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Single-Molecule Confinement Induced Intrinsic Multi-Electron Redox-Activity to Enhance Supercapacitor Performance

Energy & Environmental materials 2023年第4期6卷 227-238页

作者： Su Yang Meiling Wang Yong Zhang Pinyi He Wenhua Cong Chongji Wang Qiankun Yang Xuguang Liu Tian Wang Xianming Zhang Jiadong Zhou College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan 030024China Key Lab of Advanced Optoelectronic Quantum Architecture and Measurement(Ministry of Education) Beijing Key Lab of Nanophotonics&Ultrafine Optoelectronic Systemsand School of PhysicsBeijing Institute of TechnologyBeijing 100081China School of Materials Science and engineering Central South UniversityChangsha 410083China Department of Chemistry National University of Singapore3 Science Drive 3117543Singapore Key Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education (Taiyuan University of Technology)Taiyuan 030024China

Aggregation of polyoxometalates(POM)is largely responsible for the reduced performance of POM-based energy-storage *** address this challenge,here,the precise confinement of single Keggin-type POM molecule in a porous carbon(PC)of unimodal super-micropore(micro-PC)is *** precise single-molecule confinement enables sufficient activity center exposure and maximum electron-transfer from micro-PC to POM,which well stabilizes the electron-accepting molecules and thoroughly activates its inherent multi-electron *** particular,the redox-activities and electron-accepting properties of the confined POM molecule are revealed to be super-micropore pore size-dependent by experiment and spectroscopy as well as theoretical ***,the molecularly dispersed POM molecules confined steadily in the“cage”of micro-PC exhibit unprecedented large-negative-potential stability and multiple-peak redox-activity at an ultra-low loading of~11.4 wt%.As a result,the fabricated solid-state supercapacitor achieves a remarkable areal capacitance,ultrahigh energy and power density of 443 mF cm^(-2),0.12 mWh cm^(-2)and 21.1 mW cm^(-2),*** work establishes a novel strategy for the precise confinement of single POM molecule,providing a versatile approach to inducing the intrinsic activity of POMs for advanced energy-storage systems.

关键词： intrinsic redox-activity polyoxometalates single-molecule confinement supercapacitor

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Quasi-Flat Narrow Bandgap Copper Indium Gallium Selenium Bottom Cell Application in Perovskite/Copper Indium Gallium Selenium Tandem Solar Cells

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Energy Material Advances 2024年第1期5卷 87-96页

作者： Bowen Liang Lulu Chen Xingchao Shao Xinye Yuan Shen Yu Wei Tang Siyuan Zhu Jie Zhang Yan Jiang Chunlei Yang Weimin Li Shenzhen Institute of Advanced Technology Chinese Academy of SciencesShenzhen 518055China Department of Nano Science and Technology Institute University of Science and Technology of ChinaSuzhou 215123China University of Chinese Academy of Sciences Beijing 100049China Songshan Lake Materials Laboratory DongguanGuangdong 523429China Department of Physics Liaoning UniversityShenyang 110036China School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China

Cu(In_(1−x)Ga_(x))Se_(2)(CIGS)is a promising and ideal material for bottom cell in tandem solar cells,which can break the double junction solar cell’s Shockley-Queisser theoretical efficiency to above 40%.However,the high-efficiency CIGS solar cells deposited by the 3-stage process is normally double grading,leading to an incomplete absorption in the bottom *** this study,single bandgap grading and quasi-flat bandgap CIGS solar cells are proposed and fabricated for perovskite/CIGS 4-terminal tandem solar cells,which are more favorable for long-wavelength absorption and higher short-circuit current density J_(sc).Various characterizations have been performed to investigate the crystallization,crystal defects,composition depth profile,and carrier dynamics of the CIGS thin *** study reveals that the performance of CIGS solar cells with high Ga content is worse than *** bandgap engineering,we can obtain CIGS solar cell with an efficiency above 16.5%regardless of the GGI[Ga/(Ga+In)]varying from 0.27 to ***,CIGS solar cells with less Ga content and low bandgap exhibit superior long-wavelength spectral response,making them more suitable for bottom cell applications in tandem solar *** combination with an 18.9%semitransparent inorganic perovskite solar cell,a 25.6%perovskite/CIGS tandem device in 4-T configuration is demonstrated.

