding rate performance up to 10 A *** large-areal pouch cell is stabilized for hundreds of cycles,highlighting the bright prospects of the dielectric but ion-conductive layer in further application of AZMBs.

关键词： Zn metal battery Dielectric artificial layer Rapid ion diffusion Zincophilic diffusion Active water inhibition

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Spontaneous Orientation Polarization of Anisotropic Equivalent Dipoles Harnessed by Entropy engineering for Ultra‑Thin Electromagnetic Wave Absorber

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Nano-Micro Letters 2025年第1期17卷 424-438页

作者： Honghan Wang Xinyu Xiao Shangru Zhai Chuang Xue Guangping Zheng Deqing Zhang Renchao Che Junye Cheng liaoning key lab of Lignocellulose Chemistry and Biomaterials Liaoning Collaborative Innovation Center for Lignocellulosic BiorefinerySchool of Light Industry and Chemical EngineeringDalian Polytechnic UniversityDalian 116034People’s Republic of China School of Life Science and Biotechnology Dalian University of TechnologyDalian 116024People’s Republic of China Department of Mechanical engineering Hong Kong Polytechnic UniversityHung HomKowloonHong Kong 999077People’s Republic of China School of materials Science and engineering Qiqihar UniversityQiqihar 161006People’s Republic of China laboratory of Advanced materials Shanghai Key Lab of Molecular Catalysis and Innovative MaterialsAcademy for Engineering&TechnologyFudan UniversityShanghai 200438People’s Republic of China Department of materials Science Shenzhen MSU-BIT UniversityShenzhen 517182People’s Republic of China

The synthesis of carbon supporter/nanoscale high-entropy alloys(HEAs)electromagnetic response composites by carbothermal shock method has been identified as an advanced strategy for the collaborative competition engineering of conductive/dielectric *** migration modes within HEAs as manipulated by the electronegativity,valence electron configurations and molar proportions of constituent elements determine the steady state and efficiency of equivalent ***,enlightened by skin-like effect,a reformative carbothermal shock method using carbonized cellulose paper(CCP)as carbon supporter is used to preserve the oxygencontaining functional groups(O·)of carbonized cellulose fibers(CCF).Nucleation of HEAs and construction of emblematic shell-core CCF/HEAs heterointerfaces are inextricably linked to carbon metabolism induced by O·.Meanwhile,the electron migration mode of switchable electronrich sites promotes the orientation polarization of anisotropic equivalent *** virtue of the reinforcement strategy,CCP/HEAs composite prepared by 35%molar ratio of Mn element(CCP/HEAs-Mn_(2.15))achieves efficient electromagnetic wave(EMW)absorption of−51.35 dB at an ultra-thin thickness of 1.03 *** mechanisms of the resulting dielectric properties of HEAs-based EMW absorbing materials are elucidated by combining theoretical calculations with experimental characterizations,which provide theoretical bases and feasible strategies for the simulation and practical application of electromagnetic functional devices(e.g.,ultra-wideband bandpass filter).

关键词： High-entropy alloys Carbothermal shock Switchable electron migration modes Emblematic shell-core heterointerfaces Ultra-thin thickness

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Spin-modulated near-infrared-Ⅰ emission in a xanthene-decorated Fe(Ⅱ) spin-crossover complex

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Science China Chemistry 2025年

作者： Cheng Yi Duyong Chen Shihui Zhang Rui Cai Chunying Duan Yinshan Meng Tao Liu State key laboratory of Fine chemicals Frontier Science Center for Smart Materials and Chemical Engineering School of Chemical Engineering Dalian University of Technology Instrumental Analysis Center Dalian University of Technology School of Chemistry Dalian University of Technology liaoning Binhai laboratory

Molecular materials showing synergetic coupling of near-infrared （NIR） fluorescence and spin-crossover （SCO） are promisingly applicable in in-vivo bioimaging,temperature sensing,and spintronic *** the related study faces formidable *** this work we graft the NIR fluorophore xanthene onto the dipyridyl substituted triazole ligand and construct a new Febased SCO material,{FeⅡ（ddxc-abpt）2[N（CN）2]2}(1,ddxc-abpt:（E）-4-(((3,5-di（pyridin-2-yl）-4H-1,2,4-triazol-4-yl)imino)methyl)-N,N-diethyl-2,3-dihydro-1H-xanthen-6-amine).Magnetic studies indicate that compound 1 exhibits thermally induced SCO property in both the solid and solution ***-temperature fluorescence emission spectra reveal a remarkable 7-fold increase in photoluminescence intensity upon the transition from the low-spin state at 110 K to the high-spin state at 280 K,which is the record of all reported coupled fluorescence-SCO ***-temperature ultraviolet-visible （UV-Vis）absorption spectra show a significant change in absorption intensity within the fluorescence emission window,consistent with the F?rster resonance energy transfer （FRET） ***-dependent density functional theory （TD-DFT） calculations demonstrate that the strong coupling is attributed to disrupted energy transfer between the xanthene fluorophore and high-spin *** work provides a feasible approach for expanding the synergetic SCO-fluorescence materials to the NIR-Iwavelength region,and hopefully contributes to the applications of tunable NIR-SCO molecule-based sensors and devices.

