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Multiscale strain alleviation of Ni-rich cathode guided by in situ environmental transmission electron microscopy during the solid-state synthesis

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Journal of Energy Chemistry 2023年第9期84卷 467-475页

作者： Fengyu Zhang Yunna Guo Chenxi Li Tiening Tan Xuedong Zhang Jun Zhao Ping Qiu Hongbing Zhang Zhaoyu Rong Dingding Zhu Lei Deng Zhangran Ye Zhixuan Yu Peng Jia Xiang Liu Jianyu Huang Liqiang Zhang School of New Energy and Materials China University of Petroleum BeijingBeijing 102249China Clean Nano Energy Center state Key Laboratory of Metastable Materials Science and Technology Yanshan UniversityQinhuangdao 066004HebeiChina School of Materials Science and Engineering Beihang UniversityBeijing 100191China Sichuan New Energy Vehicle Innovation Center Yibin 644000SichuanChina School of Materials Science and Engineering Xiangtan UniversityXiangtan 411105HunanChina Peking University Institute of Advanced Agricultural Sciences Shandong Laboratory of Advanced Agricultural Sciences at WeifangWeifang 261000ShandongChina China Oil&Gas Pipeline Network Corporation Department of Engineering Beijing 100026China Hebei Key Laboratory of Applied Chemistry College of Environmental and Chemical EngineeringYanshan UniversityQinhuangdao 066004HebeiChina Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of Education School of Materials Science and EngineeringXiangtan UniversityXiangtan 411105HunanChina

Ni-rich layered oxides are one of the most promising cathode materials for Li-ion batteries due to their high energy ***,the chemomechanical breakdown and capacity degradation associated with the anisotropic lattice evolution during lithiation/delithiation hinders its practical ***,by utilizing the in situ environmental transmission electron microscopy(ETEM),we provide a real time nanoscale characterization of high temperature solid-state synthesis of LiNi_(0.8)CO_(0.1)Mn_(0.1)O_(2)(NCM811) cathode,and unprecedentedly reveal the strain/stress formation and morphological evolution mechanism of primary/second ary particles,as well as their influence on electrochemical *** show that stress inhomogeneity during solid-state synthesis will lead to both primary/secondary particle pulverization and new grain boundary initiation,which are detrimental to cathode cycling stability and rate *** to alleviate this multiscale strain during solid-state synthesis,we introduced a calcination scheme that effectively relieves the stress during the synthesis,thus mitigating the primary/secondary particle crack and the detrimental grain boundaries formation,which in turn improves the cathode structural integrity and Li-ion transport kinetics for long-life and high-rate electrochemical *** work remarkably advances the fundamental understanding on mechanochemical properties of transition metal oxide cathode with solid-state synthesis and provides a unified guide for optimization the Ni-rich oxide cathode.

关键词： Ni-rich cathode In situ ETEM solid-state synthesis Multiscale strain alleviation

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Ba_2SbGaS_5 : solid-state synthesis, Crystal and Electronic Structures, and Property Characterization

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Chinese Journal of Structural Chemistry 2013年第4期32卷 538-544页

作者：耿磊张浩程文旦 School of Physics and Electronic Information Huaibei Normal University state Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences

Single crystal of Ba2SbGaSs has been synthesized by the high temperature solidstate reaction method. The compound crystallizes in the orthorhombic space group Pnma with a = 12.177（4）, b = 8.880（3）, c = 8.982（3） A, V= 971.4（6） A3, Z = 4, De = 4.284 g/cm3,μ = 14.487 mm-1, F（000） - 1096, the final R = 0.0171 and wR = 0.0384 for all data. The structure comprises an infinite one-dimensional 1∞[SbGaS5]4- anionic chain constructed from the GaS4 tetrahedra and the SbS5 polyhedra via sharing edge alternately. The paralleled 1∞[SbGaS5]4anionic chains engage with each other and form the two-dimensional Sb-Ga-S layer perpendicular to a-axis with the isolated Ba2＋ cations arranged between layers. The IR spectrum and the UV-Vis spectrum have been investigated. Also, the first-principles band structure and density of states calculations indicate that the compound belongs to indirect semiconductor with the band gap of 2.1 eV, which is supported by the UV-Vis diffuse reflectance results.

