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Extended conjugation-induced π electron redistribution for stabilizing organic anodes in aqueous ammonium ion batteries

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Journal of Energy Storage 2025年 130卷

作者： Xinlei Tang Haode Zhang Sensen Yu Shan Hu Wen Chen State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 PR China

Organic molecules have attracted significant attention as potential anode materials for aqueous ammonium-ion batteries (AAIBs) due to their tunable structure, rich active sites, and abundant resources. However, their practical applications are hindered by structural instability and high solubility. Herein, we design an extended conjugated molecule, benzo[ a ]benzo[7,8]quinoxalino[2,3- i ]phenazine-8,17-dione (TABQ-NQ), by incorporating phenyl groups into the 5,7,12,14-tetraaza-6,13-pentacenequinone (TAPQ) structure. The strengthened intermolecular interactions arising from the extended conjugation contribute to the improved structural integrity of TABQ-NQ. Furthermore, the intramolecular charge redistribution facilitated by the extended conjugation enhances the binding affinity between TABQ-NQ and NH 4 + while reducing interactions of TABQ-NQ with H 2 O, thereby stabilizing discharge intermediates and preventing further dissolution. As a result, TABQ-NQ exhibits reduced solubility, improved stability, and superior electrochemical performance. The TABQ-NQ anode demonstrates a high initial specific capacity of 190 mAh g −1 , with a capacity of 146 mAh g −1 at 0.2 A g −1 after over 650 cycles, corresponding to the capacity retention of 76.8 %, and maintains an initial capacity of 127.5 mAh g −1 at 2 A g −1 . Ex-situ characterizations further reveal the low solubility and high redox reversibility of TABQ-NQ. This work provides new insights into the extension of conjugated structures in organic molecules and offers valuable guidance for the development of AAIBs research.

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Activated carbon clothes for wide-voltage high-energy-density aqueous symmetric supercapacitors

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Chinese Chemical Letters 2020年第6期31卷 1620-1624页

作者： Kwadwo Asare Owusu Zhaoyang Wang Longbing Qu Zi'ang Liu Jaafar Abdul-Aziz Mehrez Qiulong Wei Liang Zhou Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Department of Mechanical Engineering The University of MelbourneParkvilleVIC 3010Australia Department of Materials Science and Engineering University of California Los AngelesCA 90095-1595USA

Commercial carbon clothes have the potential to be utilized as supercapacitor electrodes due to their low cost and high ***,the negligible surface area of the carbon clothes serves as a serious impediment to their ***,we report a facile calcination activation method for carbon cloths to realize remarkable comprehensive electrochemical *** activated carbon cloths deliver a high areal capacitance(1700 mF/cm^2),good rate capability,and stable cycling performance up to 20,000 *** to the stability in the wide potential window,a designed symmetric capacitor can function in a cell voltage of 2.0 V and delivers high volumetric and gravimetric energy densities of 7.62 mWh/cm^3 and 18.2 Wh/kg,*** remarkable electrochemical performance is attributed to rich microporosity with high surface area,superior electrolyte wettability,and stability in wide potential window.

关键词： Activated carbon cloth Microporosity Aqueous symmetric supercapacitors Energy density Voltage window

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Phosphorus Coordinated Co/Se2 Heterointerface Nanowires: In-Situ Catalyst Reconstruction Toward Efficient Overall Water Splitting in Alkaline and Seawater Media

SSRN

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SSRN 2023年

作者： Boakye, Felix Ofori Harrath, Karim Tabish, Mohammad Yasin, Ghulam Owusu, Kwadwo Asare Ajmal, Saira Zhang, Wenbin Zhang, Haining Zhao, Wei Institute for Advanced Study Shenzhen University Shenzhen518060 China College of Physics and Optoelectronic Engineering Shenzhen University Shenzhen518060 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China Department of Chemistry Guangdong Provincial Key Laboratory of Catalytic Chemistry Southern University of Science and Technology Guangdong Shenzhen518055 China College of Materials Science and Engineering Beijing University of Chemical Technology Beijing100029 China

