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Strong and tough chitin hydrogel constructed by dehydration and rehydration strategy

Nano Research 2024年第9期17卷 8192-8199页

作者： Rui-Rui Liu Li-Bo Mao Shu-Hong Yu Division of Nanomaterials and chemistry Hefei National Research Center for Physical Sciences at the MicroscaleDepartment of ChemistryInstitute of Biomimetic Materials and ChemistryAnhui Engineering Laboratory of Biomimetic MaterialsUniversity of Science and Technology of ChinaHefei 230026China institute of Innovative Materials Department of Materials Science and EngineeringDepartment of ChemistrySouthern University of Science and TechnologyShenzhen 518055China

As a renewable,biocompatible,biodegradable soft material,chitin hydrogels have better advantages in stability,antibacterial activity,antifouling,cost,immunogenicity,and so on than most polymer ***,compared with other widely used polymer hydrogels with high strength and toughness,the practical applications of chitin-based hydrogels have been limited by their weak mechanical properties,such as cartilage repair and meniscus ***,we present the design and fabrication of chitin hydrogels with excellent mechanical strength and toughness by a dehydration and rehydration *** sequential dehydration and rehydration processes,the crystalline domains in the chitin hydrogels can be properly *** optimized crystallinity,the elastic modulus of the chitin hydrogels exceeds all previously reported values,and the fracture toughness is even comparable to some synthetic polymer hydrogels,while maintaining a high-water-content of about 80 wt.%.At the same water content,the mechanical properties of the chitin hydrogels are positively correlated with the hydrogel crystallinity,which proves that the change of mechanical properties of hydrogels is not simply dependent on weight *** hydrogels can be further strengthened by incorporating other biopolymers that are intrinsically weak,which makes the hydrogels promising for applications in fields such as cartilage repair and meniscus ***,the hydrogels enable loading and release of water-soluble and poorly water-soluble *** highly extendable strengthening and toughening strategy of chitin and chitin-based biopolymer hydrogels paves the way for their widely applications.

关键词： chitin hydrogel crystallinity rehydration chemical transformation strong and tough

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Photocatalyzed ditrifluoromethylthiolation of alkenes with CF_(3)SO_(2)Na

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Science China chemistry 2024年第2期67卷 587-594页

作者： Fangming Chen Lvqi Jiang Chunyang Hu Jie Liu Wenbin Yi School of chemistry and Chemical Engineering Nanjing University of Science and TechnologyNanjing210094China Key Laboratory of Organofluorine chemistry Shanghai Institute Organic ChemistryChinese Academy of SciencesShanghai200032China

Since the first report of sodium trifluoromethanesulfinate(CF_(3)SO_(2)Na) as an electrophilic trifluoromethylthiolation reagent in 2015,there has been no breakthrough in research in this ***,we disclose an unprecedented usage of CF_(3)SO_(2)Na as a radical trifluoromethylthiolation reagent.A photocatalyzed ditrifluoromethylthiolation of alkenes with CF_(3)SO_(2)Na in the presence of PPh_(3) and catalytic copper has been ***,either Ir[(p-Fppy)_(2)(bpy)]PF_6 or Ir(ppy)_(3) could facilitate this *** studies indicate that initiation of the radical chain proceeded via two different photocatalytic quenching *** protocol provides a practical method for the construction of diverse vicinal ditrifluoromethylthiolated compounds.

关键词： trifluoromethylthiolation photocatalysis radical difunctionalization alkenes

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Si/TiO2 carbon fiber core encapsulated in hierarchical multiple MXene@Co-MoS2 shells for constructing a free-standing anode of lithium storage

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Rare Metals 2024年第9期43卷 4222-4233页

作者： Xian-ping Du Ying Huang Jia-ming Wang Zhen-he Feng Xu Sun MOE Key Laboratory of Material Physics and chemistry Under Extraordinary Conditions School of Chemistry and Chemical Engineering Northwestern Polytechnical University Shanghai institute of Space Power-Sources Ningbo institute of Northwestern Polytechnical university

