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Cationic ordering transition in oxygen-redox layered oxide cathodes

Carbon Energy 2024年第1期6卷 197-206页

作者： Xinyan Li ang Gao Qinghua zhang Hao Yu Pengxiang Ji Dongdong Xiao Xuefeng Wang Dong Su Xiaohui Rong Xiqian Yu hong Li Yong-Sheng Hu Lin Gu Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijingChina College of Materials Science and Opto-Electronic Technology University of Chinese Academy of SciencesBeijingChina Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials School of Materials Science and EngineeringTsinghua UniversityBeijingChina Beijing Advanced Innovation Center for Materials Genome Engineering Huairou DivisionInstitute of PhysicsChinese Academy of SciencesBeijingChina

Understanding the structural origin of the competition between oxygen 2p and transition-metal 3d orbitals in oxygen-redox(OR)layered oxides is eminently desirable for exploring reversible and high-energy-density Li/Na-ion ***,we reveal the correlation between cationic ordering transition and OR degradation in ribbon-ordered P3-Na_(0.6)Li_(0.2)Mn_(0.8)O_(2) via in situ structural *** two different voltage windows,the OR capacity can be improved approximately twofold when suppressing the in-plane cationic ordering *** find that the intralayer cationic migration is promoted by electrochemical reduction from Mn^(4+)to Jahn–Teller Mn^(3+)and the concomitant NaO_(6) stacking transformation from triangular prisms to octahedra,resulting in the loss of ribbon ordering and electrochemical ***-principles calculations reveal that Mn^(4+)/Mn^(3+)charge ordering and alignment of the degenerate eg orbital induce lattice-level collective Jahn–Teller distortion,which favors intralayer Mn-ion migration and thereby accelerates OR *** findings unravel the relationship between in-plane cationic ordering and OR reversibility and highlight the importance of superstructure protection for the rational design of reversible OR-active layered oxide cathodes.

关键词： cationic ordering layered oxide cathodes oxygen redox sodium-ion batteries

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A new class of crystalline X-ray induced photochromic materials assembled from anion-directed folding of a flexible cation

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Chinese Chemical Letters 2024年第8期35卷 554-557页

作者： hong-Jin Liao zhu zhuo Qing Li Yoshihito Shiota Jonathan P.Hill Katsuhiko Ariga zi-Xiu Lu Lu-Yao Liu zi-ang Nan Wei Wang You-Gui Huang 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 350002China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstitutesChinese Academy of SciencesXiamen 361021China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China Institute for Materials Chemistry and Engineering Kyushu UniversityFukuoka 819-0395Japan World Premier International(WPI)Center for Materials Nanoarchitectonics(MANA) National Institute for Materials Science(NIMS)Ibaraki 305-0044Japan

Electron-deficient viologens are widely used as ligands or structure-directing agents(SDAs)to synthesize crystalline X-ray induced photochromic ***,a new rational strategy of anion-directed fold-ing a flexible cation(H_(2)imb)^(2+)((H_(2)imb)^(2+)=di-protonated 2,3-bis(imidazolin-2-yl)-2,3-dimethylbutane)has been ***-donating Cl−and(znCl4)2−are used to direct folding a flexible electron-deficient(H_(2)imb)^(2+)*** complexes(H_(2)imb)(NO_(3))2(1),(H_(2)imb)Cl2·H_(2)O(2),and(H_(2)imb)znCl4(3)have been synthesized in which(H_(2)imb)^(2+)crystallize in an anti-conformation,88.8°-gauche,and 51.8°-gauche,*** contrary to X-ray silent complex 1,X-ray induced photochromism has been achieved in both complex 2 and *** intermolecular charge-transfer mechanism has been elucidated and the anion directed folding of(H_(2)imb)^(2+)has been validated to be critical to yield colored long-lived charge-separated states.

关键词： Supramolecular Photochromic X-ray induced Anion-directed folding Electron-deficient viologens

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Interface catalytic reduction of alumina by nickle for the aluminum nanowire growth: Dynamics observed by in situ TEM

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Nano Research 2024年第3期17卷 1225-1231页

作者： zichun Wang Dan Wang ang Li Lizhuo Wang Xiaodong Han Yijiao Jiang Jianfeng Chen Jun Huang Beijing Advanced Innovation Center for Soft Matter Science and Engineering State Key Laboratory of Organic–Inorganic CompositesBeijing University of Chemical TechnologyBeijing 100029China Laboratory for Catalysis Engineering School of Chemical and Biomolecular EngineeringThe University of SydneyNew South Wales 2006Australia Beijing Key Laboratory of Microstructure and Property of Advanced Materials Beijing University of TechnologyBeijing 100024China Department of Engineering Macquarie UniversitySydneyNew South Wales 2109Australia