关键词： bandgap engineering bottom cell perovskite tandem solar cells efficiency tandem solar cellswhich solar cells copper indium gallium selenium

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Two-dimensional conjugated N-rich covalent organic frameworks for superior sodium storage

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science China Chemistry 2022年第7期65卷 1291-1298页

作者： Xiya Yang Yucheng Jin Baoqiu Yu Lei Gong Wenbo Liu Xiaolin Liu Xin Chen Kang Wang Jianzhuang Jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and TechnologyBeijing 100083China

Sodium-ion batteries(SIBs) are considered as a promising next-generation energy storage system. To achieve the large-scale application of SIBs, it is crucial to develop cost-effective anode materials with high Na-ion storage capacity. Herein twodimensional(2D) conjugated covalent organic frameworks(c COFs) with N-rich phthalocyanine(Pc) units fused via benzene moieties(named MPc-2D-c COFs) were explored as the SIBs anode materials. Electrochemical tests reveal their high reversible capacities of 538 and 342 m A h g^(-1) at 50 and 1000 m A g^(-1), respectively, good rate performance, and excellent stability,comparable to the state-of-the-art anode materials of SIBs, indicating their outstanding Na-ion storage performance. Ex situ Xray photoelectron and Fourier transform infrared spectroscopies together with theoretical calculations disclose the N atoms at the pore channels and conjugated pyrrole moieties of MPc-2D-c COFs provide abundant Na-ion storage sites. This, in cooperation with the enhanced electrical conductivity owing to the 2D conjugated structure, contributes to the outstanding Na-ion storage capacity of MPc-2D-c COFs. The present result is surely helpful for developing high-performance and cost-effective COFs as electroactive materials for SIBs.

关键词： covalent organic frameworks sodium-ion batteries phthalocyanine anode materials π-conjugated 2D COFs

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Off-stoichiometry-guided design of high-strength chemically complex intermetallic-based alloys with outstanding ductility

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Journal of materials science & technology 2023年第29期160卷 28-33页

作者： Bo Xiao Jixun Zhang Shaofei Liu Yilu Zhao Lianyong Xu C.T.Liu Tao Yang Department of Materials Science and Engineering Mechanical Behavior Division of Shenyang National Laboratory for Materials ScienceCity University of Hong KongHong KongChina Center for Advanced Nuclear Safety and Sustainable Development City University of Hong KongHong KongChina Hong Kong Institute for Advanced Study City University of Hong KongHong KongChina School of Materials Science and Engineering Harbin Institute of Technology(Shenzhen)Shenzhen 518055China School of Materials Science and Engineering Tianjin UniversityTianjin 300350China

*** The lasting drive for improved energy efficiency in power gen-eration encourages the innovative design of advanced structural materials with superb mechanical properties[1-6].Among these materials,ordered intermetallic alloys[7-9],as a unique class of metallic materials,have drawn increasing concern from both the scientific and industrial communities due to their intriguing high-temperature properties,strong chemical binding,and low atomic mobility[10,11].However,in light of the insufficient number of slip systems and/or intrinsically weak grain boundary(GB),they are usually brittle at ambient temperature,severely hindering their practical use in engineering systems[12].Previous studies reported that the change in alloy stoichiometry has a significant beneficial effect on the ductility of intermetallic *** instance,Liu et al.

