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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 products.However,the removal of the precipitated products has been unclear and even largely ignored in publications.Herein,we find that albumin,an abundant macromolecule in serum,enhances the solubility of corrosion products of iron in blood mimetic Hank’s solution significantly.This is universal for other main biodegradable metals such as magnesium,zinc and polyester-coated iron.Albumin also influences corrosion rates in diverse trends in Hank’s solution and normal saline.Based 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 surface.This 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 medicine.The 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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Recent progress on rapid diagnosis of COVID-19 by point-of-care testing platforms

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Chinese Chemical Letters 2024年第3期35卷 66-75页

作者： Ya-Nan Tang Dingding Jiang Xuejun Wang Yunqi Liu Dacheng Wei State Key Laboratory of molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200433China Institute of molecular Materials and Devices Fudan UniversityShanghai 200433China

The outbreak of COVID-19 has drawn great attention around the world.SARS-CoV-2 is a highly infectious virus with occult transmission by many mutations and a long incubation period.In particular,the emergence of asymptomatic infections has made the epidemic even more severe.Therefore,early diagnosis and timely management of suspected cases are essential measures to control the spread of the virus.Developing simple,portable,and accurate diagnostic techniques for SARS-CoV-2 is the key to epidemic prevention.The advantages of point-of-care testing technology make it play an increasingly important role in viral detection and screening.This review summarizes the point-of-care testing platforms developed by nucleic acid detection,immunological detection,and nanomaterial-based biosensors detection.Furthermore,this paper provides a prospect for designing future highly accurate,cheap,and convenient SARS-CoV-2 diagnostic technology.

关键词： COVID-19 Point-of-care testing platforms Nucleic acid detection Asymptomatic infection Biosensors

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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 process.Moreover, 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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Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage

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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li department of chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University State Key Laboratory of Surface Physics and department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable challenge.Herein,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as templates.The key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon matrix.The mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion lengths.This method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

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Knittable and washable aerogel fiber inspired by polar bear hair

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Science China Materials 2024年第2期67卷 705-706页

作者： Yue Liu Huisheng Peng State Key Laboratory of molecular Engineering of Polymers Department of Macromolecular Scienceand Institute of Fiber Materials and DevicesFudan UniversityShanghai 200438China

The advances in chemistry and materials have boosted the development of smart textiles,which are poised to revolutionize human lifestyles through multifunctional integration,such as heating,cooling,sensing and supplying energy^([1,2]).Among them,thermal insulation is an essential function of textiles to protect humans from complex and extreme environments and realize personal thermal management without energy con-sumption^([3]).

关键词： textiles insulation extreme

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Supramolecular Polymerization of Hydrogen-Bonded Trimers in Bulk and Aqueous Medium

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CCS chemistry 2024年第6期6卷 1458-1465页

作者： Freek V.de Graaf Stef A.H.Jansen Sandra M.C.Schoenmakers Bas van Genabeek Marle E.J.Vleugels Bart W.L.van den Bersselaar E.W.Meijer Ghislaine Vantomme Institute for Complex molecular Systems Laboratory of Macromolecular and Organic ChemistryEindhoven University of Technology5600 MBEindhoven School of chemistry and RNA Institute University of New South WalesSydneyNew South Wales 2052

Synthetic molecules that form functional noncovalent assemblies in water have received much attention for their potential applications as biomaterials.In this work,we introduce a novel water-compatible monomer based on the phthalhydrazide moiety that assembles into hydrogen-bonded trimeric discs.In bulk,the material exhibits a cylindrical nanostructure in the liquid-crystalline phase at elevated temperatures,morphologically distinct from the crystalline lamellar phase.In water,these molecules effectively form cylinders in a one-dimensional fashion,yielding fibrous structures.The formation of these supramolecular polymers follows a cooperative mechanism,as evidenced by denaturation studies.The trimerized pattern represents a new category of aqueous su pramolecular polymers with future prospects for functional complex molecular systems.

