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Effects of serum proteins on corrosion rates and product bioabsorbability of biodegradable metals

Regenerative Biomaterials 2024年第1期3卷 132-148页

作者： Hongjie Zhang Xin Li Zehua Qu Wanqian Zhang Qunsong Wang Dinglingge Cao Yaoben Wang Xin Wang Yang Wang Lin Yu Jiandong Ding State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200438China

Corrodible metals are the newest kind of biodegradable materials and raise a new problem of the corrosion ***,the removal of the precipitated products has been unclear and even largely ignored in ***,we find that albumin,an abundant macromolecule in serum,enhances the solubility of corrosion products of iron in blood mimetic Hank’s solution *** is universal for other main biodegradable metals such as magnesium,zinc and polyester-coated *** also influences corrosion rates in diverse trends in Hank’s solution and normal *** on quantitative study theoretically and experimentally,both the effects on corrosion rates and soluble fractions are interpreted by a unified mechanism,and the key factor leading to different corrosion behaviors in corrosion media is the interference of albumin to the Ca/P passivation layer on the metal *** work has illustrated that the interactions between metals and media macromolecules should be taken into consideration in the design of the next-generation metal-based biodegradable medical devices in the formulism of precision *** improved Hank’s solution in the presence of albumin and with a higher content of initial calcium salt is suggested to access biodegradable metals potentially for cardiovascular medical devices,where the content of calcium salt is calculated after consideration of chelating of calcium ions by albumin,resulting in the physiological concentration of free calcium ions.

关键词： biodegradable metal macromolecule albumin corrosion bioabsorbability iron polylactide magnesium zinc

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Polymer Degradation via a Mechanochemical Gating Strategy

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Chinese Journal of Chemistry 2025年第3期43卷 349-354页

作者： Xiaojing Liang Hai Qian State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai200438 China

The extensive use of plastics,valued for their lightweight,durability,and cost-effectiveness,has led to severe environmental pollution,with 72%of plastic waste ending up in landfills or natural *** methods for plastic decomposition,including both mechanical and chemical approaches,often face challenges such as incomplete degradation and stability *** innovative concept of mechanical gating presents a promising solution by incorporating mechanophores into polymer structures,enabling controlled *** advancements have focused on utilizing mechanophores,such as cyclobutane,as"door locks"to regulate the degradation *** perspective highlights recent progress in this field,demonstrating the potential of mechanophore-based strategies for achieving on-demand polymer *** addresses the limitations of conventional recycling methods and explores how this approach can balance polymer stability with environmental degradability,paving the way for more sustainable plastic management solutions.

关键词： Polymer mechanochemistry Polymer degradation Mechanophores Mechanical gating Recyclable polymers

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Ultrathin and capacity-tunable lithium metal wires for lithium-based fiber batteries

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National science Review 2025年第3期12卷 274-283页

作者： Chuanfa Li Qian Ye Jiaqi Wang Xinlin Huang Tianbing Song Kun Zhang Pengzhou Li Yanan Zhang Xiaocheng Gong Yi Jiang Yue Gao Huisheng Peng Bingjie Wang State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Science Institute of Fiber Materials and Devices and Laboratory of Advanced Materials Fudan University

Ultrathin lithium（Li） metal wires with tunable capacities have great promise for precise prelithiation of fiber anodes and high-energy-density Li-based fiber batteries. However, the application of Li metal in fiber batteries faces great challenges due to its mechanical fragility and the resulting limited micro-dimension manufacturing capability. These challenges impede the production of ultrathin Li wires with adjustable Li contents to match the capacities of Li-based fiber batteries. Herein, silver-plated aramid yarns（Ag/AYs） are employed to load Li metal for producing ultrathin Li wires. The bundled structure of Ag/AYs leads to the adjustable volume of oriented voids within the fibers, thus resulting in accurately tunable capacities(0.0048–2.4 m Ah cm-1) and diameters（20–534 μm） of Li wires. Such thin Li wires are used to precisely compensate for Li loss during the formation cycle of the fiber graphite anodes, thereby improving the initial Coulombic efficiency from ～88% to ～100%. Additionally, when employed as anodes, these Li wires enabled the fiber batteries to exhibit exceptional cycling stability for 150 cycles under a relatively low negative/positive ratio of 2.06, while achieving a high energy density of 139.822 Wh kg-1based on the total mass of the battery.