Metal nanowires show promise in a broad range of applications and can be fabricated via a number of methods,such as vapor–liquid–solid process and template-based ***,the synthesis of Al nanowires(NWs)is still challenging from the stable alumina *** this work,the Ni-catalyzed fabrication of Al NWs has been realized using various Al_(2)O_(3) *** growth dynamics of Al NWs on Ni/Al_(2)O_(3) was studied using in situ transmission electron microscopy(TEM).The effect of alumina structures,compositions,and growth temperature were *** growth of Al NWs correlates with the Na addition to the alumina *** no eutectic mixture of nickel aluminide was formed,a mechanism of Ni-catalyzed reduction of Al_(2)O_(3) for Al NWs growth has been proposed instead of the vapor–liquid–solid *** key insights reported here are not restricted to Ni-catalyzed Al NWs growth but can be extended to understanding the dynamic change and catalytic performance of Ni/Al_(2)O_(3) under working conditions.

关键词： in situ transmission electron microscopy(TEM) Al nanowires alumina reduction nanowire growth

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X-ray excited Mn^(2+)-doped persistent luminescence materials with biological window emission for in vivo bioimaging

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Journal of Rare Earths 2024年第1期42卷 28-35,I0001页

作者： Hanrun zheng Lin Liu Yi’ang Li Rui Rong Liang Song Junpeng Shi Jing Teng Xia Sun Yun zhang State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China University of the Chinese Academy of Sciences Beijing100049China Xiamen Hospital of Traditional Chinese Medicine Xiamen361015China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou350108China

In recent years,persistent luminescence materials(PLMs)excited by X-rays and emitting in biological windows have received extensive attention in the field of high-sensitivity *** metal Mn^(2+)is an ideal emission center,but few studies focus on Mn^(2+)-doped PLMs with X-ray excitation and biological window ***,we report a Mn^(2+)-doped PLM,LiYGeO_(4):Mn^(2+)(LYGM),with excellent biological window persistent luminescence *** excitation by UV,LYGM produces a durable biological window of persistent luminescence emission at 660 nm for up to 20 *** *** can be repeatedly excited by X-rays,resulting in long-term biological window persistent luminescence *** addition,we obtain LYGM around 200 nm in diameter by ball milling and centrifugation and improve its biocompatibility by surface modification to apply it to in vivo imaging in *** LYGM are injected into mice through the tail vein,in situ excitation of X-rays can be *** the persistent luminescence decays,LYGM can be re-excited for repeated ***,LYGM shows potential prospects for in vivo deep tissue and long-term bioimaging.

关键词： Persistent luminescence X-ray Biological window In vivo imaging Rare earths

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Effects of longitudinal magnetic field on primary dendrite spacing and segregation of directionally solidified single crystal superalloy

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Progress in Natural Science:Materials International 2024年第1期34卷 26-36页

作者： Congjiang zhang Yilin zhou Chen Shen Weili Ren Xiaotan Yuan Biao Ding Haibiao Lu zuosheng Lei Yunbo zhong ang zhang State Key Laboratory of Advanced Special Steel College of Materials Science and Engineering Shanghai University National Engineering Research Center for Magnesium Alloys Natural Key Laboratory of Advanced Casting Technologies College of Materials Science and EngineeringChongqing University

The primary dendrite spacing(PDS) and segregation of directionally solidified single crystal(SC) superalloy under the longitudinal magnetic field(LMF) were investigated based on the analysis of the whole cross-sectional microstructure at different solidification distances. The results show that the PDS under the LMF remains basically unchanged at different solidification distances, and it is greater than that under no LMF. With the increase of magnetic field intensity, the PDS increases and the macrosegregation decreases. The increasing PDS and reducing segregation under the LMF can be attributed to the increase of solute boundary layer, which expands the non-equilibrium freezing temperature range and brings the effective partition coefficient closer to 1. The increase of the solute enrichment layer thickness could be caused by the downward secondary circulation generated by the thermoelectric magnetic convection(TEMC) near the interface, which drives the migration of solutes towards the interdendritic region. This work not only clarifies the mechanism of LMF controlling PDS and reducing segregation by TEMC, but also provides theoretical guidance for producing high-quality SC superalloys using magnetic fields.

