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Manipulating fast Li_(2)S redox via carbon confinement and oxygen defect engineering of In_(2)O_(3)for lithium-sulfur batteries

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Nano Research 2024年第6期17卷 5179-5187页

作者： Jinlei Qin Rui Wang Zilong Yuan Pei Xiao Deli Wang Key Laboratory of Material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Lithium-sulfur(Li-S)batteries have been considered as promising energy storage systems due to the merits of high energy density and low ***,the lithium polysulfides(LiPSs)diffusion and sluggish redox kinetics hamper t... 详细信息

关键词： Li-S batteries nitrogen-doped carbon confinement oxygen vacancies bidirectional Li_(2)S redox

Dual modification of LiNi0.83Co0.11Mn0.06O2 cathode materials by K+ doping and Li3PO4 coating for lithium ions batteries

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Rare Metals 2024年第7期43卷 3007-3018页

作者： Wei Xiao Jia-Le Wang Zhi-Cheng Yi Cheng-Jin Liu Chang Miao Yu Xin Shu-Qing Nie College of chemistry and Environmental Engineering Yangtze University

Li3PO4@Li0.99K0.01Ni0.83Co0.11MnO.06O2（NCM-KP） cathode powders are synthesized via K+doping in calcination processes and H3PO4coating in sol-gel processes.K+precisely enters into the lattice to widen the（003） plane to 0.4746 nm with a lower cationic disordered degree of 1.87%.Moreover,the surface residual lithium salts are treated by H3PO4to generate a uniform Li3PO4coating layer of approximately 11.41 nm,which completely covers on the surface of secondary spherical particles to improve the interfacial *** 25℃,the NCM-KP electrode delivers a discharge specific capacity of 148.9 mAh·g-1with a remarkable capacity retention ratio of 84.1% after 200 cycles at 1.0C and retains a high reversible specific capacity of 154.4 mAh·g-1at *** at 1.0C and 60℃,it can maintain a reversible discharge specific capacity of 114.6 mAh·g-1with 0.21% of capacity decay per cycle after 200 cycles,which is significantly lower than 0.40% for the pristine NCM ***,the charge transfer resistance of 238.89 Ω for the NCM-KP electrode is significantly lower than 947.41 Ω for the pristine NCM one by restricting the interfacial side ***,combining K+doping and Li3PO4coating is an effective strategy to enable the significant improvement of the electrochemical property of high-nickel cathode materials,which may be mainly attributed to the widened diffusion pathway and the formed Li3PO4protective layer,thus promoting Li+diffusion rate and preventing the erosion of HF.

关键词： High-nickel cathode material Residual lithium K + doping Li 3 PO 4 coating Lithium ions battery

In situ crosslink polymerization induced long-lived multicolor supramolecular hydrogel based on modifiedβ-cyclodextrin

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Chinese Chemical Letters 2024年第2期35卷 374-379页

作者： Yonghui Sun Linnan Jiang Yong Chen Yu Liu College of chemistry State Key Laboratory of Elemento-Organic Chemistry Nankai UniversityTianjin 300071China

The construction of hydrogels with good mechanical properties and phosphorescent properties is full of ***,we report a supramolecular phosphorescent hydrogel with long lifetime,high tensile strength and self-healing property,which can be easily constructed through in-situ thermalinitiated polymerization of isocyanatoethyl acrylate-modifiedβ-cyclodextrin(β-CD-DA)and acrylatemodified adamantane(Ad-DA),acrylic acid(AA),followed by the non-covalent association with carbon dots(CNDs).The lifetime of phosphorescent hydrogel can reach 1261 ms at room temperature,and the quantum yield is 11%.Importantly,through the efficient triplet to singlet Förster resonance energy transfer(TS-FRET),the phosphorescent hydrogel shows the good phosphorescence energy transfer property for organic dyes Rhodamine B and Eosin Y with the delayed fluorescence lifetime up to 730 ms and 585 ms as well as the energy transfer efficiency(Φ_(ET))up to 99.9%and 99.3%,***,owing to the host-guest interactions betweenβ-CD-DA and Ad-DA,the three-dimensional cross-linked network phosphorescent hydrogel can be easily stretched to 18 times of its original length,and can achieve self-healing of the cut surfaces within 30 *** results will expand the scope of phosphorescent materials and provide new ideas and opportunities for materials science.

