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Design and preparation of a crosslinkable,oil-resistant,and bio-based elastomer from fumarate

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Science China Chemistry 2024年第2期67卷 622-631页

作者： Hui Yang Haijun Ji Xinxin Zhou Shihan Yang Liwei Li Chaoying Sun Weiwei Lei Runguo Wang Liqun Zhang beijing state key laboratory of organic-inorganic composites&beijing laboratory of Biomedical Materials Beijing University of Chemical TechnologyBeijing100029China Hubei key laboratory of Polymer Materials Faculty of Materials Science and EngineeringHubei UniversityWuhan430062China

Poly(diethyl fumarate-co-methoxyethyl acrylate-co-vinyl chloroacetate)(PDEFMV),a novel bio-based elastomer with a saturated structure,was synthesized via redox emulsion polymerization.The glass-transition temperatures of PDEFMV,adjusted through the variation of the diethyl fumarate-to-methoxyethyl acrylate feeding ratio,ranged from-36.1 to-14.8 ℃.The number-average molecular weights of PDEFMV ranged from 384,000 to 46,000 g/mol.In designing the molecular structure,vinyl chloroacetate was used to provide active sites for subsequent vulcanization and crosslinking.The active chlorine groups within the PDEFMV chain reacted with the crosslinking agent trithiocyanuric acid under high temperature and pressure to form a nonsulfur crosslinked three-dimensional network structure.To achieve the desired properties,carbon black(CB,N330) was incorporated to reinforce PDEFMV,leading to the formation of PDEFMV/CB composites.A comprehensive study was conducted on the high-temperature oil resistance of PDEFMV/CB composites.Following immersion in IRM903 oil at temperatures of 150 and 200 ℃ for 72 h,the mass and volume changes in PDEFMV/CB were lower than those observed in commercially available acrylate rubber(AR)/CB,indicating that PDEFMV exhibited superior oil resistance.Furthermore,the aging characteristics and mechanisms of oil resistance in the PDEFMV/CB and AR/CB composites were investigated at different temperatures(150,200,and 250 ℃).The results provide insights into the operational temperature ranges suitable for PDEFMV/CB and offer valuable guidance for potential industrial applications.

关键词： diethyl fumarate molecular design bio-based elastomer solvent-free synthetic route high-temperature oil resistance

Direct ink writing of multifunctional gratings with gel-like MXene/norepinephrine ink for dynamic electromagnetic interference shielding and patterned Joule heating

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Nano Research 2024年第3期17卷 1585-1594页

作者： Pei-Zhu Jiang Zhiming Deng Peng Min Lvxuan Ye Cheng-Zhang Qi Hao-Yu Zhao Ji Liu Hao-Bin Zhang Zhong-Zhen Yu beijing key laboratory of Advanced Functional Polymer composites Beijing University of Chemical TechnologyBeijing 100029China state key laboratory of organic-inorganic composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China School of Chemistry CRANN and AMBERTrinity College DublinDublin D02PN40Ireland

Intelligent electromagnetic interference(EMI)shielding modulators with a wide tuning range and cyclic stability are urgently needed but their fabrication remains challenging.A gel-like MXene/norepinephrine ink is developed and multifunctional MXene gratings with wide EMI shielding effectiveness(SE)tuning range,superior reversibility,and high mechanical flexibility are constructed by direct ink writing approach for dynamic EMI shielding and patterned Joule heating applications.The modulable MXene/norepinephrine grating with a high conductivity of 3510 S·cm-1 can conveniently realize the seamless modulation of the EMI SE by adjusting the angle between the MXene grating filaments and the electric field of the incident electromagnetic waves,offering highly reversible switching between shielding“On”(28.0 dB)and“Off”(0.5 dB)states.Notably,due to the optimized integration of the MXene ink and the rationally designed pattern,a superior specific EMI SE of 95,688.2 dB·cm^(2)·g^(-1) is achieved in the“On”state.Furthermore,the MXene/norepinephrine ink can be used to fabricate many complex patterned gratings with superior stability,instant responsibility,and superb mechanical flexibility,exhibiting a unique patterned Joule heating behavior.Direct writing of multifunctional gratings paves a means for developing intelligent EMI shielding materials,wearable electronic devices,and advanced thermal management materials.

