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Boosting thermal stability and crystallization of closed-loop-recyclable biodegradable poly(p-dioxanone) by end-group regulation

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Science China Chemistry 2024年第2期67卷 642-651页

作者： Jin Lei Zhu-Xin Gui Wan-ting Xiong Gang Wu Si-Chong chen Yu-Zhong Wang The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric Materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu610064China

A chemically closed-loop-recyclable biodegradable polymer,poly(p-dioxanone)(PPDO),is one of the ideal candidates for single-use plastic products due to its suitability for different application ***,when PPDO wastes can be collected,its monomer p-dioxanone(PDO) will be obtained through chemical recycling of these wastes;when cannot be collected,the wastes are able to be biodegraded into harmless ***,unsatisfied thermal stability and low crystallization rate of PPDO restrict its wider ***,based on end-group regulation,we simultaneously realized the significant enhancement of thermal stability and crystallization of PPDO through the simple melt processing with tributyl phosphite(TBP) or triphenyl phosphite(TPP).The model reactions were conducted to investigate the reaction mechanism and theoretical products during the preparation of PPDO/phosphite *** kinds of phosphites were proved to act as the end-capped reagent and chain extender in the melt processing,while TBP presented better *** a result,the activation energy of thermal decomposition was largely elevated,and the unprecedented T_(5%)(the temperature at a weight loss of 5%) and Tmax(the temperature at a maximum rate of weight loss) of PPDO were obtained,i.e.,T_(5%)of ~330 ℃ and Tmaxof ~385 ℃ in N_(2) atmosphere,T_(5%)of ~240 ℃ and Tmaxof ~317 ℃ in air atmosphere,***,the increased crystallization rate,crystallinity,crystalline orderliness,and realizable monomer recovery(yield >90%,purity >99.9%) of PPDO/phosphite compounds were confirmed.

关键词： poly(p-dioxanone) phosphite thermal stability crystallization end-group regulation

QL1706 (anti-PD-1 IgG4/CTLA-4 antibody) plus chemotherapy with or without bevacizumab in advanced non-small cell lung cancer: a multi-cohort, phase II study

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Signal Transduction and Targeted Therapy 2024年第2期9卷 797-806页

作者： Yan Huang Yunpeng Yang Yuanyuan Zhao Hongyun Zhao Ningning Zhou Yaxiong Zhang Likun chen ting Zhou Gang chen ting Wu Lu Lu Shilin Xue Xiaoyan Kang Li Zhang Wenfeng Fang Department of Medical Oncology Sun Yat-sen University Cancer CenterState Key Laboratory of Oncology in South ChinaCollaborative Innovation Center for Cancer MedicineNo.651 Dongfeng East RoadGuangzhouGuangdong 510060China Department of Medicine Qilu Pharmaceutical Co.Ltd.JinanChina

First-line chemoimmunotherapy(with or without bevacizumab)has improved outcomes in advanced non-small cell lung cancer(NSCLC).Here,this open-label,multi-cohort phase II study(NCT05329025)was done to investigate the safety and efficacy of QL1706(a single bifunctional MabPair product against PD-1 and CTLA-4)and chemotherapy with or without bevacizumab in this *** were enrolled into five different cohorts based on genotype(cohorts 1-4,epidermal growth factor receptor[EGFR]wild-type;cohort 5,EGFR-mutant and progressed on EGFR-tyrosine kinase inhibitors[TKIs]).Between June 11,2021 and December 29,2021,91 patients were *** frequent treatment-related adverse events(TRAEs)included decreased appetite(60[65.9%]),anemia(60[65.9%]),infusion-related reactions(48[52.7%]),and pruritus(44[48.4%]).Grade≥3 TRAEs occurred in 30(33.0%)***-seven(45%)patients with wild-type EGFR achieved partial response(PR)(objective response rate[ORR]=45%)and had a median progression-free survival(mPFS)of 6.8 months(95%CI:5.2-9.7).For 31 patients harboring mutated EGFR,17(54.8%)achieved PR(ORR=54.8%),with an mPFS of 8.5 months(95%CI:5.72-not evaluable).Overall,QL1706 plus chemotherapy,regardless of having bevacizumab,was generally tolerable and had promising antitumor activity for EGFR wild-type advanced NSCLC in first-line ***,QL1706 plus chemotherapy and bevacizumab showed favorable antitumor activity for patients who had EGFR mutated NSCLC but failed in TKI therapy,demonstrating a potential for treating this population.

