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Intelligent gold nanocluster for effective treatment of malignant tumor via tumor-specific photothermal–chemodynamic therapy with AIE guidance

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National Science Review 2024年第5期11卷 326-342页

作者： Feng Liu Tianfeng Yang Xiaowei Chang Li Chen Cheng Cheng Xiuhong Peng Haihu Liu Yanmin Zhang Xin Chen School of Energy and Power engineering Xi'an Jiaotong University department of Chemical engineering Shaanxi Key Laboratory of Energy Chemical Process IntensificationInstitute of Polymer Science in Chemical Engineering School of Chemical Engineering and Technology Xi'an Jiaotong University School of Pharmacy Health Science Center Xi'an Jiaotong University

Precise and efficient therapy of malignant tumors is always a challenge. Herein, gold nanoclusters co-modified by aggregation-induced-emission（AIE） molecules, copper ion chelator（acylthiourea） and tumor-targeting agent（folic acid） were fabricated to perform AIE-guided and tumor-specific synergistic therapy with great spatio-temporal controllability for the targeted elimination and metastasis inhibition of malignant tumors. During therapy, the functional gold nanoclusters（Au NTF） would rapidly accumulate in the tumor tissue due to the enhanced permeability and retention effect as well as folic acid-mediated tumor targeting, which was followed by endocytosis by tumor cells. After that, the overexpressed copper ions in the tumor cells would trigger the aggregation of these intracellular Au NTF via a chelation process that not only generated the photothermal agent in situ to perform the tumor-specific photothermal therapy damaging the primary tumor, but also led to the copper deficiency of tumor cells to inhibit its ***, the copper ions were reduced to cuprous ions along with the chelation, which further catalysed the excess H2O2in the tumor cells to produce cytotoxic reactive oxygen species, resulting in additional chemodynamic therapy for enhanced antitumor efficiency. The aggregation of Au NTF also activated the AIE molecules to present fluorescence, which not only imaged the therapeutic area for real-time monitoring of this tumor-specific synergistic therapy, but also allowed us to perform near-infrared radiation at the correct time point and location to achieve optimal photothermal therapy. Both in vitro and in vivo results revealed the strong tumor elimination, effective metastasis inhibition and high survival rate of tumor-bearing mice after treatment using the Au NTF nanoclusters, indicating that this AIE-guided and tumor-specific synergistic strategy could offer a promising approach for tumor therapy.

关键词： AIE-guided precise tumor treatment copper-dependent photothermal therapy copper-triggered chemodynamic therapy primary tumor elimination copper-plunder-induced metastasis inhibition

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Highly active organocatalyst from a trivalent phosphazenium salt for ring-opening copolymerization of epoxides and cyclic anhydrides enhanced by hydrogen bonding interactions

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Science China Chemistry 2024年第9期67卷 3111-3120页

作者： Chunhuan Jiang Junqi Wang Xiaoyu Liu Xiaoxia You Ronglin Zhong Chuanli Ren Zhibo Li Key Laboratory of Biobased polymer Materials Shandong Provincial Education DepartmentCollege of Polymer Science and EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Chemical engineering Qingdao University of Science and TechnologyQingdao 266042China Laboratory of Theoretical and Computational Chemistry Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130012China

It is highly desirable to develop simple organocatalysts for the controlled ring-opening alternating copolymerization(ROAC)of epoxides and cyclic anhydrides,leading to high molecular weight ***,a phosphazenium salt,namely tri[tris(dimethylamino)phosphoranylidenamino]phosphonium chloride(P_(4)^(+)Cl^(-)),is developed as a catalyst for the ROAC of epoxides and cyclic ***,the combination of P_(4)^(+)Cl^(-)with a protonic initiator,such as 1,4-benzenedimethanol(BDM)exhibited high efficiency in the copolymerization of propylene oxide(PO)and phthalic anhydride(PA).This led to the production of polyester with an exceptional high molecular weight(M_n)of up to 126 k Da,which represented a rare example of poly(PO-alt-PA)with Mnsurpassing 100 k *** that the core P atom is trivalent status and the tris[tris(dimethylamino)]phosphoranyl group will share one proton in the P_(4)^(+)Cl^(-)*** combined with protonic species,the P_(4)^(+)Cl^(-)will not only serve as a proton acceptor but also as a hydrogen bonding donor for the cyclic ***,it was assumed that the P_(4)^(+)plus proton served dual role in mimic of base/urea pair to effectively catalyze ROAC,which was supported by density functional theory(DFT)calculations.

