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Chinese Journal of Polymer Science 2024年第6期42卷 751-765页

作者： Jun-Hao Zhou Li-Ming Tang key laboratory of advanced materials of ministry of education of china Department of Chemical EngineeringTsinghua UniversityBeijing100084China

In this study,a series of hindered urea bond(HUB)containing polyurethane-urea methacrylate prepolymers and a none HUB containing polyurethane methacrylate prepolymer were prepared using isobornyl methacrylate as the reactive diluent via one-pot *** prepolymers were characterized fully by various ***,their thermosets were fabricated via UV curing in presence of a photo initiator,and their mechanical property and thermal behavior were investigated and *** from the none HUB containing thermoset,the HUB containing thermosets(defined as PUT)could be recycled and reprocessed by hot press under relatively mild conditions with high recovery ratio of mechanical ***,zinc oxide(ZnO)nanoparticles were modified with 3-(trimethoxysilyl)propyl methacrylate and the modified ZnO(defined as ZnO-TPM)was dispersed and polymerized into PUT matrix to prepare their *** influence of ZnO-TPM on the mechanical performance of the composites was evaluated,which indicated that the Young’s modulus and tensile strength increased gradually to the maximum values at ZnO-TPM content of 1 wt%and then *** composites also displayed good reprocessability with improved recovery ratio compared to the pure PUT *** addition,the composite materials exhibited strong UV absorption capacity,implying their potential application in the circumstance where UV-shielding was required.

关键词： Polyurethane-urea methacrylate Hindered urea bond ZnO nanoparticles Reprocessing UV curing

Electronic structure engineering of transition metal dichalcogenides for boosting hydrogen energy conversion electrocatalysts

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Chinese Physics B 2024年第9期33卷 13-28页

作者： Bing Hao Jingjing Guo Peizhi Liu Junjie Guo key laboratory of Interface Science and engineering in advanced materials Ministry of EducationTaiyuan University of TechnologyTaiyuan 030024China

Electrocatalytic water splitting for hydrogen production is an appealing strategy to reduce carbon emissions and generate renewable *** promising process,however,is limited by its sluggish reaction kinetics and high-cost *** two-dimensional(2D)transition metal dichalcogenides(TMDCs)have presented great potential as electrocatalytic materials due to their tunable bandgaps,abundant defective active sites,and good chemical ***,phase engineering,defect engineering and interface engineering have been adopted to manipulate the electronic structure of TMDCs for boosting their exceptional catalytic ***,it is essential to clarify the local structure of catalytically active sites of TMDCs and their structural evolution in catalytic reactions using atomic resolution electron microscopy and the booming in situ technologies,which is beneficial for exploring the underlying reaction *** this review,the growth regulation,characterization,particularly atomic configurations of active sites in TMDCs are *** significant role of electron microscopy in the understanding of the growth mechanism,the controlled synthesis and functional optimization of 2D TMDCs are *** review will shed light on the design and synthesis of novel electrocatalysts with high performance,as well as prompt the application of advanced electron microscopy in the research of materials science.

关键词： TMDCs STEM hydrogen energy conversion active site identification

Micro-nanoarchitectonic of aluminum-hydrogel propellant with static stability and dynamic rheology

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Frontiers of chemical Science and engineering 2024年第4期18卷 87-96页

作者： Huiyan Guo Huaiyu Li Hongzhi Zhang Lun Pan Chengxiang Shi Kang Xue Xiangwen Zhang Ji-Jun Zou key laboratory for advanced Fuel and Propellant of ministry of education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

The aluminum-water system is a promising propellant due to high energy and low signal characteristics,and the gel form is easier to store and *** this work,hydrogels of water and aluminum particles were prepared using the low-molecular-weight gellant *** various physical properties of gel systems,including the water loss rate,phase transition temperature,and centrifugal stability at different gellant and aluminum contents,were *** properties were assessed through shear thinning tests,thixotropy tests,strain sweep analysis,and frequency sweep *** microstructure of the gel was obtained through scanning electron microscopy *** results show that the aluminum-hydrogel network structure is composed of micron-scale aluminum and agarose nanosheets,and the unique micro-nanostructure endows the gel with excellent mechanical strength and thermal stability,which improve with increasing gellant and aluminum ***,the gel with 2% agarose and 20% aluminum had the best performance;the storage modulus reached 90647 Pa,which was within the linear viscoelastic region,and the maximum withstand pressure was 111.2 kPa,which was 118.8% greater than that of the pure ***,the gel demonstrates remarkable shear thinning behavior and can undergo gel-sol transformation upon shearing or heating to exceeding 114℃.