关键词： bevacizumab chemotherapy phase

Pyridine-regulated Sb@InSbS_(3)ultrafine nanoplates as high-capacity and long-cycle anodes for sodium-ion batteries

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Rare Metals 2024年第5期43卷 2080-2092页

作者： Jia-Ying Ren Xiang-Lin Yu Chang-Miao chen Xin-Yu Hu ting Yang Ming Zhang College of Materials Science and Engineering and College of Science Central South University of Forestry and TechnologyChangsha 410004China College of Semiconductors(College of Integrated Circuits) Changsha Semiconductor Technology and Application Innovation Research InstituteHunan UniversityChangsha 410082China

Sb-based materials exhibit considerable potential for sodium-ion storage owing to their high theoretica ***,the bulk properties of Sb-based materials always result in poor cycling and rate *** overcome these issues,pyridine-regulated Sb@InSbS_(3)ultrafine nanoplates loaded on reduced graphene oxides(Sb@InSbS_(3)@rGO)were designed and *** the synthesis process,pyridine was initially adopted to coordinate with In^(3+),and uniformly dispersed In_(2)S_(3)ultrafine nanoplates on reduced graphene oxide were generated after ***,partial In^(3+)was exchanged with Sb^(3+),and Sb@InSbS_(3)@rGO was obtained by using the subsequent annealing *** unique structure of Sb@InSbS_(3)@rGO effectively shortened the transfer path of sodium ions and electrons and provided a high *** the anode in sodium-ion batteries,the Sb@InSbS_(3)@rGO electrode demonstrated a significantly higher reversible capacity better stability(445 m Ah·g^(-1)at 0.1 A·g^(-1)after 200 cycles and 212 mAh·g^(-1)at 2 A·g^(-1)after 1200 cycles),and superior rate(210 mAh·g^(-1)at 6.4 A·g^(-1))than the electrode without pyridine(355 mAh·g-1at 0.1 A·g-1after 55 cycles and 109 mAh·g^(-1)at 2 A·g^(-1)after 770 cycles)Furthermore,full cells were assembled by using the Sb@InSbS_(3)@rGO as anode and Na_(3)V_(2)(PO_(4))_(3)as cathode which demonstrated good cycling and rate performances and exhibited promising application *** results indicate that adjusting the microstructure of electrode materials through coordination balance is A·good strategy for obtaining high-capacity,high-rate,and longcycle sodium storage performances.

关键词： Sodium-ion battery Sb-based anode material Pyridine coordination Reduced size nanostructure Half/full cell

Construction of Naphthalenediimide Lanthanide(Ⅲ)-MOFs and Composites Incorporated Electron-Rich Pyrene Derivative as Multifunctional Fluorescence Sensing for Nitro Aromatic Compounds and Aldehydes

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Chinese Journal of Chemistry 2024年第3期42卷 283-293页

作者： Rong Huo ting Zhang Guang Zeng chen Wang Yong Heng Xing Feng Ying Bai College of Chemistry and Chemical Engineering Liaoning Normal UniversityDalianLiaoning116029 China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianLiaoning116023 China