关键词： noncovalent chemistry supramolecular polymers hydrogen bonding cooperativity nanostructure

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Interparticle energy transfer between NaNdF_(4) and NaYbF_(4) in self-assembled nanostructures

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Journal of Rare Earths 2024年第6期42卷 1029-1035,I0001页

作者： Xinyu Chen Haoze Yang Yuyang Gu Chenqing Wen Yishuo Sun Jiaming Ke Wei Feng department of chemistry and State Key Laboratory of molecular Engineering of Polymers Fudan University Shanghai200433China

Forster resonance energy transfer(FRET)is a widely used spectroscopic technique.The development of donor-acceptor combinations is essential to advance this technique.To make the energy transfer efficiency independent of the external environment,we explored the potential of constructing donor—acceptor combinations with lanthanide ion-doped nanoparticles(LNPs),in which the 4f electrons of the lanthanide ions are shielded by the 5s and 6p electrons.Non-radiative energy transfer between LNPs was demonstrated in self-assembled nanostructures and core-shell structure of LNPs was used to control the distance between donor and acceptor in self-assembled nanostructures.The emission intensity ratio of donor and acceptor illustrates that the energy transfer efficiency decreases significantly with increasing distance and the effective energy transfer distance is 8.5 nm,showing the potential of using LNPs as donor-acceptor pairs in the construction of distance-dependent energy transfer system.

关键词： Lanthanide nanoparticles Self-assembly Energy transfer Distance Epitaxialgrowth Rare earths

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Beneficial use of mussel shell as a bioadditive for TPU green composites by the valorization of an aqueous waste

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Waste Disposal and Sustainable Energy 2024年第1期6卷 123-137页

作者： SedefŞişmanoğlu Yasin Kanbur Carmen-Mihaela Popescu Diana Kindzera Ümit Tayfun department of chemistry Karabuk University78050KarabukTurkey Petru Poni Institute of macromolecular chemistry of the Romanian Academy 700487IasiRomania department of Chemical Engineering Lviv Polytechnic National UniversityLviv79013Ukraine department of Basic Sciences Bartin University74110BartinTurkey

Scientific studies have focused on environmentally friendly solutions as effective as the reuse of crop products owing to plastic-waste problems in recent years.This issue is the main driving force for upcoming academic research attempts in waste valorization-related studies.Herein,we integrated an aqua-waste,mussel shell(MS),as a bioadditive form into green thermoplastic polyurethane(TPU)green composites.Tuning of the MS surface was performed to achieve strong adhesion between composite phases.The surface functionalities of MS powders were evaluated via infrared spectroscopy and scanning electron microscopy(SEM)images.Composite samples were prepared by melt-compounding followed by injection molding techniques.It was confirmed by morphological analysis that relatively better adhesion between the phases was achieved for composites involving surface-modified MS compared to unmodified MS.Tensile strength and Young’s modulus of surface-modified MS-filled composites were found to be higher than those of unmodified MS,whereas the elongation at break shifted to lower values with MS inclusions.The shore hardness of TPU was remarkably improved after being incorporated with silane-treated MS(AS-MS).Stearic acid-treated MS(ST-MS)additions resulted in an enhancement in the thermal stability of the composites.Thermo-mechanical analysis showed that the storage moduli of composites were higher than those of unfilled TPU.ST-MS additions led to an increase in the characteristic glass transition temperature of TPU.Melt flow index(MFI)of neat TPU was highly improved after MS loading regardless of modification type.According to the wear test,surface modification of MS displayed a positive effect on the wear resistance of TPU.As the water absorption data of the composites were evaluated,the TPU/AS-MS composite yielded the lowest water absorption.The silane layer on MS inclusion promoted water repellency of composites due to the hydrophobicity of silane.The results of the biodegradation investigation demonstrated that adding unmodifie

关键词： Aqua-waste Polyurethane Mussel shell Green composites Sustainability Waste valorization

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AI for organic and polymer synthesis