关键词： aluminum-water propellant gelled propellant rheological property mechanical strength

Homogenous coating of Li^(+)conductive Li_(5)AlO_(4)on single-crystalline nonstoichiometric Li_(1.04)Ni_(0.92)Al_(0.04)O_(2)for rechargeable lithium-ion batteries

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Journal of Energy Chemistry 2024年第8期95卷 651-659,I0014页

作者： Guoyu Ding Shizhou Wang Jinhan Li Ziyan Wu Jiayu Chen Jiayong Du Xinhui Huang Kuiming Liu Yudong Zhang Zhonghan Wu Yiyang Peng Qiancheng Zhao Meng Yu Fangyi Cheng key laboratory of advanced Energy materials Chemistry(ministry of education) Engineering Research Center of High-efficiency Energy Storage(Ministry of Education)College of ChemistryNankai UniversityTianjin 300071China State key laboratory of advanced chemical Power Sources Nankai UniversityTianjin 300071China Haihe laboratory of Sustainable chemical Transformations Tianjin 300192China

Cobalt-free,nickel-rich LiNi_(1-x)Al_(x)O_(2)(x≤0.1)is an attractive cathode material because of high energy density and low cost but suffers from severe structural degradation and poor rate *** this study,we propose a molten salt-assisted synthesis in combination with a Li-refeeding induced aluminum segregation strategy to prepare Li_(5)AlO_(4)-coated single-crystalline slightly Li-rich Li_(1.04)Ni_(0.92)Al_(0.04)O_(2).The symbiotic formation of Li_(5)AlO_(4)from reaction between molten lithium hydroxide and doped aluminum in the bulk ensures a high lattice matching between the Ni-rich oxide and the homogenous conductive Li_(5)AlO_(4)that permits high Li^(+)*** from mitigated undesirable side reactions and phase evolution,the Li_(5)AlO_(4)-coated single-crystalline Li_(1.04)Ni_(0.92)Al_(0.04)O_(2)delivers a high specific capacity of220.2 mA h g^(-1)at 0.1 C and considerable rate capability(182.5 mA h g^(-1)at 10 C).Besides,superior capacity retention of 90.8%is obtained at 1/3 C after 100 cycles in a 498.1 mA h pouch full ***,the particulate morphology of Li_(1.04)Ni_(0.92)Al_(0.04)O_(2)remains intact after cycling at a cutoff voltage of 4.3 V,whereas slightly Li-deficient Li_(0.98)Ni_(0.97)Al_(0.05)O_(2)features intragranular cracks and irreversible lattice *** results highlight the value of molten salt-assisted synthesis and Li-refeeding induced elemental segregation strategy to upgrade Ni-based layered oxide cathode materials for advanced Li-ion batteries.

关键词： Aluminum segregation Surface coating Nonstoichiometric oxides Molten synthesis Cathode materials

Chiral multiple-resonance thermally activated delayed fluorescence materials based on chiral spiro-axis skeleton for efficient circularly polarized electroluminescence

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Science china Chemistry 2024年第7期67卷 2257-2264页

作者： Shi-Quan Song Xiao Han Zhong-Zhong Huo Ching-Fai Yip Xian-Fang Hong Meng-Ning Ding You-Xuan Zheng State key laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China key laboratory of Mesoscopic Chemistry of ministry of education School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Chiral luminescence materials have potential applications in the field of three-dimensional displays due to their circularly polarized luminescence(CPL)***,the further development of circularly polarized organic light-emitting diodes(CP-OLEDs)needs to meet the requirements of high efficiency,high color purity,low cost,and high dissymmetry factor(gPLor gEL),chiral multiple resonance thermally activated delayed fluorescence(MR-TADF)materials are considered as candidates in these ***,based on a pair of chiral spirofluorene precursors,two pairs of high-performance chiral MR-TADF emitters((R/S)-p-Spiro-DtBuCzB and(R/S)-m-Spiro-DtBuCzB)are developed,which exhibit strong emissions peaking at 491 and 502 nm in toluene with full-width at half-maximum values of 25 and 33 nm,*** addition,small singlet–triplet energy gaps of 0.15 and 0.10 eV with high absolute photoluminescence efficiencies of 95.0%and 96.7%are observed for p-Spiro-DtBuCzB and m-Spiro-DtBuCzB molecules,*** based on p-Spiro-DtBuCzB and m-Spiro-DtBuCzB display high maximum external quantum efficiencies of 29.6%and 33.8%,*** importantly,CP-OLEDs present symmetric circularly polarized electroluminescence spectra with|gEL|factors of 3.36×10^(-4)and 7.66×10^(-4)for devices based on(R/S)-p-Spiro-DtBuCzB and(R/S)-m-Spiro-DtBuCzB enantiomers,respectively.