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Gradient‑Layered MXene/Hollow Lignin Nanospheres Architecture Design for Flexible and Stretchable Supercapacitors

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Nano-Micro Letters 2025年第2期17卷 447-462页

作者： Haonan Zhang Cheng Hao Tongtong Fu Dian Yu Jane Howe Kaiwen Chen Ning Yan Hao Ren Huamin Zhai Jiangsu Provincial key lab of Sustainable Pulp and Paper Technology and Biomass materials NanJing Forestry UniversityNanjing 210037People’s Republic of China Department of chemical engineering and Applied Chemistry University of Toronto200 College StreetTorontoON M5S 3E5Canada Department of materials Science and engineering University of Toronto184 College StreetTorontoON M5S 3E4Canada College of materials Science and engineering Nanjing Forestry UniversityNanjing 210037People’s Republic of China

With the rapid development of flexible wearable electronics,the demand for stretchable energy storage devices has *** this work,a novel gradient-layered architecture was design based on single-pore hollow lignin nanospheres(HLNPs)-intercalated two-dimensional transition metal carbide(Ti_(3)C_(2)T_(x) MXene)for fabricating highly stretchable and durable *** depositing and inserting HLNPs in the MXene layers with a bottom-up decreasing gradient,a multilayered porous MXene structure with smooth ion channels was constructed by reducing the overstacking of MXene ***,the micro-chamber architecture of thin-walled lignin nanospheres effectively extended the contact area between lignin and MXene to improve ion and electron accessibility,thus better utilizing the pseudocapacitive property of *** these strategies effectively enhanced the capacitive performance of the *** addition,HLNPs,which acted as a protective phase for MXene layer,enhanced mechanical properties of the wrinkled stretchable electrodes by releasing stress through slip and deformation during the stretch-release cycling and greatly improved the structural integrity and capacitive stability of the *** electrodes and symmetric flexible all-solid-state supercapacitors capable of enduring 600%uniaxial tensile strain were developed with high specific capacitances of 1273 mF cm^(−2)(241 F g^(−1))and 514 mF cm^(−2)(95 F g^(−1)),***,their capacitances were well preserved after 1000 times of 600%stretch-release *** study showcased new possibilities of incorporating biobased lignin nanospheres in energy storage devices to fabricate stretchable devices leveraging synergies among various two-dimensional nanomaterials.

关键词： Hollow lignin nanospheres MXene Gradient-layered architecture Wrinkled electrodes Stretchable supercapacitors

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Correlation between self-discharge behavior and heteroatoms over doped carbon sheets for enhanced pseudocapacitance

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Journal of energy Chemistry 2022年第9期31卷 291-298,I0008页

作者： Kunlun Liu Chang Yu Yuanyang Xie Wei Guo Jinhe Yu Lin Ni Zhao Wang Rong Fu Jieshan Qiu State key lab of Fine chemicals School of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina

For electric double layer supercapacitors,carbon materials originating from the purely physical energystorage mechanism limit the improvement in the capabilities of charge *** solve this problem,doping heteroatoms into carbon skeleton is a promising&charming strategy for enhancing electrochemical performance by providing the extra ***,the self-discharge behavior of such heteroatom-doped supercapacitors has been a challenging issue for a long ***,the porous carbon nanosheets with a tunable total content of heteroatoms are chosen as a demo to systemically decouple the correlation between the total content of heteroatoms and the specific capacitance as well as the self-discharge *** capacitance changes in a range of 164–331 F g^(-1)@1 A g^(-1)with the increased total contents of doped heteroatom,strongly dependent on and sensitive to the total content of *** voltage retention rate and capacitance retention rate for the porous carbon nanosheets with a tunable total content of heteroatoms completely present a quick decline tendency as the increase in the content of heteroatoms,changing from 58%to 34%and 74%to 39%,respectively,indicative of a linear negative *** importantly,the self-discharge mechanisms are elaborately explored and follow the combination of activation-and diffusion-controlled Faradic *** work illustrates the diverse impacts of the doped heteroatoms on the electrochemical performance of supercapacitors,covering specific capacitance and self-discharge behavior,and highlights the importance of balancing the contents of doped heteroatoms in energy storage fields.