关键词： intermetallic ductility alloys

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Excellent energy storage properties in non-stoichiometric Bi_(0.5)Na_(0.5)TiO_(3)-based relaxor ferroelectric ceramics

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Chinese Chemical Letters 2024年第7期35卷 470-472页

作者： Shunshun Jiang Ji Zhang Jing Wang Shan-Tao Zhang School of Materials Science and Engineering Nanjing University of Science&TechnologyNanjing 210094China State Key Laboratory of Mechanics and Control of Mechanical Structures College of Aerospace EngineeringNanjing University of Aeronautics and AstronauticsNanjing 210016China National Laboratory of Solid State Microstructures Department of Materials Science and EngineeringCollege of Engineering and Applied Science&Jiangsu Key Laboratory of Artificial Functional Materials&Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210093China

The rapid development of high-power and pulsed-power techniques inspires extensive investigates on high-performance ceramic-based ***,the low recoverable energy density(Wrec)hampers their wider ***,the non-stoichiometric Bi_(0.5)Na_(0.5)TiO_(3)-based ceramics were designed and *** proper introduction of oxygen vacancies facilitated activating defect dipole,giving rise to reduced remanent ***,the optimal composition exhibited an exceptional high Wrec of 8.3 J/cm^(3),a high efficiency of 85%,and excellent anti-fatigue and thermal *** work provides an efficient approach to explore ceramic capacitors with high capacitive energy storage performances.

关键词： Non-stoichiometric Bi_(0.5)Na_(0.5)TiO_(3) Ceramic capacitor Energy density Thermal stability

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Unveiling solid-solid contact states in all-solid-state lithium batteries:An electrochemical impedance spectroscopy viewpoint

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Journal of Energy Chemistry 2025年第2期101卷 16-22,I0002页

作者： Jin-Liang Li Liang Shen Zi-Ning Cheng Jun-Dong Zhang Ling-Xuan Li Yu-Tong Zhang Yan-Bin Gao Chunli Guo Xiang Chen Chen-Zi Zhao Rui Zhang Qiang Zhang Tsinghua Center for Green Chemical Engineering Electrification Beijing Key Laboratory of Green Chemical Reaction Engineering and TechnologyDepartment of Chemical EngineeringTsinghua UniversityBeijing 100084China Advanced Research Institute of Multidisciplinary Science School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing Huairou Laboratory Beijing 101400China College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan 030024ShanxChina Institute for Carbon Neutrality Tsinghua UniversityBeijing 100084China Shanxi Research Institute for Clean Energy Tsinghua UniversityTaiyuan 030032ShanxiChina

All-solid-state lithium batteries(ASSLBs)are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic *** solid-solid contact between lithium metal and solid electrolyte plays a vital role in the performance of working ASSLBs,which is challenging to investigate quantitatively by experimental *** work proposed a quantitative model based on the finite element method for electrochemical impedance spectroscopy simulation of different solid-solid contact states in *** the assistance of an equivalent circuit model and distribution of relaxation times,it is discovered that as the number of voids and the sharpness of cracks increase,the contact resistance Rcgrows and ultimately dominates the battery *** accurate fitting,inverse proportional relations between contact resistance Rcand(1-porosity)as well as crack angle was *** contribution affords a fresh insight into clarifying solid-solid contact states in ASSLBs.

关键词： Electrochemical impedance spectroscopy All-solid-state lithium batteries Solid-solid contacts Finite element method Equivalent circuit model Distribution of relaxation times

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Influence of Associated Cations on the Transport and Adsorption of Chloride Ions in the Nano-channel of Calcium Aluminosilicate Hydrate Gel:A Molecular Dynamics Study

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Journal of Wuhan University of technology(materials science) 2022年第5期37卷 963-976页

作者： YANG Jun ZHANG Gaozhan DING Qingjun WANG Aiguo HOU Dongshuai Anhui Province Engineering Laboratory of Advanced Building Materials School of Materials and Chemical EngineeringAnhui Jianzhu UniversityHefei230601China State Key Laboratory of Silicate Materials for Architectures School of Materials Science and EngineeringWuhan University of TechnologyWuhan430070China School of Materials Science and Engineering Department of Civil EngineeringQingdao University of TechnologyQingdao266033China