关键词： MXene ink direct ink writing electromagnetic interference shielding multifunctional gratings Joule heating

Simultaneously Improved Curing,Mechanical,Antioxidative Properties and Reduced ZnO Loading of Silica Filled NR composites by Incorporation of Low-cost Crude Carbon Dots via Conventional Melt-milling Method

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Chinese Journal of Polymer Science 2024年第6期42卷 815-825页

作者： Chao-Ying Sun Hai-Jun Ji Li-Wei Li Hui Yang Xiao-Peng An Yi-Ping Chen Ming-Jian Han Can Jiang Li-Qun Zhang Peng Yu Run-Guo Wang state key laboratory of organic-inorganic composites Beijing University of Chemical TechnologyBeijing100029China School of Materials Science and Engineering Wuhan Institute of TechnologyWuhan430205China

Rubbers or elastomers play an important role in hi-tech technology and civilian daily life because of their unique and strategical properties.Generally,the rubber additives are essential components for rubbers’practical application.Nowadays,developing novel multifunctional additives has attracted increasing research attention.In this work,low-cost crude carbon dots(CCDs)were used as multifunctional additives for natural rubber/silica system(without any additional modification)through industrial compatible melt-mixing method.The results revealed that the CCDs could disperse well in the NR/silica system,and they could not only endow the rubber compound with excellent anti-aging capability due to CCDs’radical scavenging activity because of their plenty of nitrogen-containing species,but also improve the curing rate and mechanical performance of the rubber composite.Also,the CCDs could reduce the rolling resistance of the rubber composites(tanδvalue at 7%strain of the rubber composite could be decreased by 34%),which is promising for the application of energy-saving tire industry.Lastly,the addition of CCDs could effectively reduce the ZnO dosage by at least 40%in the rubber composite without deteriorating its performance.Overall,this work provides valuable guidance to develop novel cheap yet effective additives for the elastomer.

关键词： Natural rubber Crude carbon dots Antioxidant ZnO reduction Vulcanization

Highly Conductive Ag/pCF/MVQ Composite Rubber for Efficient Electromagnetic Interference Shielding

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Chinese Journal of Polymer Science 2024年第6期42卷 864-873页

作者： Yang Chen Xiao-Ming Shao Liang He Yi-Nuo Xu Qi-Yuan Yao Ding Feng Wen-Cai Wang state key laboratory of organic-inorganic composites Beijing University of Chemical TechnologyBeijing100029China key laboratory of beijing City for Preparation and Processing of Novel Polymer Materials Beijing University of Chemical TechnologyBeijing100029China Sino-german School of Engineering Qingdao University of Science and TechnologyQingdao266400China

In this study,flexible and highly conductive composite rubber at low filler content was successfully prepared through polydopamine-assisted electroless silver plating plus mechanical mixing.Firstly,carbon fibers(CF)were activated by polydopamine(PDA)to improve the surface activity by self-polymerization reaction.Next,because of the metal chelating ability of PDA,silver layer was firmly deposited on the surface of CF through a facile electroless silver plating method.Finally,flexible silver-plated carbon fibers(Ag/pCF)silicone rubber composites prepared by mechanical mixing.By using X-ray photoelectron spectroscopy(XPS)and X-ray diffraction(XRD),the chemical composition and crystal structure of Ag/pCF were examined,and scanning electron microscopy(SEM)was used to assess the surface morphology of the Ag/pCF.The results showed that a uniform and dense silver layer was formed on the surface of the CF,and the conductivity of the Ag/pCF could reach 7885 S/cm.It was noteworthy that the composite rubber filled with only 45 phr Ag/pCF had a high electromagnetic interference shielding effectiveness(100 dB)due to the low density and high aspect ratio of Ag/pCF.The composite rubber has excellent potential for application in the field of electromagnetic interference shielding.