Silicon-based（Si-based） materials offer more possibilities for generating new portable electronic devices due to their high specific capacities. However, their inferior electrical conductivity and volume expansion during cycling seriously limit their development. The optimum solution is to select specific materials to establish an exceptionally conductive and volume buffer structure,which can assist Si materials in developing their excellent lithium storage properties. In this study, Si particles were confined in TiO2carbon fibers（TiO2CFs） via electrospinning, after which they were encapsulated with MXene and Co-MoS2（CMS） nanosheets to fabricate hierarchical ST-2@MXene@CMS films. TiO2CF, MXene and CMS were employed to establish a coherent conductive network with one-, two-and three-dimensional electronic pathways to permit the unimpeded flow of electrons inside the electrode material. TiO2CF, MXene and CMS acted precisely as multilayered buffers to ameliorate the volume change of Si particles during cycling. In addition, the CMS nanosheets were involved in lithium storage, contributing to the final electrochemical performance. Ultimately, the ST-2@MXene@CMS films served as free-standing electrodes, avoiding the impact of inactive interfaces on the electrochemical performance and fulfilling the lightweight requirement for new energy storage devices.

关键词： Co-MoS2 nanosheets Hierarchical structure Lithium-ion batteries MXene Si particles

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Copper-catalyzed asymmetric dearomatizing amination of 2-naphthols:Csp^(2)–N coupling via 1,3-reductive elimination

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Science China chemistry 2024年第8期67卷 2694-2700页

作者： Aying Yihuo Maoping Pu Zheng Tan Jibang Liao Jiuqi Tan Qi-Lin Zhou Xiaohua Liu Xiaoming Feng Key Laboratory of Green chemistry&Technology Ministry of EducationCollege of ChemistrySichuan UniversityChengdu 610064China Key Laboratory and institute of Elemento-Organic chemistry College of Chemistry Frontiers Science Centerfor New Organic MatterNankai UniversityTianjin300071China

An efficient catalytic asymmetric dearomatizing amination of 2-naphthols and phenols catalyzed by N,N′-dioxide-copper(I)complex as a chiral catalyst was presented.A variety of optically activeβ-naphthalenone compounds with a nitrogen-containing quaternary carbon stereocenter were obtained with high yield and enantioselectivity under mild reaction *** studies indicated that this Csp^(2)–N dearomatizing coupling proceeds via 1,3-reductive elimination of phenolate-Cu~Ⅲ-amino intermediate in five-membered ring transition *** origin of enantioselectivity has also been elucidated based on density functional theory calculations.

关键词： asymmetric catalysis amination dearomatization copper catalysis coupling reaction

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One dimensional CeO_(2) nanorods/poly(ethylene oxide) solid composite electrolyte for all-solid-state lithium-ion batteries

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Journal of Rare Earths 2024年第3期42卷 570-577,I0005页

作者： Yudi Guo Erqing Zhao Xiaofang Zhao Shuailei Liu School of chemistry and Materials Engineering Xinxiang UniversityXinxiang453003China School of chemistry and Chemical Engineering Henan Institute of Science and TechnologyXinxiang453003China

The research of poly(ethylene oxide)(PEO)-based solid composite electrolyte with high ionic conductivity and excellent interfacial stability is the key to the development of all-solid-state lithium-ion batteries(ASSLIBs). Herein, uniform nanorod structured CeO_(2) fillers were controllably synthesized by electrospinning, which were subsequently filled into PEO polymer to prepare CeO_(2)/PEO solid composite electrolyte. The addition of CeO_(2) nanorods can reduce both the glass transition temperature and the melting point of PEO polymer, and also interact with PEO and lithium bis(trifluoromethanesulphonyl)imide(LITFSI) by Lewis acid—base reaction. Therefore, the solid composite electrolyte exhibits a high ionic conductivity of 4.52 × 10^(-4)S/cm, a wide electrochemical stability window of about 4.8 V, and a good interfacial stability with Li at 55℃. Moreover, the LiFePO_4/Li ASSLIB divulges the discharging specific capacity of 165, 162, 156 and 146 mA,h/g at 0.2, 0.5, 1 and 2 C, respectively, and achieves the capacity retention of 90.3% after 150 cycles at 0.5 C. Consequently, one dimensional CeO_(2) nanorods can be considered as an alternative filler for polymeric solid electrolyte.