关键词： crystal structure solid-state synthesis X-ray diffraction,electronic structure calculation

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An Efficient solid-state synthesis of N-Aryl-2-phenyldiazenecarboxamides

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Chinese Chemical Letters 2001年第2期12卷 107-108页

作者： Jian Ping LI Qian Fu LUO Yi Yang SHEN Yu Lu WANG Hong WANG College of Chemistry and Environmental Science Henan Normal UniversityXinxiang 453002 Department of Chemistry Luoyang Teacher’s CollegeLuoyang 471000

A new and ancient solid-state reaction using K3Fe(CN)(6)/KOII to oxidize diaryl semicarbazides for preparing azo compounds has been reported. Nine N-aryl-2-phenyl-diazenecarboxamides have been synthesized in excellent... 详细信息

关键词： solid-state synthesis diaryl semicarbazide N-Aryl-2-phenyldiazenecarboxamide

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Carbon Nitride Nanowire Bundle and Tubes:solid-state synthesis,Characterization and Photoluminescent Properties

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Chemical Research in Chinese Universities 2009年第4期25卷 412-416页

作者： ZHAO Peng WANG Bai-nian CHEN Xiang-ying QIAN Yi-tai School of Chemical Engineering Hefei University of Technology Hefei 230009 P. R. China Hefei National Laboratory for Physical Sciences at Microscale Department of Chemistry University of Science and Technology of China Hefei 230026 P. R. China

Graphite-like carbon nitride nanowire bundles were synthesized from melamine via the solid state thermolysis at relatively low temperature（400℃）.Hexagonal carbon nitride tubes were prepared for the first time by heating the nanowire bundles at 550 ℃ in argon *** forming process of tubes and transformation of the molecular structures from s-triazine rings to tri-s-triazine units were *** blue and yellow-green emission photoluminescent（PL） properties of the products were investigated in detail,and the reasons for the differences of PL properties between the bundles and tubes were discussed.

关键词： Carbon nitride solid-state synthesis Photoluminescence Melamine

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solid state synthesis and Thermoelectric Properties of Mg-Si-Ge System

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Journal of Materials Science & Technology 2005年第5期21卷 618-622页

作者： Renbo SONG Yazheng LIU Tatsuhiko AIZAWA School of Materials Science and Engineering University of Science and Technology Beijing Beijing 100083 China Center for Collaborative Research The University of Tokyo Komaba 4-6-1 Meguro-ku Tokyo 153-8904 Japan

Thermoelectric materials, Mg2Si1-xGex （x=0, 0.2, 0.4, 0.6, 0.8, 1）, have been prepared by bulk mechanical alloying （BMA） and hot pressing （HP）. The electrical conductivity, Seebeck coefficient and thermal conductivity were measured from room temperature up to about 700 K. The electrical conductivity of all the samples increases with increasing temperature, while the Seebeck coefficient and thermal conductivity decrease with increasing temperature. Mg2Si and Mg2Si0.8Ge0.2 possess negative type of conductivity, while for other compounds it is positive. At the same time, the effect of hot processing condition on thermoelectric properties was also investigated. The maximum figure of merit of Mg2Si0.6Ge0.4 was obtained with the processing parameter of BMA at 600 cycles and hot pressing at 773 K and i GPa for i h.

关键词： solid-state synthesis Mg2Si1-xGex Bulk mechanical alloying Thermoelectric Hot pressing

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Convenient and Efficient solid-state synthesis Of Diaryl Carbazones with NaBrO3／NaHSO4·H2O

Convenient and Efficient Solid-State Synthesis Of Diaryl Car...