关键词： ring-opening copolymerization organocatalyst epoxides cyclic anhydrides phosphazenium salt

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Key progresses of MOE key laboratory of macromolecular synthesis and functionalization in 2022

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Chinese Chemical Letters 2024年第3期35卷 114-126页

作者： Xumeng Deng Kaihao Chen Kai Pang Xiaoting Liu Minsong Gao Jie Ren Guanwen Yang Guangpeng Wu Chengjian Zhang Xufeng Ni Peng Zhang Jian Ji Jianzhao Liu Zhengwei Mao Ziliang Wu Zhen Xu Haoke Zhang Hanying Li MOE Key Laboratory of Macromolecular Synthesis and Functionalization International Research Center for X PolymersDepartment of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China

In 2022,The MOE Key Laboratory of Macromolecular Synthesis and Functionalization in Zhejiang University had achieved several important ***,a series of well-defined dinuclear organoboron catalysts were developed to precisely control the enchainment of ether and carbonate segments during the copolymerization of CO_(2)and ***,polyester had been synthesized through cationic copolymerization of cyclic ***,ring-opening polymerization of carbon dioxide based valerolactone had been achieved,revealing the prospect of 3-ethylidene-6-vinyltetrahydro-2H-pyran-2-one(EVL)in utilizing CO_(2)and synthesizing functional ***,machine learning methods have been applied to biomaterial research,enabling high-throughput screening of functional biomaterial surfaces for implantable devices,and searching for potent antimicrobial peptides in whole combinatorial peptide ***,methods of characterization of biomacromolecule RNA transcription and manipulation of nucleoside modification were ***,artificial enzymes-armed Bifidobacterium Longum probiotics were established to tune down gut ***,three-dimensional(3D)printing technologies were used to engineer tough supramolecular ***,hydroplastic foaming graphene frameworks for acoustic and conductive polymer composites were provided for ***,aggregate photophysics about the nature of through-space interactions(TSIs)and manipulating their strength in small molecules with non-conjugated structure had been ***,the forming mechanism of a newfound nested texture in poly(L-lactic acid)(PLLA)spherulitic films had been ***,the isotropically dyeing mechanism of KDP single crystals grown from hydrogels have been *** related works are reviewed in this paper.

关键词： polymer Catalyst Biomaterial research mRNA Hydrogel Graphene Crystal

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Self-assembled aerogel sheet electrodes of thermocells for low-grade heat harvest

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Science China Chemistry 2024年第5期67卷 1672-1679页

作者： Ziwei Mo Shouhao Wei Daibin Xie Kaihua Zhu Hongxiong Li Xin Lu Lirong Liang Chunyu Du Zhuoxin Liu Guangming Chen College of Materials Science and engineering Shenzhen UniversityShenzhen 518055China State Key Laboratory of polymer Materials engineering Sichuan UniversityChengdu 610065China

Efficiently harvesting low-grade heat is crucial for sustainable energy management. Thermocells(TECs), inducing heat-toelectricity conversion via the thermogalvanic effect, have thus drawn tremendous attention in recent years. This study introduces a self-assembly approach for fabricating aerogel sheet electrodes(ASEs) tailored for TECs. The crafted ASEs retain a remarkable porous architecture with approximately 95% porosity, even with their slimmed-down thickness. Results reveal that the electrode composition has minimal influence on the thermopower of TECs. Notably, the porous ASE with tunned composition demonstrates an optimal effective surface area for the thermogalvanic effect, resulting in enhanced output current density. This balances the desirable traits of electrode compactness with abundant redox active sites, positioning it favorably against conventional bulky electrode designs. The TECs utilizing the optimized ASE achieve a peak output power of 22.10 μW cm^(-2)under a temperature difference of 30 K. Furthermore, a tubular TEC device is readily assembled and specially designed for harvesting heat energy from hot fluids. These findings underscore the potential of composite electrodes in the realm of low-grade heat harvest, paving the way for broader applications in sustainable energy solutions.