关键词： Primary dendrite spacing Segregation Single crystal superalloy Directional solidification Magnetic field Thermoelectric magnetic convection

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Anion-induced electrolyte chemistry enables high energy density primary battery for ultralow-temperature conditions

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Science China Chemistry 2024年

作者： zi-Hang Xue Hao-Jie Liang Yong-Li Heng Jia-Lin Yang Edison Huixiang ang hong-Yan Lü hong Yu Dong-Mei Dai Dai-Huo Liu Chuan-Yu zheng Wei Guo Xing-Long Wu Department of Chemistry Northeast Normal University MOE Key Laboratory for UV Light-Emitting Materials and Technology Northeast Normal University Natural Sciences and Science Education National Institute of Education Nanyang Technological University State Key Laboratory of Solidification Processing Center of Advanced Lubrication and Seal Materials Northwestern Polytechnical University School of Chemistry and Chemical Engineering Henan Normal University Key Laboratory of Organo-Pharmaceutical Chemistry of Jiangxi Province Gannan Normal University

Lithium/fluorinated-carbon（Li/CFx） primary batteries are widely used in defense and military fields due to their stable discharge plateau, low self-discharge rate, and adaptability across a wide temperature range. However, enhancing their overall energy density and discharge capacity at low temperatures remains a critical challenge. Herein, we report a strategically designed LiBF4-based sulfite/carboxylate electrolyte, where the anion-involved solvation structure significantly enhances electrochemical kinetics by reducing the desolvation barrier. Simultaneously, it introduces a radical reaction mechanism that contributes to additional capacity. As a result, the Li/CFxprimary batteries with this formulated electrolyte deliver a specific capacity of 2,257.15 mAh g-1at 25 °C. More importantly, when operating at -40 °C, the batteries exhibit an exceptionally high discharge capacity of 1,549.4 m Ah g-1and an energy density of 2,868.6 Wh kg-1. Even at -60 °C, the Li/CFxcells achieve a specific capacity of 444.3 mAh g-1and an energy density of 821.8 Wh kg-1at 0.1 C, significantly outperforming previously reported organic-based liquid electrolytes. This work offers a viable strategy for enhancing the specific capacity and energy density of primary batteries in extreme environments, providing valuable insights for future developments.

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Reconcile the contradictory wettability requirements for the reduction and oxidation half-reactions in overall CO_(2) photoreduction via alternately hydrophobic surfaces

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Journal of Energy Chemistry 2024年第6期93卷 202-212,I0006页

作者： Hailing Huo Ting Hu Chengxi Huang Fang Wu Tongyu Wang Xuan Liu Liang zhang Qiang Ju zhiqing zhong hongbin Xing Erjun Kan ang Li MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing Nanjing University of Science and TechnologyNanjing 210094JiangsuChina College of Information Science and Technology Nanjing Forestry UniversityNanjing 210037JiangsuChina

The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and H_(2)O into fuels represents a promising renewable energy conversion *** a typical redox reaction,the OPCRR involves two half-reactions:the CO_(2) reduction half-reaction(CRHR)and the water oxidation half-reaction(WOHR).Generally,both half-reactions can be promoted by adjusting the wettability of ***,there is a contradiction in wettability requirements for the two ***,CRHR prefers a hydrophobic surface that can accumulate more CO_(2) molecules on the active sites,ensuring the appropriate ratio of gas-phase(CO_(2))to liquid-phase(H_(2)O)***,the WOHR prefers a hydrophilic surface that can promote the departure of the gaseous product(O_(2))from the catalyst surface,preventing isolation between active sites and the reactant(H_(2)O).Here,we successfully reconciled the contradictory wettability requirements for the CRHR and WOHR by creating an alternately hydrophobic *** was achieved through a selectively hydrophobic modification method and a charge-transfer-control ***,the collaboratively promoted CRHR and WOHR led to a significantly enhanced OPCRR with a solar-to-fuel conversion efficiency of 0.186%.Notably,in ethanol production,the catalyst exhibited a 10.64-fold increase in generation rate(271.44μmol g^(-1)h~(-1))and a 4-fold increase in selectivity(55.77%)compared to the benchmark *** innovative approach holds great potential for application in universal overall reactions involving gas participation.

关键词： Hydrophobic Hydrophilic Gas transport Overall CO_(2)photoreduction z-scheme

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NiS ultrafine nanorod with translational and rotational symmetry

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National Science Review 2024年第7期11卷 218-225页

作者： Jianxin Kang Qi Hu Ruixuan zhang ang Gao zhongning Huang ziming Su Ke Pei Qinghua zhang Li-Min Liu Renchao Che Lin Gu Er-Jia Guo Lin Guo School of Chemistry Beihang University Laboratory of Advanced Materials Shanghai Key Lab of Molecular Catalysis and Innovative Materials Academy for Engineering&Technology Fudan University zhejiang Laboratory Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials School of Materials Science and Engineering Tsinghua University Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of Sciences School of Physics Beihang University