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中国化学会第四届有机化学学术会议

作者： Lei Shi Feng Pan Run-Fang Zhang Yu-Lu Wang College of Chemistry and Environmental Science, Henan Normal University, Xinxiang, 453002, P. R. China The Key Laboratory of Environmental Pollution Control Technology of Henan Province,Xinxiang, 453002, P. R. China

＜正＞Diaryl carbazone is an important organic analytical reagent normally prepared by the oxidation of diaryl carbazine, but in literatures’ methods, the yields were low and the procedures were trouble. Recently, our laboratory reported some new methods for the preparation of diaryl carbazone from diaryl carbazine. Generally, these reactions were carried out in solution and have drawbacks such as tedious operation;using large amounts of volatile and poisonous solvent which will pollute the environment inevitably;complicated oxidation system.

关键词： solid-state synthesis Diaryl carbazones NaBrO3/NaHSO4 · H2O.

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A small organic molecule strategy for remedying oxygen vacancies by bismuth defects in BiOBr nanosheet with excellent photocatalytic CO_(2)reduction

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Nano Research 2024年第1期17卷 297-306页

作者： Jing Xie Zhenjiang Lu Yue Feng Jianguo Huang Jindou Hu Aize Hao Yali Cao state Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources College of ChemistryXinjiang UniversityUrumqi 830046China

Defect modulation currently plays a decisive role in addressing the poor photoabsorption,sluggish electron hole separation,and high CO_(2)activation barrier in photocatalytic CO_(2)***,hunting for a straightforward strategy to balance the concentration of oxygen vacancy and metal cation defect in one photocatalyst is still a great ***,a bismuth vacancies BiOBr nanosheets(BiOBr-1)on the exposed[001]facets were constructed via an acetic acid molecule modification strategy,which can repair oxygen defect by bismuth vacancy in low-temperature solid-state chemical *** from the formed bismuth defects that can not only broaden light absorption and elevate charge separation efficiency,but also enhance adsorption and activation of CO_(2)molecules,the evolution rates of photocatalytic CO_(2)conversion into CO(71.23μmol·g^(-1)·h^(-1))and CH4(8.90μmol·g^(-1)·h^(-1))attained by BiOBr-1 are superior 7.1 and 11 times to that of plate-like *** photocatalytic mechanisms including adsorption concentration and activation process of CO_(2)are further revealed by the in situ diffuse reflectance infrared flourier transform spectra(DRIFTS).This finding of the existence of distinct defects in ultrathin nanosheets undoubtedly leads to new possibilities for photocatalyst design using two-dimensional materials with high solar-driven photocatalytic activity.

关键词： solid-state synthesis BiOBr metal vacancies photocatalysis carbon dioxide reduction

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Mechanical densification synthesis of single-crystalline Ni-rich cathode for high-energy lithium-ion batteries

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Journal of Energy Chemistry 2023年第4期79卷 562-568页

作者： Gwonsik Nam Jaeseong Hwang Donghun Kang Sieon Oh Sujong Chae Moonsu Yoon Minseong Ko Division of Convergence Materials Engineering Pukyong National UniversityBusan 48547Republic of Korea Namyang R&D Center Hyundai Motor CompanyHwaseong 18280Republic of Korea Division of Industrial Chemistry and Polymer Engineering Pukyong National UniversityBusan 48547Republic of Korea Department of Nuclear Science and Engineering Massachusetts Institute of TechnologyCambridgeMA 02139USA

The intergranular microcracking in polycrystalline Ni-rich cathode particle is led by anisotropic volume change and stress corrosion along grain boundary,accelerating battery performance ***,we have suggested a simple but advanced solid-state method that ensures both uniform transition metal distribution and single-crystalline morphology for Ni-rich cathode synthesis without sophisticated ***-assisted mechanical densification(PAMD)process on solid-state precursor mixture enables the dynamic mass transfer through the increased solid-solid contact area which facilitates the grain growth during sintering process,readily forming micro-sized single-crystalline ***,the improved chemical reactivity by a combination of capillary effect and vacancyassisted diffusion provides homogeneous element distribution within each primary *** a result,single-crystalline Ni-rich cathode with PAMD process has eliminated a potential evolution of intergranular cracking,thus achieving superior energy retention capability of 85%over 150 cycles compared to polycrystalline Ni-rich particle even after high-pressure calendering process(corresponding to electrode density of~3.6 g cm^(-3))and high cut-off voltage *** work provides a concrete perspective on developing facile synthetic route of micron-sized single-crystalline Ni-rich cathode materials for high energy density lithium-ion batteries(LIBs).

