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

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 *** 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/*** designing the molecular structure,vinyl chloroacetate was used to provide active sites for subsequent vulcanization and *** 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 *** 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 *** 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 ***,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

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Study on trifluoromethanesulfonic acid-promoted synthesis of daidzein: Process optimization and reaction mechanism

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Chinese Journal of Chemical Engineering 2024年第7期71卷 132-139页

作者： Hai Cao Haibin Yang Yanxiong Fang Yuandi Zeng Xiaolan Cai Jingjing Ma School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China Jieyang Branch of Chemistry and Chemical Engineering Guangdong laboratory(Rongjiang laboratory) Jieyang 515200China

Daidzein has been widely used in pharmaceuticals,nutraceuticals,cosmetics,feed additives,*** preparation process and related reaction mechanism need to be further investigated.A cost-effective process for synthesizing daidzein was developed in this *** this article,a two-step synthesis of daidzein(Friedel–Crafts acylation and[5+1]cyclization)was developed via the employment of trifluoromethanesulfonic acid(TfOH)as an effective promoting *** effect of reaction conditions such as solvent,the amount of TfOH,reaction temperature,and reactant ratio on the conversion rate and the yield of the reaction,respectively,was systematically investigated,and daidzein was obtained in 74.0%isolated yield under optimal *** to the facilitating effect of TfOH,the Friedel–Crafts acylation was completed within 10 min at 90℃ and the[5+1]cyclization was completed within 180 min at 25℃.In addition,a possible reaction mechanism for this process was *** results of the study may provide useful guidance for industrial production of daidzein on a large scale.

关键词： Synthesis Optimal design Chemical processes Reaction mechanism

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Design and construction of size-controlled CoO/CS catalysts for Fischer–Tropsch synthesis

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Nano Research 2024年第4期17卷 2520-2527页

作者： Wei Sun Ting Kuang Guiyou Wei Yue Li Yaqin Liu Shuai Lyu Yuhua Zhang Jinlin Li Li Wang Key laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education&Hubei Key laboratory of Catalysis and Materials Science South-Central Minzu UniversityWuhan 430074China Hubei Key laboratory of Biomass Fibers and Eco-dyeing&Finishing College of Chemistry and Chemical EngineeringWuhan Textile UniversityWuhan 430200China

The use of supported Co-based catalysts is widespread in various catalytic reactions due to their unique *** structural sensitivity of these catalysts is closely linked to their particle size and crystal ***,comprehending the structure–activity relationship requires the development of well-defined Co-based ***,we employed a colloidal wet chemical process and a heterogeneous nucleation method to prepare well-defined Co-based catalysts supported by inert carbon *** nanospheres’surface possesses abundant functional groups that efficiently capture metal complexes and facilitate the nucleation and growth of CoO *** adjusting the Co source concentration,solvent molar ratio,and nucleation growth kinetics,we successfully prepared CoO/carbon sphere(CS)catalysts with different particle sizes and crystal *** influence of metallic face-centered cubic(fcc)-Co^(0) particle size in the range of 6.6–17.6 nm on the performance of Fischer–Tropsch synthesis(FTS)using well-defined CoO/CS catalysts has been *** result demonstrated that the turnover frequency(TOF)remained constant for CoO/CS catalysts with metallic fcc-Co^(0) particle size larger than 7.7 ***,both the selectivity and the activity changed for CoO/CS catalysts with smaller particles(<7.7 nm).Significantly,when metallic fcc-Co^(0) particle size was reduced from 17.6 to 7.7 nm,the cobalt time yield increased to 6.7μmolCO·gCo^(-1)·s^(-1),indicating improved catalytic *** the same time,the CH_(4) selectivity decreased to 4.9%,suggesting a higher preference for hydrocarbon *** findings demonstrate the importance of particle size in Co catalyzed Fischer–Tropsch *** use of well-defined CoO/CS catalysts offers valuable insights into the structure–activity relationship,leading to a better understanding of Co catalyzed Fischer–Tropsch synthesis.