关键词： Poly(ethylene oxide) Solid composite electrolyte CeO_(2)nanorods Ionic conductivity Rare earths

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Stabilization and detection of labile reaction intermediates in supramolecular containers

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Chinese Chemical Letters 2024年第6期35卷 47-52页

作者： Rui Wang Yang Liang Julius Rebek Jr. Yang Yu Center for Supramolecular chemistry&Catalysis and Department of chemistry College of ScienceShanghai UniversityShanghai 200444China Skaggs institute for Chemical Biology and Department of chemistry The Scripps Research InstituteLa JollaCA 92037United States

Detection and observation of reactive intermediates is an essential step in investigation of reaction ***,most reactive intermediates are unstable and present at low concentrations;their short lifetimes make them difficult to detect and *** containers offer opportunities for the stabilization and characterization of those labile species,through isolation from the media and protection inside the cavity of the *** this review,we summarize the examples of labile reaction intermediates that are stabilized and characterized with the help of supramolecular *** container compounds include carcerands,deep cavitands and amide *** focus on unstable guest species-cyclobutadiene,benzocyclopropenone,o-benzyne,1,2,4,6-cycloheptatetraene,anti-Bredt's olefin,fluorophenoxycarbene,O-acylisoamide,and hemiaminalthat act as intermediates in certain organic reactions.

关键词： Supramolecular containers Reaction intermediates Labile species stabilization Short-lived species detection Supramolecular chemistry

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Molecular Chain Flexibility and Dielectric Loss at High-Frequency:Impact of Ester Bond Arrangement in Poly(ester imide)s

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Chinese Journal of Polymer Science 2024年第8期42卷 1122-1133页

作者： Ya-Dong Li Hong Li Lu-Kun Feng Feng Bao Ming-Liang Wang Cai-Zhen Zhu Zhao-Hui Zheng Xiao-Bin Ding Jian Xu Chengdu institute of Organic chemistry Chinese Academy of SciencesChengdu 610041China university of Chinese Academy of Sciences Beijing 100081China institute of Low-Dimensional Materials Genome Initiative College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060China

The evolution of high-frequency communication has accentuated the significance of controlling dielectric properties in polymer ***,it has been theorized that rigid molecular chains lead to lower dielectric ***,the validity of this proposition at high frequencies remains *** scrutinize the correlation between chain flexibility and dielectric properties,we synthesized six poly(ester imide)s(PEIs)with systematically varied molecular chain flexibilities by modifying the ester's substitution on the aromatic *** introduction of ester bonds bestowed all PEI films with a low dielectric dissipation factor(D_(f)),ranging from 0.0021 to 0.0038 at 10 GHz in dry *** dry D_(f)displayed a pattern consistent with volume polarizability(P/V).Unexpectedly,PI-mmm-T,featu ring the most flexible molecular chain,exhibited the lowest dielectric loss under both dry(0.0021@10 GHz)and hygroscopic(0.0029@10 GHz)***,the observed increase in D_(f)after humidity absorption suggests that the high dielectric loss of PEI in applications may be attributed to its hygroscopic *** simulations and characterization of the aggregation structure revealed that the smaller cavities within flexible molecular chains,after close stacking,impede the entry of water *** sacrificing high-temperature resistance,the precursor exhibited enhanced solubility properties and could be processed into high-quality *** research unveils new insights into the relationship between flexibility and highfrequency dielectric loss,offering innovative perspectives on synthesizing aromatic polymers with exceptional dielectric properties.