关键词： Carbon fibers Polydopamine Electroless plating Silver Electromagnetic interference shielding

Electrochemical converting ethanol to hydrogen and acetic acid for large scale green hydrogen production

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Nano Research 2024年第3期17卷 1542-1551页

作者： Yufeng Zhang Wei Zhu Jinjie Fang Zhiyuan Xu Yanrong Xue Jiajing Pei Rui Sui Xingdong Wang Xuejiang Zhang Zhongbin Zhuang state key Lab of organic-inorganic composites and beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing 100029China laboratory of Advanced Functional Materials of Nanjing Nanjing Xiaozhuang UniversityNanjing 211171China beijing key laboratory of Energy Environmental Catalysis Beijing University of Chemical TechnologyBeijing 100029China

Electrochemical coupling hydrogen evolution with biomass reforming reaction(named electrochemical hydrogen and chemical cogeneration(EHCC)),which realizes green hydrogen production and chemical upgrading simultaneously,is a promising method to build a carbon-neutral society.Herein,we analyze the EHCC process by considering the market assessment.The ethanol to acetic acid and hydrogen approach is the most feasible for large-scale hydrogen production.We develop AuCu nanocatalysts,which can selectively oxidize ethanol to acetic acid(>97%)with high long-term activity.The isotopic and in-situ infrared experiments reveal that the promoted water dissociation step by alloying contributes to the enhanced activity of the partial oxidation reaction path.A flow-cell electrolyzer equipped with the AuCu anodic catalyst achieves the steady production of hydrogen and acetic acid simultaneously in both high selectivity(>90%),demonstrating the potential scalable application for green hydrogen production with low energy consumption and high profitability.

关键词： selective ethanol electrooxidation gold alloy catalyst electrochemical-coupled hydrogen production market assessment interfacial water activation

Micro-sized nanoaggregates:Spray-drying-assisted fabrication and applications

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Particuology 2024年第2期85卷 22-48页

作者： Dan-Lei Yang Rong-Kun Liu Yan Wei Qian Sun Jie-Xin Wang School of Life Sciences and Chemical Engineering Jiangsu Second Normal UniversityNanjing210013China state key laboratory of organic-inorganic composites Beijing University of Chemical TechnologyBeijing100029China Guangxi key laboratory of Petrochemical Resource Processing and Process Intensification Technology School of Chemistry and Chemical EngineeringGuangxi UniversityNanning530004China

The applications of nanoparticles suffer from their extremely small size and intrinsic trend of agglom-eration.Rearranging nanoparticles to form micro-sized nanoaggregates(MNAs)with increased size,ordered structure,as well as controllable size,shape,and morphology is a crucial step in various fields of science and technology to maintain the unique characteristics of nanoparticles while obtaining greatly enhanced or new performance at the microscale.The structure of MNAs prominently affects their functionality,which is determined by the arrangement of nanoparticles and the interaction between primary particles.Several methods have been proposed to prepare the MNAs,in which spray-drying technology stands out considering the feasibility,scalability for industry,cost,and efficiency.Forced assembly of nanoparticles through spray-drying under tunable process parameters yields diverse physical properties and structural arrangements of nanoparticles of the MNAs,they therefore exhibit enormous potential in a wide range of application fields.This review presents the construction and applications of spray-dried MNAs.The factors that influence the size,morphology,and structure of the MNAs are discussed in detail.In addition,the outstanding application performance resulting from the tightly packed nanoparticles in regular-shaped MNAs obtained by the spray-drying process is illustrated.

关键词： Spray-drying Micro-sized nanoaggregates Applications

Designed imidazole-based supramolecular catalysts for accelerating oxidation/hydrolysis cascade reactions

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Nano Research 2024年第6期17卷 4916-4923页

作者： Yuanxi Liu Wenjie Xu Shichao Xu Haifeng Wu Baoli Zhang Li Song Zhen-Gang Wang state key laboratory of organic-inorganic composites Key Lab of Biomedical Materials of Natural Macromolecules(Ministry of Education)Beijing Laboratory of Biomedical MaterialsCollege of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China National Synchrotron Radiation laboratory CAS Center for Excellence in NanoscienceUniversity of Science and Technology of ChinaHefei 230029China