关键词： Fischer–Tropsch synthesis(FTS) cobalt size effects phase effects carbon nanospheres

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Rational design multi-color-emissive chemiluminescent carbon nanodots in a single solvothermal reaction

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Nano Research 2024年第6期17卷 4651-4660页

作者： Guang-Song Zheng Cheng-Long Shen Yuan Deng Kai-Kai Liu Jin-Hao Zang Lin Dong Qing Lou Chong-Xin Shan Henan Key laboratory of Diamond Optoelectronic Materials and Devices Key Laboratory of Materials PhysicsMinistry of Educationand School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou 450052China

Recently,the chemiluminescence(CL)induced by carbon nanodots(CDs)has intrigued researchers’extensive interests in various applications due to its special light emission ***,the difficulty of synthesizing chemiluminescent CDs with full-spectrum emission severely hinders the further regulation of the CL emission ***,the multi-color-emissive chemiluminescent CDs are rational designed and further synthesized by regulating the sp2-hybrid core and sp3-hybrid surface from the citrate-ammonia molecular in a single solvothermal *** experimental characterizations and density functional theory calculations reveal that the higher temperature can promote the crosslinking polymerization/carbonization of carbon core and the higher protonation of solvent can determine the core size of final CDs,resulting in the variant CL emission from molecular-,crosslinking-and ***,the CL emission of the CDs can be further synthesized by tuning the luminescence chromophores in the formation process via regulating the temperature and solvent,enabling the applications of the CL CDs in illumination and information *** study paves a new technology to understand the luminescence of CDs and affords an industry translational potential over traditional chemiluminescent molecular.

关键词： carbon nanodots chemiluminescence regulation energy level alignment mechanism

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Highly crystallization-induced emissive luminophores with mechanoluminescent features for two-photon harvesting fluorescence imaging and latent fingerprint identification

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Nano Research 2024年第7期17卷 6475-6482页

作者： Jian Lu Juan Gao Rui-Xuan Qian Shuai-Hua Wang Fa-Kun Zheng Guo-Cong Guo Fujian Science and Technology Innovation laboratory for Optoelectronic Information of China Fuzhou 350108China State Key laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Fluorescence imaging can be employed in fields of medical treatment,astronomical exploration,and national defense *** fluorescence imaging often takes the single-photon techniques,which is vulnerable to background interference and ***,two-photon fluorescence imaging can achieve much higher-resolution fluorescence imaging for reducing scattering and deeper ***,by assembling the tetraphenylethylene backbones with nontoxic and non-noble K^(+)ions,compound 1([(Hdma)K(H_(2)ettc)]_(n),H_(4)ettc=4',4''',4''''',4'''''''-(ethene-1,1,2,2-tetrayl)tetrakis(([1,1'-biphenyl]-4-carboxylic acid)))with the crystallization-induced emissions exhibited charming fluorescence imaging under two-photon excitation microscopy(TPEM).Besides,luminescent powders based on compound 1 can achieve high-resolution fingerprint recognition,providing secure access control and identification for a novel authentication *** with the commercial fluorescent dyes coumarin-6,the as-synthesized compound 1 showed great solvent stability,indicating its durability against harsh ***,compound 1 shows mechanoluminescent properties for the perturbation of weak supramolecular interactions within ordered arrangements of the H_(2)ettc^(2−)*** novel compound has provided an important insight to the development of twophoton fluorescence imaging and advanced external-stimuli responsive materials.

关键词： crystallization-induced emission fluorescence imaging two-photon absorption fingerprint recognition mechanoluminescence

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Selective type II TRK inhibitors overcome xDFG mutation mediated acquired resistance to the second-generation inhibitors selitrectinib and repotrectinib

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Acta Pharmaceutica Sinica B 2024年第2期14卷 517-532页

作者： Shuang Xiang Xiaoyun Lu International Cooperative laboratory of Traditional Chinese Medicine Modernization and Innovative Drug Discovery of Chinese Ministry of Education(MOE) Guangdong Provincial Key Laboratory of New Drug Design and EvaluationGuangzhou City Key Laboratory of Precision Chemical Drug DevelopmentSchool of PharmacyJinan UniversityGuangzhou 510632China