关键词： Supercapacitor Heteroatom-doped carbon Self-discharge Capacitance

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Intrinsic pentagon defect engineering in multiple spatial-scale carbon frameworks for efficient triiodide reduction

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Journal of energy Chemistry 2024年第8期95卷 20-28,I0002页

作者： Siyi Hou Xuedan Song Chang Yu Jiangwei Chang Yiwang Ding Yingbin Liu Xiubo Zhang Weizhe Liu Jieshan Qiu State key lab of Fine chemicals Liaoning Key Lab for Energy Materials and Chemical EngineeringFrontier Science Center for Smart MaterialsSchool of Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina liaoning key lab for energy materials and chemical engineering Frontier Science Center for Smart MaterialsSchool of ChemistryDalian University of TechnologyDalian 116024LiaoningChina State key laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Intrinsic topological defect engineering has been proven as a promising strategy to elevate the electrocatalytic activity of carbon ***,the controllable construction of high-density and specific topological defects in carbon frameworks to reveal the relationship between reactivity and defect structure remains a challenging ***,the intrinsic pentagon carbon sites that can favor electron overflow and enhance their binding affinity towards the intermediates of catalytic reaction are firstly presented by the work function and the p-band center *** experimentally verify this,the cage-opening reaction of fullerene is proposed and utilized for synthesizing carbon quantum dots with specific pentagon configuration(CQDs-P),subsequently utilizing CQDs-P to modulate the micro-scale defect density of three-dimensional reduced graphene oxide(rGO)viaπ-π*** multiple spatial-scale rGO-conjugated CQDs-P structure simultaneously possesses abundant pentagon and edge defects as catalytic active sites and long-range-orderedπelectron delocalization system as conductive *** defects-rich CQDs-P/rGO-4 all-carbon-based catalyst exhibits superb catalytic activity for triiodide reduction reaction with a high photoelectric conversion efficiency of 8.40%,superior to the Pt reference(7.97%).Theoretical calculations suggest that pentagon defects in the carbon frameworks can promote charge transfer and modulate the adsorption/dissociation behavior of the reaction intermediates,thus enhancing the electrocatalytic activity of the *** work confirms the role of intrinsic pentagon defects in catalytic reactions and provides a new insight into the synthesis of defects-rich carbon catalysts.

关键词： Defect engineering Pentagon carbon Carbon quantum dots Electrocatalytic activity Triiodide reduction

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An effective'salt in dimethyl sulfoxide/water'electrolyte enables high-voltage supercapacitor operated at-50℃

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Journal of energy Chemistry 2024年第6期93卷 361-367,I0009页

作者： Yingbin Liu Chang Yu Xuedan Song Siyi Hou Shuqin Lan Jinhe Yu Yuanyang Xie Jieshan Qiu State key lab of Fine chemicals Frontier Science Center for Smart MaterialsSchool of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina School of Chemistry Frontier Science Center for Smart MaterialsLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina College of chemical engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Compared with organic electrolytes,aqueous electrolytes exhibit significantly higher ionic conductivity and possess inherent safety features,showcasing unique advantages in ***,challenges remain for low-salt aqueous electrolytes operating at high voltage and low ***,we report a low-salt(0.87 m,m means mol kg^(-1))'salt in dimethyl sulfoxide/water'hybrid electrolyte with non-flammability via hybridizing aqueous electrolyte with an organic co-solvent of dimethyl sulfoxide(hydrogen bond acceptor).As a result,the 0.87 m hybrid electrolyte exhibits enhanced electrochemical stability,a freezing temperature below-50℃,and an outstanding ionic conductivity of 0.52mS cm~(-1)at-50℃.Dimethyl sulfoxide can anchor water molecules through intermolecular hydrogen bond interaction,effectively reinforcing the stability of water in the hybrid ***,the interaction between dimethyl sulfoxide and water molecules diminishes the involvement of water in the generation of ordered ice crystals,finally facilitating the low-temperature performance of the hybrid *** paired with the 0.87 m'salt in dimethyl sulfoxide/water'hybrid electrolyte,the symmetric supercapacitor presents a 2.0 V high operating voltage at 25℃,and can operate stably at-50℃.Importantly,the suppressed electrochemical reaction of water at-50℃further leads to the symmetric supercapacitor operated at a higher voltage of 2.6 *** modification strategy opens an effective avenue to develop low-salt electrolytes for high-voltage and low-temperature aqueous supercapacitors.