关键词： Room temperature phosphorescence Hydrogel Phosphorescence energy transfer Cyclodextrin Supramolecular interaction

Critical Role of Ethylene-Propylene Block Copolymer in Impact Polypropylene Copolymer

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Chinese Journal of Polymer Science 2024年第3期42卷 344-351,I0007页

作者： Yu-Hui Tang Na Zhang Wei Bao Wei Jiang Yuan Lin Zhao-Hui Su State Key Laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Ethylene-propylene block copolymer(EbP) is a vital component in impact polypropylene copolymer(IPC), yet its distribution in the multiphase composite material and how it influences the phase structure and the mechanical properties are not well understood. In this work,four IPCs were investigated by atomic force microscopy-infrared(AFM-IR) to assess the phase compositions in situ, based on which in conjunction with the chain microstructure information obtained ex situ the distributions of the copolymer components were derived for each alloy. For the IPCs whose EbP comprises long P and long E segments, the EbP fraction was found to phase separate from the rubber and the PP matrix to form the cores of the disperse particles with the E-P segmented copolymer(EsP). In contrast, in the IPC with EbP composed of long P and short E segments, the EbP fraction formed an outer shell for the rubber particles with the cores comprising the EsP alone, and this IPC, containing a lower E comonomer content than its counterpart, exhibited both better impact resistance and higher flexural modulus. These results clarify how the chain structure of EbP governs the phase morphology in IPC, which in turn impacts the properties of the composite material.

关键词： Impact polypropylene copolymers AFM-IR Ethylene-propylene block copolymers Core-shell rubber particles

Liquid-metals-induced formation of MXene/polyacrylamide composite organohydrogels for wearable flexible electronics

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Nano Research 2024年第3期17卷 1913-1922页

作者： Minying Wu Bin Chen Xueliang Fan Tong Ye Yuanyuan Fang Qian Zhang Fangzhou Zhou Yajun Wang Yi Tang Department of chemistry Fudan UniversityShanghai 200433China College of chemistry&Materials Engineering Wenzhou UniversityWenzhou 325027China

Organohydrogels have demonstrated superior environmental adaptability and frost resistance compared to conventional hydrogels,thereby prompting considerable interests in the development and design of innovative ***,we report an effective one-pot method for fabricating MXene/polyacrylamide(MXene/PAM)composite organohydrogel(MAOH)by employing Ga liquid metals(Ga LMs)as a highly reactive component in the induced free radical polymerization reaction,without the need for additional heating or cross-linking *** synthetic protocol addresses the time-consuming and organic solvent waste concerns associated with traditional solvent displacement methods for organohydrogel *** incorporation of MXene not only highly enhances the conductivity but also confers improved mechanical properties of *** MAOH exhibits excellent environmental adaptability(>7 d),sustained moisture retention,remarkable self-healing capabilities,and outstanding mechanical properties under low temperatures(-20℃).It demonstrates exceptional performance in micro-motion monitoring,rapid response time(125 ms),superior stretchability,and a broad range of strains(0.3%–600%).Therefore,the designed MAOH has great potential for applications in diverse fields such as prosthetics,electronic skin,human–machine interaction,and smart terminals.

关键词： organohydrogels MXene conductivity mechanical properties environmental adaptability

Pd-catalyzed intermolecular Si–O formation via Si–C activation

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Science China chemistry 2024年第8期67卷 2661-2669页

作者： Shuang Liu Yu-Shu Chen Yichen Wu Peng Wang State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesShanghai 200032China School of chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China College of Material chemistry and Chemical Engineering Key Laboratory of Organosilicon Chemistryand Material Technology of Ministry of EducationHangzhou Normal UniversityHangzhou 311121China

The development of efficient Si–O bond formation reaction with 100% atom-economy, excellent functional group tolerance, and broad scope under mild conditions is highly desired due to the prevalence of silanol, silyl ether, and their derivatives in synthetic chemistry and materials science. Here, we have realized the Pd-catalyzed Si–O formation reaction via a Si–C activation approach with 100% atom-economy by employing silacyclobutanes(SCBs) and various hydroxy-containing substrates, including water,alcohols, phenols, and silanols. This protocol features a broad substrate scope, remarkable functional compatibility and mild conditions, providing a series of silanols, silyl ethers in high efficiency. Notably, this protocol could also be used for selective protection of hydroxy functionalities, and for the access of a class of novel polymers containing Si–O main chain. Preliminary mechanistic studies unveiled that this reaction underwent a Pd-catalyzed concerted ring-opening mechanism.