关键词： ultrathin Li wires tunable capacities precise prelithiation high-energy-density fiber batteries

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Production of Functional Materials Derived from Regenerated Silk Fibroin by Utilizing 3D Printing and Biomimetic Enzyme-induced Mineralization

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Chinese Journal of Polymer science 2024年第3期42卷 299-310,I0005页

作者： Ni Chen Fei-Yu Luo Gong-Wen Yang Jin-Rong Yao Xin Chen Zheng-Zhong Shao State Key Laboratory of Molecular Engineering of Polymers Laboratory of Advanced Materials and Department of Macromolecular ScienceFudan UniversityShanghai 200433China

Critical-sized bone defects, commonly encountered in clinical orthopedic surgery, present a significant challenge. One of the promising solutions is to prepare synthetic bone substitute materials with precise structural control, mechanical compatibility, and enhanced osteogenic induction performance, nevertheless the successful preparation of such materials remains difficult. In this study, a two-step technique,integrating an extrusion-based printing process with biomimetic mineralization induced by alkaline phosphatase(ALP), was developed. Initially,a pre-cured hydrogel of regenerated silk fibroin(RSF) with a small quantity of hydroxypropyl cellulose(HPC) and ALP was prepared through heating the mixed aqueous solution. This pre-cured hydrogel demonstrated thixotropic property and could be directly extruded into predetermined structures through a 3D-printer. Subsequently, the 3D-printed RSF-based materials with ALP underwent biomimetic in situ mineralization in calcium glycerophosphate(Ca-GP) mineralizing solution, utilizing the polymer chains of RSF as templates and ALP as a trigger for cleaving phosphate bonds of Ca-GP. The resulting 3D-printed RSF-mineral composites including hydrogel and sponge possessed adjustable compression modulus of megapascal grade and variable hydroxyapatite content, which could be controlled by manipulating the duration of the mineralization ***, these 3D-printed RSF-mineral composites demonstrated non-cytotoxicity towards rat bone marrow mesenchymal stem cells. Therefore, they may hold great potential for applications involving the replacement of tissues characterized by osteoinductivity and intricate structures.

关键词： Silk protein Alkaline phosphatase Extrusion-based printing Biomineralization

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Regulating the Photoisomerization of Covalent Organic Framework for Enhanced Photocatalytic Hydrogen Evolution

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Chinese Journal of Chemistry 2024年第21期42卷 2621-2626页

作者： Xingye Huang Jia Guo State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai200438 China

Covalent organic framework(COF)is a desirable platform to tailor electronic properties for improving photocatalytic ***,the study on excited-state configurations that determine photogenerated carrier dynamics has long been ***,we concentrate on the molecular design ofβ-ketoenamine-linked COFs to drive their photoisomerization via the excited-state intra-molecular proton transfer(ESIPT),which can induce the partial keto-to-enol tautomerization and accordingly rearrange the photoinduced charge *** demonstrate that the push-pull electronic effect of functional side groups attached on the framework linkers is directly correlated with the ESIPT *** phenylene linkers modified with electron-withdrawing cyano-groups reinforce the ESIPT-induced tautomerization,leading to the in situ partial enolization for extendedπ-conjugation and rearranged electron-hole *** contrast,the electron-rich linkers limit the photoisomerization of COF and suppress the photoinduced electron ***,the maximum hydrogen evolution rate is achieved by the cyano-modified COF,reaching as high as 162.72 mmol·g^(-1)·h^(-1) with an apparent quantum efficiency of 13.44%at 475 nm,which is almost 11.5-fold higher than those of analogous COFs with electron-rich *** work opens up an avenue to control over the excited-state structure transformation for enhanced photochemical applications.

关键词： Covalent organic framework Hydrogen evolution reaction Photoisomerization Photocatalysis Charge separation Water splitting

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Emerging Bio-relevant Applications of Polymer Mechanochemistry

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Chinese Journal of Chemistry 2024年第17期42卷 2066-2070页

作者： Wenjie Liu Hai Qian State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200438China

Polymer mechanochemistry has rapidly evolved since the *** advancements highlight the development of mechanophore platforms for the controlled release of bioactive payloads and the exploration of biocompatible activation *** platforms,ranging from furan-maleimide Diels-Alder adducts to disulfide motifs withβ-carbonate linkages,demonstrate promising prospects in targeted drug ***,supramolecular assemblies and free radical-generating mechanophores present innovative avenues for potential therapeutic *** activation methods,notably high-intensity and/or low-intensity focused ultrasound,hold potential for in vivo ***,challenges persist in comprehending the fundamental physics of ultrasound and its utilization for activation.