关键词： Dimethyl sulfoxide Co-solvent High voltage Low temperature Supercapacitors

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A long/short-range interconnected carbon with well-defined mesopore for high-energy-density supercapacitors

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Nano Research 2022年第2期15卷 1399-1408页

作者： Yuanyang Xie Chang Yu Wei Guo Lin Ni Zhao Wang Jinhe Yu Le Yang Rong Fu Kunlun Liu Jieshan Qiu State key lab of Fine chemicals School of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024China

Amorphous carbon derived from biomass unusually combines the merits of large specific surface area and abundant micropores,offering massive anchoring points for ion adsorption in ***,the short-range ordered structure in amorphous carbon hinders the fast electron ***,graphitic carbon with long-range ordered structure is beneficial for electron ***,a low-cost strategy is required to marry hierarchical porous structure with long-range ordered structure,resulting in a long/short-range interconnected porous carbon and then leading to fast ion and electron ***,we modified the solid-phase conversion process of biomass by employing the features of liquid-phase carbonization for petroleum *** the assistance of asphalt,the large specific surface area(>2,000 m^(2)·g^(-1)),high ratio of mesopores(ca.60%)together with long-range ordered structure are in-situ created in as-made porous *** to the well configured structure in small scale,the as-made co-converted carbon can be operated in high-viscosity EMIMBF4 electrolyte with a superior capacitance(315 F·g^(-1)@1 A·g^(-1)).Besides,the as-assembled symmetric supercapacitor can deliver a super-high specific energy of 174 Wh·kg^(-1)@2.0 kW·kg^(-1).This work provides a new version for designing highly porous biomass-derived carbon with long/short-range alternating structure at molecular level.

关键词： long/short-range interconnected porous carbon hierarchical porous structure specific energy/power supercapacitors

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Recent research advances of self-discharge in supercapacitors:Mechanisms and suppressing strategies

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Journal of energy Chemistry 2021年第7期30卷 94-109页

作者： Kunlun Liu Chang Yu Wei Guo Lin Ni Jinhe Yu Yuanyang Xie Zhao Wang Yongwen Ren Jieshan Qiu State key lab of Fine chemicals School of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina College of chemical engineering Beijing University of Chemical TechnologyBeijing 100029China

Supercapacitors are one of the most promising energy storage devices in the fields of vehicle transportation,flexible electronic devices,aerospace,***,the existed self-discharge that is the spontaneous voltage decay after supercapacitors are fully charged,brings about the wide gap between experimental studies and practical utilization of *** eliminating the selfdischarge completely is not reachable,suppressing the self-discharge rate to the lowest point is possible and *** far,the significant endeavors have been devoted to achieve this ***,we summary and discuss the possible mechanisms for the self-discharge and the underlying influence ***,the strategies to suppress the self-discharge are systemically summed up by three independent but unified aspects:modifying the electrode,modulating the electrolyte and tuning the ***,the major challenges to suppress the self-discharge of supercapacitors are concluded and the promising strategies are also pointed out and *** review is presented with the view of serving as a guideline to suppress the self-discharge of supercapacitors and to across-the-board facilitate their widespread application.

关键词： Supercapacitors Self-discharge Mechanism Suppressing strategy

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Solar-driven salt-free deposition evaporation for simultaneous desalination and electricity generation based on tip-effect and siphon-effect

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Journal of energy Chemistry 2024年第11期98卷 364-373页

作者： Wan Xue Zongbin Zhao Guanyu Zhao Honghui Bi Huijun Zhu Xuzhen Wang Jieshan Qiu State key laboratory of Fine chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina State key laboratory of Fine chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of ChemistryDalian University of TechnologyDalian 116024LiaoningChina State key laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Solar-driven desalination is a promising way to alleviate the freshwater shortage,while is facing challenges posed by low evaporation rates and severe salt ***,a high-performance twodimensional(2D) solar absorber with Co_(3)O_(4) nanoneedle arrays(Co_(3)O_(4)-NN) grown on the surface of reduced graphene oxide-coated pyrolyzed silk cloth(Co_(3)O_(4)-NN/rGO/PSC) was prepared,and a salt-free evaporator system was assembled based on the composite material and siphonage-the flowing water *** is revealed that the evaporation enthalpy of water can be reduced over the 2D solar absorber grown with Co_(3)O_(4)-NN_T enabling an evaporation rate of up to 2.35 kg m^(-2) h^(-1) in DI water under one solar *** desalination process can be carried out continuously even with salt concentration up to 20 wt%,due to the timely removal of concentrated brine from the interface with the assistance of directed flowing ***,the 2D structure and the flowing water also provide an opportunity to convert waste solar heat into electricity in the evaporator based on the seebeck effect,ensuring simultaneous freshwater production and power *** is believed that this work provides insights into designing hybrid systems with high evaporation rate,salt resistance,and electricity generation.

关键词： Co_(3)O_(4)nanoneedle arrays Solar water evaporation Evaporation enthalpy Salt free Siphon effect Power generation

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