关键词： chiral spiro-axis skeleton-based material multiple resonance thermally activated delayed fluorescence circularly polarized electroluminescence dissymmetry factor external quantum efficiency

Tunable Phase Structure of Side-chain Liquid Crystalline Polymers Enabled by Molecular engineering of Dual Mesogenic Cores

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Chinese Journal of Polymer Science 2024年第10期42卷 1459-1469,I0009页

作者： Wen-Huan Yao Lan-Sheng Liu Jie Zhao Yan-Xia Wang An-Zhi Ma Zheng-Rui Ma Lan-Ying Zhang Ruo-Chen Lan College of Chemistry and chemical engineering Hunan UniversityChangsha410082China key laboratory of Eco-Functional Polymer materials of the ministry of education Key Laboratory of Eco-Environmental Polymer Materials of Gansu ProvinceCollege of Chemistry and Chemical EngineeringNorthwest Normal UniversityLanzhou730070China department of materials Science and engineering College of EngineeringPeking UniversityBeijing100871China Institute of advanced materials&key Lab of Fluorine and Silicon for Energy materials and Chemistry of ministry of education College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang330022China

A series of novel side-chain liquid crystalline(SCLC)copolymers were synthesized by attaching two distinct mesogenic units,namely a chiral cholesteryl-based monomer(M1)and an achiral biphenyl-based monomer(M2),to a poly(3-mercaptopropylmethylsiloxane)(PMMS)backbone via thiol-ene click *** influence of side chain composition on the self-assembly behavior and phase structures of these SCLC copolymers was systematically investigated using different *** indicate that three distinct liquid crystalline phases and four unique molecular configurations were identified within the polymer series,with the emergence of the liquid crystalline phase being a synergistic outcome of the two distinct side *** study underscores the critical influence of side chain dimensions,rigidity,and spatial volume on the self-assembly structures and phase characteristics of liquid crystalline polymers,providing valuable insights for the rational design and development of advanced functional materials with tailored properties.

关键词： Liquid crystalline copolymers Self-assembly Phase structure Chiral molar ratio

pH Induced Self-assembly of AIE Fluorescent Probe for Tumor Imaging

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Chinese Journal of Polymer Science 2024年第1期42卷 7-13,I0005页

作者： Jing-Yuan Xiang Wen-Long Zhang He-Ting Li Ya-Ning He department of chemical engineering Key Laboratory of Advanced Materials(MOE)Tsinghua UniversityBejing 100084China

This work reported an AIE fluorescent probe for tumor imaging based on the p H induced self-assembly strategy. The fluorescent probe was composed of an acid-responsive soluble copolymer PEG-b-PAMA-DMMA with a maleic acid amide group and an anionic soluble aggregation-induced emission fluorogen(AIEgen) TPE-2SO_(3)^(-). The polymer could be transformed into a protonated amine-containing polymer after the hydrolysis of maleic acid amide in acidic tumor microenvironment, which would be further self-assembled with TPE-2SO_(3)^(-)to form aggregated nanoparticles. The transition of TPE-2SO_(3)^(-)from dispersed state to aggregated state led to an obvious increase in fluorescence intensity due to its AIE characteristics.

关键词： p H-responsive Self-assembly Fluorescent probe AIE Tumor imaging

Work-function effect of Ti_(3)C_(2)/Fe-N-C inducing solid electrolyte interphase evolution for ultra-stable sodium storage

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Nano Research 2024年第8期17卷 7163-7173页

作者： Huicong Xia Lingxing Zan Hongliang Dong Yifan Wei Yue Yu Jinfu Shu Jia-Nan Zhang Chong-Xin Shan key laboratory of advanced Energy Catalytic and Functional Material Preparation of Zhengzhou College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China key laboratory of materials Physics of ministry of education School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou 450001China key laboratory of chemical Reaction engineering of Shaanxi Province College of Chemistry and Chemical EngineeringYan’an UniversityYan’an 716000China Center for High Pressure Science and Technology advanced Research PudongShanghai 201203China key laboratory of advanced Energy materials Chemistry(ministry of education) Nankai UniversityTianjin 300071China

