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Block Sequence Effects on the Self-Assembly Behaviors of Polypeptide-Based Penta-Block Copolymer Hydrogels

ACS Applied Materials and Interfaces 2024年第5期16卷 6674-6686页

作者： Wang, Ke-Hsin Liu, Chung-Hao Tan, Dun-Heng Nieh, Mu-Ping Su, Wei-Fang Department of Materials Science and Engineering National Taiwan University No. 1 Sec. 4 Roosevelt Road Taipei10617 Taiwan Polymer program Institute of Materials Science University of Connecticut 25 King Hill Road Unit 3136 StorrsCT06269-3136 United States Department of Chemical and Biomolecular Engineering University of Connecticut StorrsCT06269 United States Department of Materials Engineering Ming-Chi University of Technology 84 Gungjuan Rd. New Taipei City243303 Taiwan

Peptide-based hydrogels have great potential for applications in tissue engineering, drug delivery, and so on. We systematically synthesize, characterize, and investigate the self-assembly behaviors of a series of polypeptide-based penta-block copolymers by varying block sequences and lengths. The copolymers contain hydrophobic blocks of poly(γ-benzyl-l-glutamate) (PBG, Bx) and two kinds of hydrophilic blocks, poly(l-lysine) (PLL, Ky) and poly(ethylene glycol) (PEG, EG34), where x and y are the number of repeating units of each block, where PBG and PLL blocks have unique functions for nerve regeneration and cell adhesion. It shows that a sufficient length of the middle hydrophilic segment capped with hydrophobic end PBG blocks is required. They first self-assemble into flower-like micelles and sequentially form transparent hydrogels (as low as 2.3 wt %) with increased polymer concentration. The hydrogels contain a microscale porous structure, a desired property for tissue engineering to facilitate the access of nutrient flow for cell growth and drug delivery systems with high efficiency of drug storage. We hypothesize that the structure of Bx-Ky-EG34-Ky-Bx agglomerates is beyond micron size (transparent), while that of Ky-Bx-EG34-Bx-Ky is on the submicron scale (opaque). We establish a working strategy to synthesize a polypeptide-based block copolymer with a wide window of sol-gel transition. The study offers insight into rational polypeptide hydrogel design with specific morphology, exploring the novel materials as potential candidates for neural tissue engineering. © 2024 The Authors. Published by American Chemical Society

关键词： Block copolymers

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Biomass-Based Discrete Furan Oligomers as Materials for Electrochromic Devices

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ACS Sustainable Chemistry and Engineering 2024年第1期12卷 459-469页

作者： Atayde, Eduardo C. Fong, Guan-Lun Yeh, Jyun-Yi Matsagar, Babasaheb M. Wang, Yu-Cheng Chen, De-Chian Peng, Chi-How Li, Yi-Pei Yamauchi, Yusuke Ho, Kuo-Chuan Wu, Kevin C.-W. Molecular Science and Technology Program Taiwan International Graduate Program (TIGP-MST) Academia Sinica No. 128 Sec. 2 Academia Road Taipei 11529 Taiwan Department of Chemistry National Tsing Hua University No. 101 Sec. 2 Kuang-Fu Road Hsinchu 30013 Taiwan Department of Chemical Engineering National Taiwan University No. 1 Sec. 4 Roosevelt Road Taipei 10617 Taiwan Sustainable Chemical Science and Technology Program Taiwan International Graduate Program (TIGP-SCST) Academia Sinica No. 128 Sec. 2 Academia Road Taipei 11529 Taiwan School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology (AIBN) The University of Queensl Brisbane 4072 QLD Australia Department of Materials Process Engineering Graduate School of Engineering Nagoya University Nagoya 464-8603 Japan Institute of Polymer Science and Engineering National Taiwan University No.1 Sec. 4 Roosevelt Rd. Taipei 10617 Taiwan Department of Chemical Engineering and Materials Science Yuan Ze University No. 135 Yuandong Rd. Taoyuan 320 Taiwan

Electrochromic devices (ECDs) are materials that can undergo reversible changes in transmittance when exposed to different applied potentials. While many conjugated heterocyclic oligomers, such as oligothiophenes, have been developed for this purpose, there is no reported study on the use of discrete oligomeric furans as ECD materials. In this work, we introduce a furan trimer that can be utilized as a discrete electrochromic material, which transitions from light yellow to red and has a very high coloration efficiency of 1940 cm²/C at 507 nm. We propose that the reversible π-stack formation of the oligomer radical cations is behind this phenomenon, as evidenced by both experimental and computational results. The derivability of this oligomer from biomass and its facile synthesis make it an interesting alternative for other existing organic electrochromic materials. © 2023 American Chemical Society

关键词： electrochromism furan oligomer hydroxyalkylation−alkylation reaction solvatochromism π-stacks

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Electrospun Aligned PCL/Gelatin Scaffolds Mimicking the Skin ECM for Effective Antimicrobial Wound Dressings

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Advanced Fiber Materials 2023年第1期5卷 235-251页