The development of host-guest MOF luminescent composites has attracted considerable attention. However,it is still a challenge to reasonably design large scale conjugated polycarboxylic acids metal-organic framework (MOF) and modulate donor-acceptor interaction. Herein,a series of isostructural 3D porous lanthanide MOF [Ln_(2)(BINDI)0.5(NO_(3))(DMA)(H_(2)O)]∙DMA∙2.5H_(2)O (Ln = La (1),Ce (2),Pr (3) and Nd (4);H_(4)BINDI (N,N’-bis(5-isophthalic acid)-1,4,5,8-naphthalenediimide) were synthesized. Considering the electron-deficient performances of Ln-BINDI MOFs,D-A type composites Ln-MOFs (1—4@H_(4)TBAPy) were prepared via the incorporation of electron-rich H_(4)TBAPy (1,3,6,8-tetrakis(p-benzoic acid) pyrene),which more improved the luminescence performance of complexes 1—4 and can be used as fluorescence sensors for the detection of nitro compounds and aldehydes. High sensitivity of 1@H_(4)TBAPy towards pNBA,pNA PNP,DNP,and TNP could be achieved through hydrogen bond interactions between MOF and analytes,as well as the π-π interaction between H_(4)TBAPy and the naphthalene ring of BINDI,thus the fluorescence quenching efficiency of 1@H_(4)TBAPy was better than that of the complex 1. In addition,it is found that 1@H_(4)TBAPy has high selectivity and sensitivity to aromatic aldehyde SA,5-Mesal and HMBA. Such strategy to enhance the emission of NDI based Ln-BINDI MOFs,will open up an avenue to obtain more fluorescent MOFs for sensing.

关键词： Ln-MOF Pyrene molecule NACs Aldehydes Fluorescence sensing Carboxylate ligands Charge transfer Donor-acceptor systems

Text Difficulty Study:Do Machines Behave the Same as Humans Regarding Text Difficulty?

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Machine Intelligence Research 2024年第2期21卷 283-293页

作者： Bowen chen Xiao Ding Yi Zhao Bo Fu tingmao Lin Bing Qin ting Liu Research Center for Social Computing and Information Retrieval Harbin Institute of TechnologyHarbin 150001China Fundamental Technology Center China Construction Bank Financial Technology Co.Ltd.Beijing 100033China

With the emergence of pre-trained models,current neural networks are able to give task performance that is comparable to ***,we know little about the fundamental working mechanism of pre-trained models in which we do not know how they approach such performance and how the task is solved by the *** example,given a task,human learns from easy to hard,whereas the model learns ***,difficulty-insensitive learning leads to great success in natural language processing(NLP),but little attention has been paid to the effect of text difficulty in *** propose a human learning matching index(HLM Index)to investigate the effect of text *** results show:1)LSTM gives more human-like learning behavior than ***,UID-SuperLinear gives the best evaluation of text difficulty among four text difficulty *** nine tasks,some tasks’performance is related to text difficulty,whereas others are not.2)Model trained on easy data performs best in both easy and medium test data,whereas trained on hard data only performs well on hard test data.3)Train the model from easy to hard,leading to quicker convergence.

关键词： Cognition inspired natural language processing psycholinguistics explainability text difficulty curriculum learning

Tuning the cross-linked structure of basic poly(ionic liquid)to develop an efficient catalyst for the conversion of vinyl carbonate to dimethyl carbonate

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Chinese Journal of Chemical Engineering 2024年第8期72卷 106-116页

作者： Zhaoyang Qi Shiquan Zhong Huiyun Su Changshen Ye Limei Ren ting Qiu Jie chen College of Chemical Engineering Fuzhou UniversityFuzhou 350108China Department of Chemical Engineering Shijiazhuang UniversityShijiazhuang 050035China Qingyuan Innovation Laboratory Quanzhou 362801China Fuzhou University International Joint Laboratory of Thermochemical Conversion of Biomass Fuzhou UniversityFuzhou 350108China

Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other *** current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and ***,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and *** address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and *** poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic *** was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing *** was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant *** results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.