Anisotropy is a significant and prevalent characteristic of materials, conferring orientation-dependent properties, meaning that the creation of original symmetry enables key functionality that is not found in nature. Even with the advancements in atomic machining, synthesis of separated symmetry in different directions within a single structure remains an extraordinary challenge. Here, we successfully fabricate NiS ultrafine nanorods with separated symmetry along two directions. The atomic structure of the nanorod exhibits rotational symmetry in the radial direction, while its axial direction is characterized by divergent translational symmetry, surpassing the conventional crystalline structures known to date. It does not fit the traditional description of the space group and the point group in three dimensions, so we define it as a new structure in which translational symmetry and rotational symmetry are separated. Further corroborating the atomic symmetric separation in the electronic structure, we observed the combination of stripe and vortex magnetic domains in a single nanorod with different directions, in accordance with the atomic *** manipulation of nanostructure at the atomic level introduces a novel approach to regulate new properties finely, leading to the proposal of new nanotechnology mechanisms.

关键词： separated symmetry NiS anisotropy structure atomic machining magnetic domain

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Negative enthalpy alloys and local chemical ordering:a concept and route leading to synergy of strength and ductility

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National Science Review 2024年第4期11卷 172-184页

作者： zibing An Tao Yang Caijuan Shi Shengcheng Mao Lihua Wang ang Li Wei Li Xianmeng Xue Ming Sun Yifan Bai Yapeng He Fuzeng Ren zhouguang Lu Ming Yan Yang Ren Chain-Tsuan Liu ze zhang Xiaodong Han Beijing Key Lab of Microstructure and Property of Advanced Materials College of Materials Science &Engineering Beijing University of Technology Department of Materials Science and Engineering City University of Hong Kong Key Laboratory of Partial Acceleration Physics& Technology Institute of High Energy PhysicsChinese Academy of Sciences Department of Materials Science &Engineering Southern University of Science and Technology Department of Physics City University of Hong Kong State Key Laboratory of Silicon Materials Department of Materials Science and Engineering Zhejiang University

Solid solutions are ubiquitous in metals and alloys. Local chemical ordering(LCO) is a fundamental sub-nano/nanoscale process that occurs in many solid solutions and can be used as a microstructure to optimize strength and ductility. However, the formation of LCO has not been fully elucidated, let alone how to provide efficient routes for designing LCO to achieve synergistic effects on both superb strength and ductility. Herein, we propose the formation and control of LCO in negative enthalpy alloys. With engineering negative enthalpy in solid solutions, genetic LCO components are formed in negative enthalpy refractory high-entropy alloys(RHEAs). In contrast to conventional ‘trial-and-error' approaches, the control of LCO by using engineering negative enthalpy in RHEAs is instructive and results in superior strength(1160 MPa) and uniform ductility(24.5%) under tension at ambient temperature, which are among the best reported so far. LCO can promote dislocation cross-slip, enhancing the interaction between dislocations and their accumulation at large tensile strains; sustainable strain hardening can thereby be attained to ensure high ductility of the alloy. This work paves the way for new research fields on negative enthalpy solid solutions and alloys for the synergy of strength and ductility as well as new functions.

关键词： negative enthalpy alloys local chemical ordering strength ductility dislocation

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创造性执行的定位与调适策略研究——基于z省Q市环境医院项目执行过程的个案分析

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中国行政管理 2024年第5期40卷 28-36页

作者：徐强吴昂中国人民大学生态环境学院北京100872 中国人民大学法学院北京100872

创造性执行是新一届政府提出的施政要求。就其本质而言,创造性执行可被视为政策执行活动的一种细分类型,创造性执行的核心要义是服务高质量发展导向下执行方式的灵活创新,以服务发展目标补充、强化、平衡、修正原政策的形式目标与实质精... 详细信息

创造性执行是新一届政府提出的施政要求。就其本质而言,创造性执行可被视为政策执行活动的一种细分类型,创造性执行的核心要义是服务高质量发展导向下执行方式的灵活创新,以服务发展目标补充、强化、平衡、修正原政策的形式目标与实质精神,追求政策执行效果的整体提升。在创造性执行中,执行主体需注意与目标群体的调适,通过多种调适策略增进目标群体的理解和接受程度。本文基于对z省Q市环境医院项目执行过程的分析,呈现了创造性执行中执行主体与目标群体的调适过程,其中既包含了与企业平等对话交流和主动服务的对话型策略,也有通过严格监管激发企业需求、借势中央生态环保督察的压力型策略。由此可知,采取多样调适策略增进目标群体的理解和接受,对推动创造性执行具有重要意义。

关键词：创造性执行政策执行互适模型调适策略

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