Designing a highly efficient electrocatalyst to realize overall water splitting is vital, yet identifying the active site remains an ongoing challenge. Herein, the electrochemical in situ surface activation of P@Co/Se2-NW/CC was investigated to understand the enhanced OER activity of P@Co/Se2-NW/CC. The incorporation of phosphorus is thought to increase the number of vacancies surrounding the Co cations in the initial Co/Se2 and speed up the structural change into "active species" like cobalt oxide/oxyhydroxide. The as-synthesized P@Co/Se2-NW/CC required a low overpotential for OER (η20 = 170 and 200 mV) and HER (η10 = 52 and 82 mV), respectively, in alkaline water and alkaline seawater media. In situ FTIR and Post characterization unraveled the existence of surface-bounded Co oxide species on P@Co/Se2-NW/CC after OER catalysis, which is responsible for the enhanced electrocatalytic activity. This study offers a valuable strategy for developing noble-metal-free bifunctional catalysts for efficient hydrogen generation from alkaline seawater and alkaline water electrolysis. © 2023, The Authors. All rights reserved.

关键词： Oxygen

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Operando Selenium Treatment Towards Enhanced Cyclic Stability for Single-Crystal Ni-Rich Cathode at Ultra-High Voltage of 4.7 V

SSRN

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SSRN 2023年

作者： Zhang, Zhi Ding, Xiang He, Xinyou Gong, Yang Xiao, Biaobiao Shen, Jixue Ou, Xing Hunan Provincial Key Laboratory of Water Treatment Functional Materials Hunan Provincial Key Laboratory for Control Technology of Distributed Electric Propulsion Aircraf College of Chemistry and Materials Engineering Hunan University of Arts and Science Changde415000 China Engineering Research Center of the Ministry of Education for Advanced Battery Materials School of Metallurgy and Environment Central South University Changsha410083 China Institute of Advanced Battery Materials and Devices Faculty of Materials and Manufacturing Beijing University of Technology Beijing100124 China Tianmu Lake Institute of Advanced Energy Storage Technologies Co. Ltd Liyang213300 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China

Developing high-voltage (≥4.3 V vs Li/Li+) single-crystal Ni-rich LiNixCoyMn1-x-yO2 offers an enticing strategy to achieve high energy density for lithium-ion batteries. However, at high-voltage operation, the cathode will be vulnerable to induce the intrinsic Oα- (α 0.6Co0.1Mn0.3O2 (SC-NCM) cathode materials by introducing the surface Se element, exhibiting an "anti-aging" effect of inhibiting the escape of oxygen on SC-NCM particles during the ultra-high voltage (4.7 V) cycling. Both theoretical calculation and experimental results confirm that the outside-in nanostructure would substitute some mobile Oα- at the surface of highly charged SC-NCM particle, stabilizing the oxygen lattice and suppressing O2 release during long-term cycling. Meanwhile, the surface modification of thin Se layer will alleviate the parasitic reactions and improve the electronic conductivity. Under the synergistic strategy of surface modification and interface doping, the obtained SC-NCM exhibits boosted cyclic stability in coin half-cell and pouch full-cell simultaneously. Therefore, the reversible capacity of LiNi0.6Co0.1Mn0.3O2 at high voltage is competitive with comercial LiNixCoyMn1-x-yO2 (x ≥ 0.8), demonstrating more superior safety ability and cyclic property. It provides an effective approach for improving the long-term performance of Ni-rich cathode materials for practical application under ultra-high working voltage. © 2023, The Authors. All rights reserved.