In the quest to enhance the efficiency of sodium-ion batteries,the dynamics of solid electrolyte interphase(SEI)formation are of paramount *** SEI layer’s integrity is integral to the charge–discharge efficiency and the overall longevity of the ***,a novel two-dimensional Ti_(3)C_(2) fragments enmeshed on iron-nitrogen-carbon(Fe-N-C)nanosheets(Ti_(3)C_(2)/Fe-NC)has been *** electrode features a matrix which has been shown to expedite SEI layer formation through the facilitation of selective anion adsorption,thus augmenting battery *** functional theory calculation reveals that the SEI evolution energy of NaPF6 at the Ti_(3)C_(2)/Fe-N-C interface is 0.81 eV,significantly lower than the Ti_(3)C_(2)(1.23 eV).This process is driven by the electron transportation from Ti_(3)C_(2) to Fe-N-C substrate,facilitated by their work-function difference,leading to the formation of ferromagnetic Fe species,which possesses Fe 3d d_(xz)d_(z)2 orbitals and undergoes hybridization with theπandσorbitals of NaF,creating a key intermediate during *** process diminishes the antibonding energy and attenuates the orbital interaction with NaF,thus reducing the activation energy and improving the SEI formation reaction ***,it leads to the creation of multi-interface SEI characterized by high-throughput ion transport and an efficient reaction network.

关键词： Ti_(3)C_(2)/Fe-N-C heterostructure work-function electron interaction solid electrolyte interphase sodium storage

Rationally construction of atomic-precise interfacial charge transfer channel and strong build-in electric field in nanocluster-based Zscheme heterojunctions with enhanced photocatalytic hydrogen production

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Nano Research 2024年第6期17卷 5002-5010页

作者： Qingtao Zhu Honglei Shen Chao Han Liu Huang Yanting Zhou Yuanxin Du Xi Kang Manzhou Zhu department of materials Science and engineering Centre for Atomic Engineering of Advanced MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationKey Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui UniversityHefei 230601China

The lack of effective charge transfer driving force and channel limits the electron directional migration in nanoclusters(NC)-based heterostructures,resulting in poor photocatalytic ***,a Z-scheme NC-based heterojunction(Pt1Ag28-BTT/CoP,BTT=1,3,5-benzenetrithiol)with strong internal electric field is constructed via interfacial Co-S bond,which exhibits an absolutely superiority in photocatalytic performance with 24.89 mmol·h^(−1)·g−1 H_(2)production rate,25.77%apparent quantum yield at 420 nm,and~100%activity retention in stability,compared with Pt1Ag28-BDT/CoP(BDT=1,3-benzenedithiol),Ag29-BDT/CoP,and *** enhanced catalytic performance is contributed by the dual modulation strategy of inner core and outer shell of NC,wherein,the center Pt single atom doping regulates the band structure of NC to match well with CoP,builds internal electric field,and then drives photogenerated electrons steering;the accurate surface S modification promotes the formation of Co-S atomic-precise interface channel for further high-efficient Z-scheme charge directional *** work opens a new avenue for designing NC-based heterojunction with matchable band structure and valid interfacial charge transfer.

关键词： atomically precise metal nanocluster Z-scheme heterojunction interfacial charge transfer build-in electric field photocatalytic hydrogen production

Bimetallic CoNi single atoms supported on three-dimensionally ordered mesoporous chromia: highly active catalysts for n-hexane combustion

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Green Energy & Environment 2024年第7期9卷 1122-1137页

作者： Xiuqing Hao Yuxi Liu Jiguang Deng Lin Jing Jia Wang Wenbo Pei Hongxing Dai Beijing key laboratory for Green Catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution Control Key Laboratory of Advanced Functional Materials Education Ministry of China Laboratory of Catalysis Chemistry and Nanoscience Department of Chemical Engineering Faculty of Environment and Life Beijing University of Technology

Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds （VOCs）.In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom （Co1Ni1/meso-Cr2O3） and bimetallic Co and Ni nanoparticle (CoNPNiNP/mesoCr2O3) catalysts adopting the one-pot polyvinyl pyrrolidone （PVP）-and polyvinyl alcohol （PVA）-protecting approaches,*** results indicate that the Co1Ni1/meso-Cr2O3catalyst exhibited the best catalytic activity for n-hexane (C6H14) combustion (T50%and T90%were 239 and 263℃ at a space velocity of 40,000 mL g-1h-1;apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol-1and 4.3×10-7mol g-1cats-1,respectively),which was associated with its higher (Cr5++Cr6+) amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni1was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co1preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen（MvK） mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→COx→CO2and H2O.

关键词： Three-dimensional ordered mesoporous chromium oxide Supported bimetallic single-atom catalyst Cobalt−nickel single atoms n -Hexane combustion Catalytic reaction mechanism