Neurotrophic receptor kinase(NTRK) fusions are actionable oncogenic drivers of multiple pediatric and adult solid tumors,and tropomyosin receptor kinase(TRK) has been considered as an attractive therapeutic target for "pan-cancer" harboring these ***,two generations TRK inhibitors have been *** representative second-generation inhibitors selitrectinib and repotrectinib were designed to overcome clinic acquired resistance of the first-generation inhibitors larotrectinib or entrectinib resulted from solvent-front and gatekeeper on-target ***,xDFG(TRKAG667C/A/S,homologous TRKCG696C/A/S) and some double mutations still confer resistance to selitrectinib and repotrectinib,and overcoming these resistances represents a major unmet clinical *** this review,we summarize the acquired resistance mechanism of the first-and second-generation TRK inhibitors,and firstly put forward the emerging selective type Ⅱ TRK inhibitors to overcome xDFG mutations mediated ***,we concluded our perspectives on new challenges and future directions in this field.

关键词： NTRK fusions TRK kinase Clinical resistance xDFG mutations Selective type II inhibitors

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Solvothermal synthesis and adsorption performance of layered boehmite using aluminum chloride and high-alumina fly ash

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Chinese Journal of Chemical Engineering 2024年第6期70卷 280-290页

作者： Jing Wen Ruirui Yuan Tao Jiang Tangxia Yu Yufan Zhang School of Metallurgy Northeastern UniversityShenyang 110819China Key laboratory for Ecological Metallurgy of Multimetallic Mineral(Ministry of Education) Northeastern UniversityShenyang 110819China Liaoning Key laboratory for Metallurgical Sensor and Technology Shenyang 110819China

High alumina fly ash(FAHAl)is a kind of bulk solid waste unique to China,whose availability of high-value aluminum and the threat to the environment makes its high-value utilization *** this work,the alumina containing leaching solution obtained from Na_(2)CO_(3) roasting and HCl leaching of FAHAl was used as the mother liquor to prepare layered boehmite in *** preparation process with AlCl_(3) as the raw material was also *** formation process and mechanism of boehmite,the choice of solvent,along with the adsorption capability of Congo red were analyzed by X-ray diffraction,scanning electron microscopy,Fourier transform infrared spectroscopy,Brunauer-Emmett-Teller method and adsorption *** showed that during the preparation of layered boehmite,the precursor Al(OH)_(3) from the reaction of Al^(3+) and OH-is transformed into boehmiteγ-*** existence of ethanol is beneficial to regulate and promote the growth of boehmite crystal *** water and ethanol are mixed with a volume ratio of 2:1 and used as the solvent,the maximum specific surface area of the boehmite is obtained at 135.7 m^(2)·g^(-1),and 99.16%of Congo red can be absorbed after 10 min when AlCl3 is used as a raw *** purified leaching solution is used as the mother liquid,the crystallinity of boehmite decreases slightly when the pH value decreases from 12.5 to *** pH is 11,the removal efficiency of Congo red reaches a maximum of 72.25%.This process not only achieves the extraction of aluminum and high-value utilization of FAHAl but also provides a thought to prepare layered boehmite with adsorption properties.

关键词： High-alumina fly ash Layered boehmite In-situ preparation Solvothermal synthesis Adsorption High-value utilization

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Branch-Chain-Rich Diisopropyl Ether with Steric Hindrance Facilitates Stable Cycling of Lithium Batteries at-20℃

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Nano-Micro Letters 2024年第10期16卷 121-135页

作者： Houzhen Li Yongchao Kang Wangran Wei Chuncheng Yan Xinrui Ma Hao Chen Yuanhua Sang Hong Liu Shuhua Wang State Key laboratory of Crystal Materials Shandong UniversityJinan 250100People's Republic of China