关键词： Single crystals

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Entropy-Driven Structural Transition from Tetragonal to Cubic Phase: High Thermoelectric Performance of Cucdinse3 Compound

SSRN

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SSRN 2023年

作者： Luo, Tingting Hu, Yihao Liu, Shi Xia, Fanjie Qiu, Junhao Peng, Haoyang Liu, Keke Guo, Quansheng Li, XingZhong Yang, Dongwang Su, Xianli Wu, Jinsong Tang, Xinfeng State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Hubei Wuhan430070 China Key Laboratory for Quantum Materials of Zhejiang Province Department of Physics School of Science Westlake University Zhejiang Hangzhou310024 China School of Materials Science and Engineering Hubei University Hubei Wuhan430062 China Nebraska Center for Materials and Nanoscience University of Nebraska LincolnNE68588 United States

Cu based Chalcopyrite is an important class of thermoelectric materials with excellent electronic properties, however, the thermal conductivity is relatively high due to the simple tetragonal structure with highly ordered configuration on cation sites, limiting the thermoelectric performance. Herein, we realize that the modulation of entropy via alloying CdSe achieves the structural transition from tetragonal structure with ordered configuration on cations sites in CuInSe2 compound to cubic structured CuCdInSe3. CuCdInSe3 crystallizes in a zinc blende (ZnS) structure where Cu, Cd and In cations randomly occupy the Zn site with the occupancy rate of 1/3. This entropy driven order-disorder transition on the cation site, in conjunction with the intensified point defect phonon scattering via alloying CdSe in CuInSe2, dramatically suppress the thermal conductivity. An ultra-low thermal conductivity of 0.76 Wm-1K-1 at 780 K is achieved for CuCdInSe3 compound, which is only about 2/3 in comparison with that of CuInSe2 compound. CuCdInSe3 compound is an indirect semiconductor, where the minimum of conduction band (CBM) locates at Γ point and the maximum of valence band (VBM) locates at between Γ and A. The density of states in VBM of CuCdInSe3 compound are mainly contributed by the hybridization between Se-4p and Cu-3d orbitals, while that of CBM is dominant by Se-4p and In-5s orbitals. Minute adjustment of Cd content in CuCd(1+x)InSe3 compounds effectively modulates the carrier concentration and an optimized power factor of 0.58 Wm-1K-2 is attained at 578 K for CuCd1.01InSe3 compound, which is improved by 7.6 times in contrast with that of pristine CuCdInSe3 compound. The improved electronic properties integrating with the intrinsically low thermal conductivity result in an enhanced thermoelectric Figure of Merit ZT value of 0.45 at 780 K for CuCd1.005InSe3, which is six times higher than that of the pristine CuCdInSe3. © 2023, The Authors. All rights reserved.

关键词： Zinc sulfide

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Operando Selenium Treatment Towards Enhanced Cyclic Stability for Single-Crystal Ni-Rich Cathode at Ultra-High Voltage of 4.7 V

SSRN

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SSRN 2023年

作者： Zhang, Zhi Ding, Xiang He, Xinyou Gong, Yang Xiao, Biaobiao Shen, Jixue Ou, Xing Engineering Research Center The Ministry of Education for Advanced Battery Materials School of Metallurgy and Environment Central South University Changsha410083 China Hunan Provincial Key Laboratory of Water Treatment Functional Materials Hunan Provincial Key Laboratory for Control Technology of Distributed Electric Propulsion Aircraf College of Chemistry and Materials Engineering Hunan University of Arts and Science Changde415000 China Institute of Advanced Battery Materials and Devices Faculty of Materials and Manufacturing Beijing University of Technology Beijing100124 China Tianmu Lake Institute of Advanced Energy Storage Technologies Co. Ltd Liyang213300 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China

关键词： Single crystals

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MXene-based photocatalysts

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Journal of materials Science & technology 2020年第21期56卷 18-44页

作者： Panyong Kuang Jingxiang Low Bei Cheng Jiaguo Yu Jiajie Fan State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan430070China Hefei National Laboratory for Physical Sciences at the Microscale Collaborative Innovation Center of Chemistry for Energy Materials(iChEM)School of Chemistry and Materials Scienceand National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei230026China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou450001China