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Science China chemistry 2024年第8期67卷 2461-2496页

作者： Xin Hong Qi Yang Kuangbiao Liao Jianfeng Pei Mao Chen Fanyang Mo Hua Lu Wen-Bin Zhang Haisen Zhou Jiaxiao Chen Lebin Su Shuo-Qing Zhang Siyuan Liu Xu Huang Yi-Zhou Sun Yuxiang Wang Zexi Zhang Zhunzhun Yu Sanzhong Luo Xue-Feng Fu Shu-Li You department of Chemical Sciences National Natural Science Foundation of China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences Center of chemistry for Frontier Technologies Department of Chemistry Zhejiang University Center of Basic molecular Science Department of Chemistry Tsinghua University Guangzhou National Laboratory Center for Quantitative Biology Academy for Advanced Interdisciplinary Studies Peking University State Key Laboratory of molecular Engineering of Polymers Department of Macromolecular Science Fudan University School of Materials Science and Engineering Peking University AI for Science (AI4S)-Preferred Program Shenzhen Graduate School Peking University Beijing National Laboratory for molecular Sciences Center for Soft Matter Science and Engineering Key Laboratory of Polymer Chemistry and Physics of Ministry of Education College of Chemistry and Molecular Engineering Peking University State Key Laboratory of Chemical Biology Shanghai Institute of Organic Chemistry University of Chinese Academy of SciencesChinese Academy of Sciences

Recent years have witnessed the transformative impact from the integration of artificial intelligence with organic and polymer synthesis. This synergy offers innovative and intelligent solutions to a range of classic problems in synthetic chemistry. These exciting advancements include the prediction of molecular property, multi-step retrosynthetic pathway planning, elucidation of the structure-performance relationship of single-step transformation, establishment of the quantitative linkage between polymer structures and their functions, design and optimization of polymerization process, prediction of the structure and sequence of biological macromolecules, as well as automated and intelligent synthesis platforms. Chemists can now explore synthetic chemistry with unprecedented precision and efficiency, creating novel reactions, catalysts, and polymer materials under the datadriven paradigm. Despite these thrilling developments, the field of artificial intelligence(AI) synthetic chemistry is still in its infancy, facing challenges and limitations in terms of data openness, model interpretability, as well as software and hardware support. This review aims to provide an overview of the current progress, key challenges, and future development suggestions in the interdisciplinary field between AI and synthetic chemistry. It is hoped that this overview will offer readers a comprehensive understanding of this emerging field, inspiring and promoting further scientific research and development.

关键词： automated synthesis chemical database machine learning prediction organic synthesis polymer synthesis

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Nanomaterial Assisted Exosome Analysis Using Mass Spectrometry

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Chemical Research in Chinese Universities 2024年第2期40卷 237-254页

作者： ZHANG Yi ZHOU Bokai LI Qiuning JIN Mingshi BAI Yu Beijing National Laboratory for molecular Sciences Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871P.R.China department of chemistry Yanbian UniversityYanji133002P.R.China

Exosomes,extracellular vesicles(EVs)that play crucial roles in biological processes,have emerged as attractive targets for noninvasive disease diagnosis and monitoring.Mass spectrometry(MS)offers high sensitivity,high throughput,and excellent qualification and quantification capacity,which is the ideal approach for exosome analysis.Nanomaterials’unique physiochemical properties,controllable morphology,and large surface area make them promising in biological sample pretreatment and detection.They contributed diverse functions to the exosome MS analysis,encompassing substrates for exosome isolation and cargos enrichment,matrices for laser desorption/ionization(LDI),read-out signals and supporters for signal amplification strategies,etc.In this review,recent progress in the applications of nanomaterial in the exosome MS analysis was summarized and a comprehensive discussion on the challenges and perspectives was proposed for the development of an advancing analysis approach of exosomes for the accurate diagnosis and monitoring of diseases.

关键词： Exosome Nanomaterial Enrichment Matrix Mass spectrometry

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