关键词： thermocells low-grade heat harvest energy conversion composite electrodes

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An interfacial robust and entire self-healing ionogel-elastomer hybrid for elastic electronics enables discretionary assembly and reconfiguration

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Science China Chemistry 2024年第4期67卷 1316-1323页

作者： Lei Yang Lijie Sun Hongfei Huang Rasoul Esmaeely Neisiany Zhengwei You State Key Laboratory for Modification of Chemical Fibers and polymer Materials Institute of Functional MaterialsCollege of Materials Science and EngineeringDonghua UniversityResearch Base of Textile Materials for Flexible Electronics and Biomedical Applications(China Textile Engineering Society)Shanghai Engineering Research Center of Nano-Biomaterials and Regenerative MedicineShanghai 201620China department of polymer engineering Hakim Sabzevari UniversitySabzevar ***Iran Biotechnology Centre Silesian University of TechnologyGliwice 44-100Poland

Inspired by the multi-layer architecture of mammal skins,interfacial robust,stretchable,and entirely healable gel-elastomer hybrids hold great potential in diverse fields including biomedical devices,wearable electrical devices,and soft ***,existing gel-elastomer hybrids have numerous limitations including low interfacial bonding toughness,complex and time-consuming preparation process,unhealable,and ***,we propose a simple and general chemical strategy through the interfacial dynamic bonding between gel and elastomer to simultaneously address the abovementioned *** covalent bonds readily and repeatably covalent bonding ionogel and elastomer(interfacial toughness:390 J m^(-2)),endowed the hybrids with entire self-healing features like skin and enabled discretionary assembly and ***,this strategy resolved the troublesome contradiction between interfacial stability and *** advantage of the aforementioned features,we readily constructed a multi-module,self-healing,self-powered,and realtime monitoring of personal status integrated elastic electronics,which could simply reconfigure the output signal of elastic electronics into an input signal of the devices-braille keyboard.

关键词： ionogel elastomer interface bonding self-healing dynamic covalent bond

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Study on Catalytic Behavior of Iron-based Catalyst with IITP as Electron Donor in the polymerization of Butadiene

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Chinese Journal of polymer Science 2024年第5期42卷 612-619,I0007页

作者： Shi-Liang Xu Ying-Nan Zhao Yao Yu Qi Yang Li-Hua Na Heng Liu Chun-Yu Zhang Xue-Quan Zhang Key Laboratory of Advanced Rubber Material Ministry of EducationSchool of Polymer Science and EngineeringQingdao University of Science&TechnologyQingdao266042China Shandong Provincial College Laboratory of Rubber Material and engineering School of Polymer Science and EngineeringQingdao University of Science&TechnologyQingdao266042China Key Lab of Rubber-Plastics Ministry of Education/Shandong Provincial Key Lab of Rubber-plasticsSchool of Polymer Science and EngineeringQingdao University of Science&TechnologyQingdao266042China

In this study,a novel iron-based catalyst system,Fe(acac)3/(isocyanoimino)triptenylphosphorane(IITP)/AlR3,was employed for the synthesis of syndiotactic 1,2-polybutadiene in *** catalyst system exhibits remarkably high catalytic activity,achieving a polymerization activity of 762 kgpolymer·molcatalyst^(-1)·h^(-1)at 50℃with a[BD]/[Fe]molar ratio of ***,living polymerization characteristic were observed during the investigation of the polymerization kinetics of 1,3-butadiene *** characteristics were well demonstrated by a narrow molecular weight distribution(PDI≈2.0)of the resulting polybutadiene and a linear relationship between-ln(1-c)and polymerization time as well as number average molecular weight and polymer *** resultant polymer showed a 1,2-selectivity of approximately 76%and stereoregularity ranging from 62%to 73%(rrrr).Additionally,through kinetic studies on polymerization reaction,an apparent activation energy Ea value of this catalytic system was calculated to be 84.98 kJ·mol^(-1),which suggests that high polymerization temperature favors efficient polymerization.