Transition metal carbide or nitride(MXene)is regarded as next-generation two-dimensional(2D)materials for various applications,such as photocatalysis,electrocatalysis,supercapacitor,lithium-ion battery and biomedicine,because of its unique physicochemical *** photocatalysis,MXene could allow fast photogenerated charge carrier separation and provide abundant surface functional groups for light harvesting materials,rendering feasible the high photoconversion ***,enormous theoretical and experimental studies have been recently made and shown the potential of MXene in various photocatalytic ***,we provide a brief overview of the MXene-based materials,along with their functions in photocatalytic ***,we summarize the recent advances and progresses of MXene-based photocatalysts,ranging from solar fuel production to pollutant ***,we present concluding remarks and the outlooks for achieving highly efficient MXene-based photocatalysts.

关键词： MXene Two-dimensional material Photocatalysis Ti3C2 Solar fuel production

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Recent advances in non-metal doped titania for solar-driven photocatalytic/photoelectrochemical water-splitting

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能源化学 2022年第3期66卷 529-559页

作者： Ying-Ying Wang Yan-Xin Chen Tarek Barakat Yu-Jia Zeng Jing Liu Stéphane Siffert Bao-Lian Su Laboratory of Inorganic Materials Chemistry(CMI) University of NamurB-5000 NamurBelgium Namur Institute of Structured Matter(NISM) University of NamurB-5000 NamurBelgium Laboratory of Inorganic Materials Chemistry(CMI) University of NamurB-5000 NamurBelgium CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhen 518060GuangdongChina State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430074HubeiChina Unité de Chimie Environnementale et Interactions sur le Vivant Université Littoral Cote d'Opale145Avenue Maurice Schuman59140 DunkerqueFrance Laboratory of Inorganic Materials Chemistry(CMI) University of NamurB-5000 NamurBelgium Namur Institute of Structured Matter(NISM) University of NamurB-5000 NamurBelgium State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430074HubeiChina

Photocatalytic(PC)/Photoelectrochemical(PEC)water splitting under solar light irradiation is consid-ered as a prospective technique to support the sustainable and renewable H2 economy and to reach the ultime goal of carbon ***2 based photocatalysts with high chemical stability and excellent photocatalytic properties have great potential for solar-to-H2 *** conquer the challenges of the large band-gap and rapid recombination of photo generated electron-holepairs in TiO2,non-metal doping turns out to be economic,facile,and effective on boosting the visible light *** localized defect states such as oxygen vacancy and Ti3+generated by non-metal doping are located in the band-gap of TiO2,which result in the reduction of band-gap,thus a red-shift of the absorption *** hetero dop-ing atoms such as B3+,I7+,S4+/S6+,P5+can also act as electron donors or trap sites which facilitate the charge carrier separation and suppress the recombination of electron-hole *** this comprehensive review,we present the most recent advances on non-metal doped TiO2 photocatalysts in terms of funda-mental aspects,origin of visible light activity and the PC/PEC behaviours for water *** particular,the characteristics of different non-metal elements(N,C,B,S,P,Halogens)as dopants are discussed in details focusing on the synthesis approaches,characterization as well as the efficiency of PC and PEC water *** present review aims at guiding the readers who want quick access to helpful infor-mation about how to efficiently improve the performance of photocatalysts by simple doping strategies and could stimulate new intuitive into the new doping strategies.