Li metal batteries(LMBs)offer signifi-cant potential as high energy density alternatives;nev-ertheless,their performance is hindered by the slow desolvation process of electrolytes,particularly at low temperatures(LT),leading to low coulombic efficiency and limited cycle ***,it is essential to opti-mize the solvation structure thereby achieving a rapid desolvation process in LMBs at ***,we introduce branch chain-rich diisopropyl ether(DIPE)into a 2.5 M Li bis(fluorosulfonyl)imide dipropyl ether(DPE)elec-trolyte as a co-solvent for high-performance LMBs at-20℃.The incorporation of DIPE not only enhances the disorder within the electrolyte,but also induces a steric hindrance effect form DIPE’s branch chain,excluding other solvent molecules from Li+solvation *** of these factors contribute to the weak interactions between Li^(+)and solvent molecules,effectively reducing the desolvation energy of the ***,Li(50μm)||LFP(mass loading~10 mg cm^(-2))cells in DPE/DIPE based electrolyte demonstrate stable performance over 650 cycles at-20℃,delivering 87.2 mAh g^(-1),and over 255 cycles at 25℃ with 124.8 mAh g^(-1).DIPE broadens the electrolyte design from molecular structure considera-tions,offering a promising avenue for highly stable LMBs at LT.

关键词： Solvation structure Li metal battery Low temperature Steric hindrance Disorder

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Evolution of hollow nanosphere to microtube in the self-assembly of chiral dansyl derivatives and inversed circularly polarized luminescence

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Chinese Chemical Letters 2024年第7期35卷 285-290页

作者： Sifan Du Yuan Wang Fulin Wang Tianyu Wang Li Zhang Minghua Liu Beijing Key laboratory for Science and Application of Functional Molecular and Crystalline Materials Department of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China National laboratory for Molecular Science(BNLMS) CAS Key Laboratory of ColloidInterface and Chemical ThermodynamicsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Here,we designed asymmetric(m DS)and symmetrical(d DS)chiral V-shaped molecules by linking one or two dansyl groups to trans-1,2-cyclohexane diamine and investigated the solvent-regulated structural transformation and inversed circularly polarized luminescence(CPL)in the *** increasing water volume fraction(fw)in the mixed solvent of water/acetonitrile,asymmetric mDS selfassembled into hollow nanospheres and microtubes,while solid nanospheres and solid microplates were corresponding to symmetric d *** this transformation process,the emission of m DS and d DS was changed from yellow-green to blue and cyan color,which was ascribed to twisted intramolecular charge transfer(TICT)and locally excited(LE)fluorescence of V-shaped DS *** conformation of N,Ndimethyl groups with respect to naphthalene ring also led to the transformation of *** tubular and platelike structures had stronger and reversed CPL signals in comparison with spheroidal *** chiral information of DS assembly could be effective transferred to achiral Nile red via co-assembly strategy,which endowed Nile red exhibiting inversed induced CPL signal regulated by water *** work provides a method for achieving a variety of self-assembled structures with adjustable chiroptical properties.

关键词： CPL inversion Hollow structure Self-assembly Dansyl Chirality transfer

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Recent advances in post-chiroptical manipulation of supramolecular aggregates assembled with molecular modules

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Science China Chemistry 2024年第9期67卷 2842-2863页

作者： Yanling Shen Wanhua Wu Zhipeng Yu Cheng Yang Key laboratory of Green Chemistry & Technology of Ministry of Education College of Chemistry Institution Sichuan University

Recently, various supramolecular assembly systems have been identified where the pre-existing chiral supramolecular structure can be manipulated through environmental adjustments, such as temperature, solvent, and concentration. These changes result in diverse microscopic morphologies during the assembly process and induce chiroptical variations, particularly in circular dichroism(CD) and circularly polarized luminescence(CPL) spectra. These chiroptical properties serve as direct indicators of the chiral supramolecular structure and hold promise for applications in sensing, molecular recognition, asymmetric synthesis, and material science. This review focuses on research published in the last five years, highlighting instances where assembled structures aggregated by small organic molecular modules demonstrate in-situ chiroptical changes through external condition control. It categorizes and discusses different modes of regulation, aiming to offer insights and guidelines for exploring dynamic changes in assembly processes and designing in-situ adjustable structures of assembly modules.

关键词： supramolecular assemblies post-chiroptical manipulation in-situ structural changes

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