关键词： Si–O formation Si–C activation palladium silacyclobutane silanol silyl ether

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Atomic-level coupled RuO_(2)/BaRuO_(3) heterostructure for efficient alkaline hydrogen evolution reaction

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Journal of Energy chemistry 2024年第1期88卷 356-362,I0009页

作者： Yueying Yan Tian Meng Yuting Chen Yang Yang Dewen Wang Zhicai Xing Xiurong Yang State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina

The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction(HER).Optimizing the surface electronic structure of the catalyst to lower the energy barrier of water dissociation and regulating the binding strength of adsorption intermediates are crucial strategy for boosting the catalytic performance of *** this study,RuO_(2)/BaRuO_(3)(RBRO)heterostructures with abundant oxygen vacancies and lattice distortion were in-situ constructed under a low temperature via the thermal decomposition of *** RBRO heterostructures obtained at 550℃ exhibited the highest HER activity in 1 M KOH,showing an ultra-low overpotential of 16 mV at 10 mA cm^(-2)and a Tafel slope of 33.37 m V dec^(-1).Additionally,the material demonstrated remarkable durability,with only 25 mV of degradation in overpotential after 200 h of stability testing at 10 mA cm^(-2).Density functional theory calculations revealed that the redistribution of charges at the heterojunction interface can optimize the binding energies of H*and OH*and effectively lower the energy barrier of water *** research offers novel perspectives on surpassing the water dissociation threshold of alkaline HER catalysts by means of a systematic design of heterogeneous interfaces.

关键词： Heterostructure Hydrogen evolution reaction Interfacial electron transfer Oxygen vacancies

Suppressing the lattice oxygen diffusion via high-entropy oxide construction towards stabilized acidic water oxidation

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Nano Research 2024年第3期17卷 1107-1113页

作者： Jing Ni Zhaoping Shi Yibo Wang Jiahao Yang Hongxiang Wu Pengbo Wang Kai Li Meiling Xiao Changpeng Liu Wei Xing State Key Laboratory of Electroanalytic chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The scale-up deployment of ruthenium(Ru)-based oxygen evolution reaction(OER)electrocatalysts in proton exchange membrane water electrolysis(PEMWE)is greatly restricted by the poor *** the lattice-oxygen-mediated mechanism(LOM)has been identified as the major contributor to the fast performance degradation,impeding lattice oxygen diffusion to inhibit lattice oxygen participation is imperative,yet remains challenging due to the lack of efficient ***,we strategically regulate the bonding nature of Ru–O towards suppressed LOM via Ru-based high-entropy oxide(HEO)*** lattice disorder in HEOs is believed to increase migration energy barrier of lattice *** a result,the screened Ti_(23)Nb_(9)Hf_(13)W_(12)Ru_(43)O_(x) exhibits 11.7 times slower lattice oxygen diffusion rate,84%reduction in LOM ratio,and 29 times lifespan extension compared with the state-of-the-art RuO_(2) *** work opens up a feasible avenue to constructing stabilized Ru-based OER catalysts towards scalable application.

关键词： ruthenium-based high-entropy oxide suppressing the lattice oxygen diffusion acidic oxygen evolution reaction

Dimensional reduction enhances photocatalytic carbon dioxide reduction performance of metal-organic frameworks

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Nano Research 2024年第5期17卷 3653-3659页

作者： Kaiyue Ma Jixin Li Jinlu Liu Chunguang Li Zhan Shi Shouhua Feng State Key Laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China

Metal-organic frameworks(MOFs)have shown significant potential as *** has been widely assumed that all catalytic active sites within MOFs are functional in photocatalytic reactions but for a three-dimensional MOF,whether the internal catalytic active sites can effectively absorb light and actively contribute to photocatalytic reactions remains to be *** this context,we synthesized a two-dimensional nanosheet MOF(2D-MOF)and a three-dimensional bulk MOF(3D-MOF)composed of Zr^(6) clusters and tetracarboxylic porphyrin(TCPP)by the approach described in the ***(bpy)(CO)^(3)Cl(bpy=2,2’-bipyridine),which has remarkable CO_(2) photoreduction ability,was introduced to the two MOFs to create two new photocatalysts 2D-MOF-Re and 3D-MOF-Re,*** CO_(2) reduction experiments show that based on the equal number of catalytic active sites,the CO turnover number(TON)of 2D-MOF-Re reaches 27.8 in 6 h,which is 50 times that of *** result shows that certain catalytic active sites inside the bulk MOF are inactive due to the inability to absorb *** study illuminates the potential of the dimensional reduction approach in the design of photocatalysts to exploit the capabilities fully.

关键词： photocatalysis CO_(2)reduction metal-organic frameworks(MOFs) nanosheets light absorption