关键词： Photocatalytic/Photoelectrochemical water splitting Titania Non-metal doping Visible light photocatalysis

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Functionally Graded Triply Periodic Minimal Surface Scaffold of Ha-Al2o3 Via Vat Photopolymerization 3d Printing

SSRN

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SSRN 2023年

作者： Liu, Qiuyu Tang, Qinchao Huang, Zhifeng Li, Zhiwei Wang, Xuye Wen, Pin Bai, Yi Chen, Fei Hubei Longzhong Laboratory Wuhan University of Technology Xiangyang Demonstration Zone Xiangyang441000 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China International School of Materials Science and Engineering Wuhan University of Technology Wuhan430070 China State Key Laboratory of Oral & Maxillofacial Reconstruction and Regeneration Key Laboratory of Oral Biomedicine Ministry of Education Hubei Key Laboratory of Stomatology School & Hospital of Stomatology Wuhan430079 China Hubei Key Laboratory of Theory and Application of Advanced Materials Mechanics School of Science Wuhan University of Technology Wuhan430070 China

Hydroxyapatite (HA) is widely used in scaffolds due to its high similarity in the composition to natural bone. However, the weak and fragile characteristics of synthetic HA limit its application. The strength of HA can be increased by the incorporation of alumina (Al2O3) to obtain composites with extraordinary compressive strength and biocompatibility. HA-Al2O3 composites with different ratios were prepared by Vat photopolymerization 3D printing, and their shrinkage, porosity, phase composition and biocompatibility were systematically investigated. In addition, the Diamond structure of the scaffold was chosen to achieve the trade-off relationship between compressive strength and porosity. The results suggest that the HA-Al2O3 composite with 20 vol% HA possesses the maximum compressive strength and 60 vol% HA has optimal biocompatibility. A compositional gradient scaffold from 60 vol% HA and 20 vol% HA was proposed to satisfy different needs of the different parts in scaffold for biocompatibility and compressive strength. The HA-Al2O3 gradient scaffold achieves a preferable compressive strength of 13.7 MPa while possessing gradient biocompatibility. © 2023, The Authors. All rights reserved.

关键词： Hydroxyapatite

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Vacancy-Based Defect Regulation for High Thermoelectric Performance in Ge9Sb2Te12-x Compounds

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ACS APPLIED materials & INTERFACES 2020年第17期12卷 19664-19673页

作者： Chen, Shuo Bai, Hui Li, Junjie Pan, Wenfeng Jiang, Xianyan Li, Zhi Chen, Zhiquan Yan, Yonggao Su, Xianli Wu, Jinsong Uher, Ctirad Tang, Xinfeng State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Hubei Nuclear Solid Physics Key Laboratory Department of Physics Wuhan University Wuhan 430072 China Department of Physics University of Michigan Ann Arbor Michigan 48109 United States

Defect engineering is the core strategy for improving thermoelectric properties. Herein, cation doping along with modulation of cation vacancy has been developed in GeTe-based materials as an effective method to induce vacancy-based defects to boost their thermoelectric performance. A series of ternary compounds of Ge9Sb2Te12-x (x = 0, 0.03, 0.06, 0.09, 0.12, 0.15) was prepared by vacuum-melting and annealing combined with the spark plasma sintering (SPS) process. The role of Sb doping and cation vacancy on thermoelectric properties was systematically investigated. It is found that alloying Sb2Te3 into GeTe increases the concentration of cation vacancies, which is corroborated by both positron annihilation measurements and theoretical calculations. The vacancies, stacking faults, and planar defect interactions determine the thermoelectric transport properties. Adjusting the deficiency of Te effectively tunes the concentration of cation vacancies and dopant defects in the structure. In turn, this tunes the carrier concentration close to its optimum. A high power factor of 32.6 mu W cm(-1) K-2 is realized for Ge9Sb2Te11.91 at 725 K. Moreover, large strains induced by the defect structures, including Sb dopant, vacancy, staking faults, as well as planar defects intensify phonon scattering, leading to a significant decrease in the thermal conductivity from 7.6 W m(-1) K-1 for pristine GeTe to Ge9Sb2Te11.85 at room temperature. All of the above contribute to a high ZT value of 2.1 achieved for the Ge9Sb2Te11.91 sample at 775 K.

关键词： GeTe-based compounds alloying with Sb2Te3 deficiency of Te stacking fault vacancy plane thermoelectric

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