Molecular dynamics simulation was utilized to investigate the transport and adsorption of chloride in the nanopore of calcium aluminosilicate hydrate(C-A-S-H)with associated cation types of Ca,Mg,Na and *** local ionic structure,atomic dynamics and bond stability were analyzed to elucidate the interaction between cations and chloride *** results show that interfacial chloride is absorbed through the ion pairing formation in the vicinity of C-A-S-H *** cations can simultaneously interact aluminosilicate chains,water molecules and Cl^(-)ions,which restrict the motion of interfacial Cl^(-)*** solution chloride can be immobilized through the solvation effect of *** along with their hydration shell can connect to neighboring Cl^(-)ions to decrease their *** to the varied ionic chemistry,cations show different interaction strength with neighboring water molecules and anions,which determines the chloride transport behavior in the nanopore of *** chloride immobilization capacity of C-A-S-H nanopore with different associated cations is listed in following order:Mg^(2+)Ca^(2+)

关键词： calcium aluminosilicate hydrate nanometer channel confinement chloride immobilization associated cations ionic structure

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Interface-induced polymerization strategy for constructing titanium dioxide embedded carbon porous framework with enhanced chemical immobilization towards lithium polysulfides

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Nano Research 2024年第3期17卷 1473-1481页

作者： Yue Ouyang Xiaoxiao Li Jiexin Zhu Wei Zong Yuhang Dai Xuan Gao Wei Zhang Shengyuan Yang Roohollah Bagherzadeh Feili Lai Yue-E Miao Tianxi Liu State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua University2999 North Renmin RoadShanghai 201620China The Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122China Advanced Fibrous Materials LAB Institute for Advanced Textile Materials and Technologies(ATMT)School of Advanced Materials and ProcessesAmirkabir University of TechnologyTehran 15914Iran Christopher Ingold Laboratory Department of ChemistryUniversity College London20 Gordon StreetLondon WC1H 0AJUK Department of Chemistry KU LeuvenCelestijnenlaan 200FLeuven 3001Belgium

The shuttle effect induced by soluble lithium polysulfides(LiPSs)is known as one of the crucial issues that limit the practical applications of lithium-sulfur(Li-S)***,a titanium dioxide nanoparticle embedded in nitrogen-doped porous carbon nanofiber(TiO_(2)@NCNF)composite is constructed via an interface-induced polymerization strategy to serve as an ideal sulfur *** the protection of the nanofiber walls,the uniformly dispersed TiO_(2) nanocrystalline can act as capturing centers to constantly immobilize LiPSs towards durable sulfur ***,the mesoporous microstructure in the fibrous framework endows the TiO_(2)@NCNF host with strong physical reservation for sulfur and LiPSs,sufficient pathways for electron/ion transfer,and excellent endurance for volume *** expected,the sulfur-loaded TiO_(2)@NCNF composite electrode presents a fabulous rate performance and long cycle lifespan(capacity fading rate of 0.062%per cycle over 500 cycles)at 2.0 ***,the assembled Li-S batteries harvest superb areal capacity and cycling stability even under high sulfur loading and lean electrolyte conditions.

关键词： interface-induced polymerization electrospun porous nanofibers lithium-sulfur(Li-S)batteries high sulfur loading lithium polysulfides(LiPSs)immobilization

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Sparse identification-assisted exploration of the atomic-scale deformation mechanism in multiphase CoCrFeNi high-entropy alloys

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science China(Technological sciences) 2024年第4期67卷 1124-1132页

作者： XIAO Lu GUO XiaoXiang SUN YuTong WANG Gang LONG WeiMin LIAW Peter K. REN JingLi School of Mathematics and Statistics Zhengzhou UniversityZhengzhou 450001China Academy of Mathematics and Systems Science Chinese Academy of SciencesBeijing 100190China Institute of Materials Shanghai UniversityShanghai 200444China SKL of Advanced Brazing Metals&Technology Zhengzhou Research Institute of Mechanical EngineeringZhengzhou 450001China Department of Materials Science and Engineering The University of TennesseeKnoxvilleTN 37996USA