关键词： Iron catalyst Syndiotactic 1,2-polybutadiene Elastomers Donor Selectivity

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Improving Thermal-oxidative Aging Resistance of Styrene-butadiene Rubber by Antioxidant Loaded Silica Aerogel

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Chinese Journal of polymer Science 2024年第8期42卷 1198-1209页

作者： Xue-Fei Ping Yu Wang Lu Liu Fu-Yong Liu Hong-Wei He Pi Wang Wen-Wen Yu Qiang Zheng College of Materials Science and engineering Taiyuan University of TechnologyTaiyuan 030024China Shanxi-Zheda Institute of Advanced Materials and Chemical engineering Taiyuan 030032China Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310058China

The antioxidant N-isopropyl-N'-phenyl-p-phenylenediamine(4010NA)was dissolved in ethanol and impregnated into silica aerogel(SAG)via vacuum-pressure cycles,yielding composite particles(A-N)with enhanced sustained-release and reinforcing *** effect of A-N on the mechanical properties and thermal-oxidative aging resistance of styrene-butadiene rubber(SBR)vulcanizates was *** and BET assessments indicated that the loading efficiency of 4010NA in SAG reached 14.26%within ethanol's solu bility *** A-N into SBR vulcanizates significantly elevated tensile strength by 17.5%and elongation at break by 41.9%over those with fumed silica and ***,A-N notably enhanced the thermal-oxidative aging resistance of *** aging for 96 h at 100℃,the tensile strength and elongation at break of SBR with A-N sustained 70.09%and 58.61%of their initial values,respectively,with the retention rate of elongation at break being 62.8%higher than that of SBR with fumed silica and free *** study revealed that A-N composite particles significantly inhibited the crosslinking in SBR's molecular chains,reducing hardening and embrittlement during later thermal-oxidative aging stages.

关键词： Styrene-butadiene rubber Silica aerogel Loading modification Thermal-oxidative aging

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Antibacterial and antioxidant bifunctional hydrogel based on hyaluronic acid complex MoS_(2)-dithiothreitol nanozyme for treatment of infected wounds

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Regenerative Biomaterials 2024年第4期3卷 98-110页

作者： Yongping Lu Weiqi Kang Yue Yu Ling Liang Jinrong Li Haiying Lu Ping Shi Mingfang He Yuemin Wang Jianshu Li Xingyu Chen Guangyuan Central Hospital Guangyuan 628000P.R.China State Key Laboratory of polymer Materials engineering College of Polymer Science and EngineeringSichuan UniversityChengdu 610065P.R.China Institute of Biomedical engineering College of MedicineSouthwest Jiaotong UniversityChengdu 610031P.R.China

Wound repair is a complex physiological process that often leads to bacterial infections,which significantly threaten human ***,developing wound-healing materials that promote healing and prevent bacterial infections is *** this study,the coordination interaction between sulfhydryl groups on dithiothreitol(DTT)and MoS_(2)nanosheets is investigated to synthesize a MoS_(2)-DTT nanozyme with photothermal properties and an improved free-radical scavenging ***-bond-modified hyaluronic acid is used as a monomer and is cross-linked with a PF127-DA *** is prepared in coordination with MoS_(2)-DTT as the functional *** hydrogel exhibits antioxidant and antibacterial properties,attributed to the catalytic activity of catalase-like enzymes and photothermal *** the near-infrared(NIR),it exhibits potent antibacterial effects against gram-positive(Staphylococcus aureus)and gram-negative bacteria(Escherichia coli),achieving bactericidal rates of 99.76%and 99.42%,***,the hydrogel exhibits remarkable reactive oxygen species scavenging and antioxidant capabilities,effectively countering oxidative stress in L929 ***,in an animal model,wounds treated with the PHMoD(2.0)and NIR laser heal the fastest,sealing completely within 10 *** results indicate the unique biocompatibility and bifunctionality of the PHMoD,which make it a promising material for wound-healing applications.