关键词： 5G communications Poly(ester imide)s Molecular chain flexibility Dielectric properties Humidity absorption

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Wood anatomy chronologies of Scots pine in the foothills of the Western Sayan(Siberia)

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Journal of Forestry Research 2024年第3期35卷 13-27页

作者： Elena A.Babushkina Dmitry R.Dergunov Mikhail S.Zharkov Liliana V.Belokopytova Dina F.Zhirnova Bao Yang Jingjing Liu Xiaomei Peng Eugene A.Vaganov Khakass Technical institute Siberian Federal UniversityAbakan 655017Russia institute of Ecology and Geography Siberian Federal UniversityKrasnoyarsk 660036Russia Mathematical Methods and IT Department Siberian Federal UniversityKrasnoyarsk 660036Russia Key Laboratory of Desert and Desertification Northwest Institute of Eco-Environment and ResourcesChinese Academy of SciencesLanzhou 730000People's Republic of China School of Geographic and Oceanographic Sciences Nanjing UniversityNanjing 210093People's Republic of China Department of Dendroecology V.N.Sukachev Institute of ForestSiberian Branch of the Russian Academy of ScienceKrasnoyarsk 660036Russia

Recent methodological advances in quantitative wood anatomy have provided new insights into the climatic responses of radial growth at the scale of cell structure of tree rings. This study considered long-term chronologies of tracheid measurements, indexed by a novel approach to separate their specific climatic responses from signal recorded in cell production(closely reflected in tree-ring width). To fill gaps in understanding the impact of climate on conifer xylem structure, Scots pine(Pinus sylvestris L.)trees > 200 years old were selected within the forest-steppe zone in southern Siberia. Such habitats undergo mild moisture deficits and the resulting climatic regulation of growth processes. Mean and maximum values of cell radial diameter and cell wall thickness were recorded for each tree *** a low level of climatogenic stress, components of cell chronologies independent of cambial activity were separated to obtain significant climatic signals revealing the timing of the specific stages of tracheid differentiation. Cell expansion lasted from mid-April to July and was impacted similarly to tree-ring width(stimulated by precipitation and stressed by heat), maximum cell size formed late June. A switch in the climatic responses of mean anatomical traits indicated transition to latewood in mid-July. Secondary wall deposition lasted until mid-September, suppressed by end of season temperatures. Generally, anatomical climatic responses were modulated by a less dry May and September compared with summer months.

关键词： Quantitative wood anatomy Cell radial size Cell wall thickness Pinus sylvestris Climatic response

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Heteroatom doping regulates the catalytic performance of singleatom catalyst supported on graphene for ORR

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Nano Research 2024年第3期17卷 1086-1093页

作者： Ji-Kai Sun Yu-Wei Pan Meng-Qian Xu Lei Sun Shaolong Zhang Wei-Qiao Deng Dong Zhai institute of Molecular Sciences and Engineering Institute of Frontier and Interdisciplinary ScienceShandong UniversityQingdao 266237China College of chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China

Replacing fossil fuels with fuel cells is a feasible way to reduce global energy shortages and environmental ***,the oxygen reduction reaction(ORR)at the cathode has sluggish kinetics,which limits the development of fuel *** is significant to develop catalysts with high catalytic activity of *** single-atom catalysts(SACs)of Pt supported on heteroatom-doped graphene are potential candidates for *** we studied the SACs of Pt with different heteroatoms doping and screened out Pt-C_(4) and Pt-C_(3)O_(1) structures with only 0.13 V overpotential for ***,it is found that B atoms doping could weaken the adsorption capacity of Pt,while N or O atoms doping could enhance *** regularity was verified on Fe *** the electronic interaction analysis between Pt and adsorbate,we explained the mechanism of this regularity and further proposed a new descriptor named corrected d-band center(ε_(d-corr))to describe *** descriptor is an appropriate reflection of the number of free electrons of the SACs,which could evaluate its adsorption *** work provides a purposeful regulatory strategy for the design of ORR catalysts.

关键词： single-atom catalyst(SAC) oxygen reduction reaction(ORR) heteroatom doping corrected d-band center descriptor

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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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