This study investigated the atomic-scale deformation mechanism of multiphase CoCrFeNi high-entropy alloys(HEAs)at liquid helium,liquid nitrogen,and room temperatures.A million-atom multiphase HEA was prepared using molecular dynamics simulation involving melt and quench *** HEA exhibited high-density dislocations and some twins,consistent with experimental *** analysis revealed an inconsistent evolution of the microstructure under tensile *** particular,the elastic and initial plastic stages exhibited an increase in the disordered structure at the expense of the face-centered cubic and hexagonal close-packed structures,followed by a subsequent transformation involving multiple structural ***,through sparse identification,a model depicting microstructural evolution during tension was extracted for the CoCrFeNi HEA at three typical temperatures and three tensile *** model highlighted the importance of the body-centered cubic structure in the evolutionary process.

关键词： high-entropy alloy data-driven method microstructure evolution multiphase structure molecular dynamics simulation

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Trifunctional robust electrocatalysts based on 3D Fe/N-doped carbon nanocubes encapsulating Co4N nanoparticles for efficient battery-powered water electrolyzers

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Carbon Energy 2024年第6期6卷 124-139页

作者： Hyung Wook Choi Hongdae Lee Jun Lu Seok Bin Kwon Dong In Jeong Beum Jin Park Jiwon Kim Bong Kyun Kang Gun Jang Dae Ho Yoon Ho Seok Park SKKU Advanced Institute of Nano Technology(SAINT) Sungkyunkwan UniversitySuwon-siGyeonggi-doRepublic of Korea School of Chemical Engineering Sungkyunkwan UniversitySuwon-siGyeonggi-doRepublic of Korea School of Advanced Materials Science and Engineering Sungkyunkwan UniversitySuwon-siGyeonggi-doRepublic of Korea Department of Electronic Materials Devicesand Equipment EngineeringSoonchunhyang UniversityAsan CityChungnamRepublic of Korea SKKU Institute of Energy Science and Technology(SIEST) Sungkyunkwan UniversitySuwon-siGyeonggi-doRepublic of Korea Department of Health Sciences and Technology Samsung Advanced Institute for Health Sciences and Technology(SAIHST)Sungkyunkwan UniversitySuwonRepublic of Korea

Herein,we have designed a highly active and robust trifunctional electrocatalyst derived from Prussian blue analogs,where Co_(4)N nanoparticles are encapsulated by Fe embedded in N-doped carbon nanocubes to synthesize hierarchically structured Co_(4)N@Fe/N-C for rechargeable zinc-air batteries and overall water-splitting *** confirmed by theoretical and experimental results,the high intrinsic oxygen reduction reaction,oxygen evolution reaction,and hydrogen evolution reaction activities of Co_(4)N@Fe/N-C were attributed to the formation of the heterointerface and the modulated local electronic ***,Co_(4)N@Fe/N-C induced improvement in these trifunctional electrocatalytic activities owing to the hierarchical hollow nanocube structure,uniform distribution of Co_(4)N,and conductive encapsulation by Fe/***,the rechargeable zinc-air battery with Co_(4)N@Fe/N-C delivers a high specific capacity of 789.9 mAh g^(-1) and stable voltage profiles over 500 ***,the overall water electrolyzer with Co_(4)N@Fe/N-C achieved better durability and rate performance than that with the Pt/C and IrO2 catalysts,delivering a high Faradaic efficiency of 96.4%.Along with the great potential of the integrated water electrolyzer powered by a zinc-air battery for practical applications,therefore,the mechanistic understanding and active site identification provide valuable insights into the rational design of advanced multifunctional electrocatalysts for energy storage and conversion.

关键词： battery-powered electrolyzers hierarchical structure Prussian blue analog trifunctional electrocatalyst zinc-air battery

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