关键词： Lithium-ion batteries Ni-rich cathode materials Mechanical densification solid-state synthesis

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Facile Mechanochemical Preparation of Polyamide-derivatives via solid-state Benzoxazine-isocyanide Chemistry

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Chinese Journal of Polymer Science 2021年第5期39卷 573-584,I0006页

作者： Xu Sun Wei Shi Xin-Yu Zhou Sheng Ding Oil&Gas Field Applied Chemistry Key Laboratory of Sichuan Province College of Chemistry and Chemical EngineeringSouthwest Petroleum UniversityChengdu 610500China

With the exploration of novel sustainable protocol for functional polyamides'(PAs)construction as the starting point,herein,the small molecular model compound(M 1-ssBIC)was prepared firstly by manual grinding of monofunctional benzoxazine(1a)and isocyanide(1 b)via solid-state benzoxazine-isocyanide chemistry(ssBIC)to evaluate the feasibility of *** PAs(P1-series polymers)were subsequently synthesized from biunctional benzoxazine(2a)and isocyanide(2b),and the influence of the loading of catalyst(octylphosphonic acid)(OPA)on the polymerization was ***,two kinds of cross-linked PAs were successfully constructed via ssBIC by using trifunctional benzoxazine(3a)and cross-linked polybenzoxazine(4a)as reaction substrates,respectively,thus verifying the adaptability of *** characterization indicates that amide,phenolic hydroxyl and tertiary amine substructures,with metal-complexing capability,have been successfully integrated into the obtained PAs.A type of representative PA/silver composite(P3-AgNPs)was prepared subsequently via in situ reduction treatment,and its application as recyclable reduction catalyst for organic pollutant p-nitrophenol(4-NP)was preliminarily investigated here to provide the example for possible downstream application of *** think that this current work could provide a new pathway for the construction of functional PAs through facile and sustainable ssBIC protocol.

关键词： Mechanochemistry solid-state synthesis Benzoxazine Isocyanide Polyamide

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Modulating proton binding energy on the tungsten carbide nanowires surfaces for boosting hydrogen evolution in acid

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Journal of Energy Chemistry 2021年第11期30卷 610-616,I0014页

作者： Qjngshui Hong Tangyi Li Shisheng Zheng Haibiao Chen Wenju Ren Honghao Chu Kuangda Xu Zongwei Mei Feng Pan School of Advanced Materials Peking UniversityShenzhen Graduate SchoolShenzhen 518055GuangdongChina School of Advance Manufacturing Engineering Chongqing University of Posts and TelecommunicationsChongqing 400065China

ungsten carbides have attracted wide attentions as Pt substitute electrocatalysts for hydrogen evolution reaction (HER), due to their good stability in an acid environment and Pt-like behaviour in hydrolysis. However, quantum chemistry calculations predict that the strong tungsten-hydrogen bonding hinders hydrogen desorption and restricts the overall catalytic activity. Synergistic modulation of host and guest electronic interaction can change the local work function of a compound, and therefore, improve its electrocatalytic activity over either of the elements individually. Herein, we develop a creative and facile solid-state approach to synthesize self-supported carbon-encapsulated single-phase WC hybrid nanowires arrays (nanoarrays) as HER catalyst. The theoretical calculations reveal that carbon encapsulation modifies the Gibbs free energy of H* values for the WC adsorption sites, endowing a more favorable C@WC active site for HER. The experimental results exhibit that the hybrid WC nanoarrays possess remarkable Pt-like catalytic behavior, with superior activity and stability in an acidic media, which can be compared to the best non-noble metal catalysts reported to date for hydrogen evolution reaction. The present results and the facile synthesis method open up an exciting avenue for developing cost-effective catalysts with controllable morphology and functionality for scalable hydrogen generation and other carbide nanomaterials applicable to a range of electrocatalytic reactions.

关键词： Carbon-encapsulated tungsten carbide solid-state synthesis Self-supported nanoarrays electrode Hydrogen evolution reaction First-principles calculations

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