关键词： Polymer mechanochemistry Mechanophores Bio-relevant applications Ultrasound Drug delivery

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Semiconductor fibers for textile integrated electronic systems

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National science Review 2024年第6期11卷 100-101页

作者： Yuanyuan Zheng Zhen Wang Peining Chen Huisheng Peng State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceInstitute of Fiber Materials and Devices and Laboratory of Advanced Materials Fudan University

Over 5000 years of development, the functions of clothing have been mainly limited in warmth and modesty. With the development of smart fibers, fabrics are anticipated to revolutionize multidisciplinary applications, ... 详细信息

关键词： Fibers

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Alternating current electroluminescent fibers for textile displays

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National science Review 2023年第1期10卷 14-16页

作者： Zhen Wang Xiang Shi Huisheng Peng State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Scienceand Laboratory of Advanced Materials Fudan University

With the emerging 5G and Internet of Things,wearables are developing vigorously [1].Wearables are expected to be flexible,lightweight,breathable and comfortable to satisfy daily applications[2].Integrating electronic devices into textiles to form an electronic textile(e-textile) will simultaneously meet the above requirements and the need for daily clothes.E-textiles with functions of communicating,sensing and supplying power have been widely explored.

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Stride Strategy to Enable a Quasi-ergodic Search of Reaction Pathways Demonstrated by Ring-opening Polymerization of Cyclic Esters

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Chinese Journal of Polymer science 2023年第5期41卷 745-759,I0009页

作者： Wei-Han Rao Lin Yu Jian-Dong Ding State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200438China

Coordination-insertion ring-opening polymerization(ROP)of cyclic esters is an industrial way to synthesize polyesters,which are widely applied in biomedical and environment-benign ***,the rate-determining transition state(TS)identified by the conventional reaction pathways(pathway A and pathway B)presented in the literature did not well describe the structure-reactivity *** misidentification of the rate-determining TS might arise from the less ergodicity in the search of reaction ***,we suggested a stride strategy based on the insight that even a partial double bond is rotatable at the catalysis *** a result,we revealed a new reaction pathway,pathway C with a torsion transition state TSC2,by density functional theory(DFT).We also carried out kinetic experiments of ROP of D-lactide(D-LA),L-lactide(L-LA),ε-caprolactone(CL),andδ-valerolactone(VL),using poly(ethylene glycol)as the initiator and stannous octoate as the *** excellent linearity between the calculated free energy barriers and logarithms of the experimental kinetic constants of the two kinds of lactide and lactone monomers,was established,validating the quasi-ergodic search of reaction pathways and the scaling predicted by transition state *** linearity was highly predictive for the other lactide and lactone monomers,demonstrated by glycolide(GA)and trimethylene urethane(TU).

关键词： Coordination-insertion mechanism Ring-opening polymerization Density functional theory Biodegradable polymer Lactide Lactone Cyclic ester

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Meniscus-Assisted Solution Printing Enables Cocrystallization in Poly(3-alkylthiophene)-based Blends for Field-Effect Transistors

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Chinese Journal of Polymer science 2023年第8期41卷 1269-1276,I0009页

作者： Shu-Yin Zhu Juan Peng State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200438China

The formation of cocrystallization in two various conjugated components may endow the newly formed conjugated cocrystals with multiple functionalities and improved charge transport ***,compared to conjugated small molecules,this strategy is rather limitedly realized in conjugated ***,a simple meniscus-assisted solution printing(MASP)strategy is utilized to achieve the cocrystallization in the blends of two conjugated polymers,i.e.,poly(3-hexylthiophene)(P3HT)and poly(3-octylthiophene)(P3OT),and the cocrystalline structures are correlated closely to their charge *** P3HT/P3OT blends phase separate and crystallize individually in their drop-cast thin *** subjecting the P3HT/P3OT blended solution to MASP,the confined solvent evaporation between two nearly parallel plates triggers them to cocrystallize progressively when accelerating the moving lower *** cocrystallization kinetics and the changes in P3HT/P3OT molecular structures are ***,these different crystalline structures of P3HT/P3OT blends are applied in organic fieldeffect transistors,imparting the cocrystallization-enhanced charge transport than respective P3HT and P3OT crystal *** MASP method can be extended to craft cocrystals of other conjugated polymer blends for their diverse optoelectronic applications.

关键词： Conjugated polymer blends Polythiophene Cocrystallization Charge mobility Meniscus-assisted solution printing

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