关键词： Poly(ionic liquid) Cross-linking degree Dimethyl carbonate production Transesterification reaction Mechanism

Character Sheaves for Classical Graded Lie Algebras

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Acta Mathematica Sinica,English Series 2024年第3期40卷 870-884页

作者： ting XUE School of Mathematics and Statistics University of MelbourneVIC 3010Australia Department of Mathematics and Statistics University of HelsinkiHelsinki 00014Finland

In this note we study character sheaves for graded Lie algebras arising from inner automorphisms of special linear groups and Vinberg’s type Ⅱ classical graded Lie algebras.

关键词： Graded Lie algebras character sheaves Fourier transform nilpotent orbits

Investigating the Absorption and Desorption Behavior of Methylene Chloride in the Poly(aryl ether ketone) Film with Different Crystallinities

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Chinese Journal of Polymer Science 2024年第2期42卷 239-246,I0009页

作者： Hong-Ru Yang Jin-Dong Zhang Dong-ting Gao Gang Liu Chun-Hai chen Jia-Nan Yao Center for Advanced Low-Dimension Materials State Key Laboratory for Modification of Chemical Fibers and Polymer MaterialsCollege of Materials Science and EngineeringDonghua UniversityShanghai201620China

Poly(aryl ether keton e)(PAEK) films with different crystallinities were obtained by controlling the cooling rate,which were subjected to the absorption and desorption of methylene chloride(CH_(2)Cl_(2)).We employed attenuated total reflection Fourier transform infrared(ATR-FTIR)spectroscopy analyses to investigate the diffusion behavior of CH_(2)Cl_(2) in PAEK films with different *** to the Fickian diffusion model,the calculated diffu sion coefficients of CH_(2)Cl_(2) in PAEK films were observed to decrease with increasing *** effect of CH_(2)Cl_(2)absorption and desorption on the mechanical properties of PAEK films with different crystallinity was further analyzed using tensile *** tensile tests exhibited that CH_(2)Cl_(2) has two concurrent effects:plasticization and solvent-induced *** scanning calorimetry(DSC) and wide-angle X-ray diffraction(WXRD) techniques further confirmed solvent-induced crystallization *** results would be beneficial to understand the solvent resistance of PAEK materials and consequently provide the practical application conditions of PAEK with a theoretical basis.

关键词： Poly(aryl ether ketone) Diffusion behavior Infrared spectra Solvent-induced crystallization Mechanical properties

Chemotactic nanomotor for multimodal combined therapy of glioblastoma

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Science China Chemistry 2024年第4期67卷 1277-1288页

作者： ting Li Lin chen Yunxin Xue Xiangyu Xiao Wenjun Dai Kaiyuan Tan Tiantian chen Yingfang Tao Chun Mao Jian Shen Mimi Wan National and Local Joint Engineering Research Center of Biomedical Functional Materials School of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China

Glioblastoma(GBM) is the most aggressive malignant brain tumor. Due to the infiltration and heterogeneity of GBM, the obstruction of the blood-brain barrier(BBB) and the unique immunosuppressive mechanism, it is hard to achieve significant effects of GBM treatment. Here, a kind of chemotactic nanomotor that loaded with glucose oxidase(GOx) and carboxylated cisplatin(Pt(IV)) prodrug on the L-arginine-derived polymer is proposed. The nanomotors are driven by catalysis of glucose decomposition and the positive chemotaxis towards the GBM microenvironment where inducible nitric oxide synthase and reactive oxygen species are highly expressed. This facilitates the BBB crossing and GBM targeting of the nanomotors. In addition, the released nitric oxide(NO) during propulsion as well as the loaded GOx and Pt(IV) can exert combined NO/starvation/chemotherapy. Meanwhile, it is able to induce and enhance the immune response through multiple pathways, thus better coping with the complexities of GBM treatment.

关键词： chemotaxis combined therapy glioblastoma nanomotors