关键词： hydrogel wound repair antibacterial antioxidant nanozyme photothermal therapy

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Bioinspired anti-freezing 3D-printable conductive hydrogel microfibers for highly-sensitive and wide-range detection of ultralow and high strains

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Green Chemical engineering 2024年第1期5卷 132-143页

作者： Yi-Min Yang Ting-Yuan Hu Haidong Fan Lu Shi Shi-Yuan Zhang Zhuang Liu Xiao-Jie Ju Rui Xie Wei Wang Liang-Yin Chu School of Chemical engineering Sichuan UniversityChengdu610065China department of Mechanics Sichuan UniversityChengdu610065China State Key Laboratory of polymer Materials engineering Sichuan UniversityChengdu610065China

Soft strain sensors that can transduce stretch stimuli into electrical readouts are promising as sustainable wearable ***,most strain sensors cannot achieve highly-sensitive and wide-range detection of ultralow and high *** by bamboo structures,anti-freezing microfibers made of conductive poly(vinyl alcohol)hydrogel with poly(3,4-ethylenedioxythiphene)-poly(styrenesulfonate)are developed via continuous microfluidic *** microfibers provide unique bamboo-like structures with enhanced local stress to improve both their length change and resistance change upon stretching for efficient signal *** microfibers allow highlysensitive(detection limit:0.05%strain)and wide-range(0%-400%strain)detection of ultralow and high strains,as well as features of good stretchability(485%strain)and anti-freezing property(freezing temperature:-41.1°C),fast response(200 ms),and good *** experimental results,together with theoretical foundation analysis and finite element analysis,prove their enhanced length and resistance changes upon stretching for efficient signal *** integrating microfluidic spinning with 3D-printing technique,the textiles of the microfibers can be flexibly *** microfibers and their 3D-printed textiles enable highperformance monitoring of human motions including finger bending and throat vibrating during *** work provides an efficient and general strategy for developing advanced conductive hydrogel microfibers as highperformance wearable strain sensors.

关键词： Conductive hydrogel microfibers Microfluidics Sensitive detection Wide detection range Anti-freezing

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π-conjugated chromophore functionalized high-nuclearity titanium-oxo clusters containing structural unit of anatase for photocatalytic selective oxidation of sulfides

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Rare Metals 2024年第4期43卷 1736-1746页

作者： Ling-Rong Liao Dong-Chun Zheng Pin-Xi Ou Qi-Xin Zhao Wei-Min Xuan Qi Zheng State Key Laboratory for Modification of Chemical Fibers and polymer Materials&College of Materials Science and engineering Donghua UniversityShanghai201620China State Key Laboratory for Modification of Chemical Fibers and polymer Materials and College of Chemistry and Chemical engineering Donghua UniversityShanghai 201620China

N-doping has significant influence in manipulating the properties of TiO_(2),and this has stimulated the development of N-donor-functionalized titanium-oxo clusters(TOCs)as molecular models to study the structure-property ***,the structural type and photoresponsive application are still limited for such TOCs,especially regarding the high-nuclearity TOCs that contain structure unit of TiO_(2)for ***,we showed the synthesis of a series of high-nuclearity TOCs 1-3 compounds usingπ-conjugated 1,10-phenanthroline(phen)as chromophore and N-donor functional *** 1 features cocrystal structure composed of one[Ti_(26)]~(2+)and half[Ti_(22)]~(2+),which renders it as the first cocrystallized TOC containing two positively charged species and phen-functionalized TOC showing the highest nuclearity up to 37 Ti *** adjusting the synthetic conditions,the individual{Ti_(22)}and{Ti_(26)}clusters can also be isolated as Compounds 2 and 3,*** core structure of{Ti_(22)}is mainly constructed from four lacunary{Ti_(4)}derived from pentagonal{Ti(Ti)_5}unit,while{Ti_(26)}is built from four complete{Ti(Ti)_5}***,a{Ti_8O_(14)}structure unit of anatase TiO_(2)can be identified in{Ti_(26)}.Based on the unique structural features and proper photophysical and photochemical properties of Compounds 1-3,they are applied for photocatalytic *** to the presence of anatase structure unit in{Ti_(26)}and the synergistic effect from{Ti_(22)}and{Ti_(26)},the catalytic performance presents in the order of Compound 1>Compound 3>Compound *** work provides excellent models to understand the structureproperty relationship from the perspective of cocrystallization and Ti-O binding model and will further promote the application of TOCs as functional catalysts for organic transformation.

关键词： Titanium-oxo cluster Molecular model of anatase TiO_(2) High nuclearity π-conjugated chromophore Photocatalytic sulfoxidation

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