Reconstructing enzymatic active sites presents a significant challenge due to the intricacies involved in achieving enzyme-like scaffold folding and spatial arrangement of essential functional groups.There is also a growing interest in building biocatalytic networks,wherein multiple enzymatic active sites are localized within a single artificial system,allowing for cascaded transformations.In this work,we report the self-assembly of imidazole or its derivatives with fluorenylmethyloxycarbonyl-modified histidine and Cu2+to fabricate a supramolecular catalyst,which possesses catechol oxidase-like dicopper center with multiple imidazole as the coordination sphere.Transmission electron microscopy,low-temperature X-band continuous-wave electron paramagnetic resonance,K-edge X-ray absorption spectra/the extended X-ray absorption fine structure analysis,and density functional theory modeling were used for the structural characterization of the catalyst.The phenol derivatives and the dissolved oxygen were used as the substrates,with the addition of 4-aminoantipyrine to generate a red adduct with a maximum absorbance at 510 nm,for obtaining time-dependent absorbance change curves and estimating the activities.The results reveal that the addition of imidazole synergistically accelerates the oxidative activity about 10-fold and the hydrolysis activity about 14-fold than fluorenylmethyloxycarbonyl modified-histidine/Cu2+.The supramolecular nanoassembly also exhibits the ability to catalyze oxidation/hydrolysis cascade reactions,converting 2′,7′-dichlorofluorescin diacetate into 2′,7′-dichlorofluorescein.This process can be regulated through the methylation of the imidazole component at various positions.This work may contribute to the design of advanced biomimetic catalysts,and shed light on early structural models of the active sites of the primitive copper-dependent enzymes.

关键词： enzyme mimic self-assembly supramolecular catalyst cascade reactions

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 electrodeposition.However,the synthesis of Al nanowires(NWs)is still challenging from the stable alumina substrate.In this work,the Ni-catalyzed fabrication of Al NWs has been realized using various Al_(2)O_(3) substrates.The 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 investigated.The growth of Al NWs correlates with the Na addition to the alumina support.Since 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 mechanism.The 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

Hydrothermal synthesis of polyimide-linked covalent organic frameworks towards ultrafast and stable cathodic sodium storage

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Science China Chemistry 2024年第4期67卷 1300-1310页

作者： Xiya Yang Lei Gong Zhixin Liu Qianjun Zhi Baoqiu Yu Xin Chen Kang Wang Xiaofeng Li Dongdong Qi Jianzhuang Jiang beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China state key laboratory of organic-inorganic composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Redox-active organic materials are capturing growing attention as cathode materials for sustainable alkaline metal ion batteries.However,the storage of Na+in most organic materials-based cathodes is plagued by low capacity and unsatisfying rate performance due to their low active site densities and limited exposed active sites.Herein,two polyimide-linked covalent organic frameworks(COFs),namely HATN-PD-COF and HATN-TAB-COF,were fabricated from hydrothermal synthesis with redoxactive triphenylene-2,3,6,7,10,11-hexacarboxylic acid and aromatic amines as starting materials.Powder X-ray diffraction and electron microscopy analysis indicate the high crystalline nature of these COFs with AA stacking configuration and orderly mesoporous tunnel.N_(2) sorption measurement discloses the permanent porosity of these two COFs with a Brunauer-EmmettTeller surface area of 1,065-1,200 m^(2)g^(-1)and a large pore size of 2.0-3.1 nm.Galvanostatic intermittent titration technique and density functional theory calculations reveal the facile Na+ion diffusion along the mesoporous tunnel of these COFs with a small energy barrier of 0.13-0.40 e V.In particular,the as-prepared COFs based-cathodes show ultrafast and stable Na+storage associated with their conjugated electronic structure,highly ordered mesoporous tunnel,robust structure,and redox-active C=N/C=O-rich framework as exemplified by the high reversible capacity of 210 m A h g^(-1)at 200 m A g^(-1),record-high rate performance(195 m A h g^(-1)at a high current density of 10,000 m A g^(-1))among organic electrodes and the capacity retention of nearly 91%at 10,000 m A g^(-1)after 7,000 cycles for HATN-PD-COF.

关键词： covalent organic framework sodium ion battery cathode high rate organic electrode