作者： Erfan Rezvani Ghomi Rajamani Lakshminarayanan Vijila Chellappan Navin Kumar Verma Amutha Chinnappan Rasoul Esmaeely Neisiany Kottaiswamy Amuthavalli Zhi Sheng Poh Brandon Han Siang Wong Nileshkumar Dubey Roger Narayan Seeram Ramakrishna Department of Mechanical Engineering Center for Nanotechnology and SustainabilityNational University of SingaporeSingapore 117581Singapore Ocular Infections and Antimicrobials Research Group Singapore Eye Research InstituteThe Academia20 College RoadDiscovery TowerSingapore 169856Singapore Institute of Materials Research and Engineering(IMRE) Agency for Science Technology and Research(A*STAR)#08‑032 Fusionopolis WayInnovisSingapore 138634Singapore Lee Kong Chian School of Medicine Nanyang Technological University SingaporeClinical Sciences Building11 Mandalay RoadSingapore 308232Singapore Department of Pharmacy National University of Singapore18 Science Drive 4Singapore 117543Singapore Academic Clinical Program in Ophthalmology and Visual Sciences Academic Clinical Program Duke-NUS Medical SchoolSingapore 169857Singapore National Skin Centre 1 Mandalay RoadSingapore 308205Singapore Department of Materials and Polymer Engineering Faculty of EngineeringHakim Sabzevari UniversitySabzevar ***Iran Faculty of Dentistry National University of SingaporeSingapore 119085Singapore ORCHIDS:Oral Care Health Innovations and Designs Singapore National University of SingaporeSingaporeSingapore 119085Singapore Department of Biomedical Engineering University of North Carolina at Chapel HillChapel HillNC 27514USA

Bacterial infections and multidrug-resistant bacteria are major health burdens in wound *** antimicrobial agents,e.g.,ε-polylysine(ε-PL),provide a broad spectrum of antibacterial properties and support dermal cell ***,ε-PL was incorporated into polycaprolactone(PCL)/gelatin electrospun scaffolds collected at varying rotation ***,the samples were crosslinked using dopamine hydrochloride to provide highly proliferative dressings with broad antimicrobial *** morphological study showed that the electrospun wound dressings were smooth,continuous,and bead-free,with a mean diameter ranging from 267±7 to 331±8 nm for all random and aligned *** fiber alignment of the electrospun PCL/gelatin scaffolds improved their tensile strength and ***,nanofiber mats are highly hydro-philic,which is crucial for an efficient wound *** samples also demonstrated high antimicrobial properties against common wound bacterial strains,including methicillin-resistant Staphylococcus aureus(MRSA),Staphylococcus aureus(SA),Escherichia coli(EC),Acinetobacter baumannii(AB),and Pseudomonas aeruginosa(PA).Mammalian cell prolifera-tion and morphology assays involving primary human dermal fibroblasts(hDFs)and immortalized keratinocytes(HaCaT)showed excellent biocompatibility of the electrospun mats and remarkably aligned ***,aligned mats showed more cell migration than randomly oriented mats,which is desirable for more efficient wound ***,it can be concluded that aligned PCL/gelatin mats containingε-PL are promising for potential use in wound dressings.

关键词： Electrospinning Wound healing Fiber alignment Biomaterials Nanofiber dressing Bacterial infections

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Nanostructured Multicomponent Bioinks with Nanodiamond and Magnesium-Doped Nanohydroxyapatite for Enhanced Bone Tissue Engineering

SSRN

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SSRN 2025年

作者： Nicolae, Carmen-Valentina Jahani Kadousaraei, Masoumeh Yamada, Shuntaro Aydin, Mehmet Serhat Al-Sharabi, Niyaz Campodoni, Elisabetta Sandri, Monica Steinmüller-Nethl, Doris Syverud, Kristin Rashad, Ahmad Stancu, Izabela Cristina Mustafa, Kamal Advanced Polymer Materials Group University Politehnica of Bucharest 1-7 Gh. Polizu Street Bucharest011061 Romania Center of Translational Oral Research Department of Clinical Dentistry Faculty of Medicine University of Bergen Bergen Norway CNR-ISTEC Institute of Science and Technology for Ceramics National Research Council of Italy Faenza Italy DiaCoating GmbH Wattens Austria RISE PFI AS Trondheim Norway Bioengineering Graduate Program Aerospace and Mechanical Engineering University of Notre Dame Notre DameIN46556 United States

The development of bioinks for bone tissue engineering (BTE) requires a precise balance of printability, stability and bioactivity to ensure cell viability while supporting cell attachment, proliferation and osteogenic differentiation. Although numerous bioink formulations for BTE demonstrate good printability and bioactivity, they often lack the stability or osteogenic potential required to support long-term bone regeneration. To address these limitations, we developed multicomponent formulations for extrusion-based bioprinting by combining TEMPO-oxidized cellulose nanofibrils (TO-CNFs) with gelatin methacryloyl (GelMA) and sodium alginate (SA). The formulation was further loaded with nanodiamond particles (NDs), magnesium-doped nanohydroxyapatite (MgHA) or a combination of both to impart synergistic effects. This study investigates the individual and combined effects of NDs and MgHA on the printability, structural integrity, biocompatibility, and osteogenic performance of the bioink, hypothesizing that a dual nanoparticle system could provide superior multifunctionality. Rheological and printability tests confirmed that the incorporation of NDs improved the structural integrity and printing fidelity of the printed structures, with all formulations showing comparable mechanical properties. Seeded human gingival fibroblasts showed enhanced viability and spreading, and favorable metabolic activity and proliferation on ND-containing hydrogels. While the viability and elongation of bioprinted osteoblast-like cells in all four bioinks were comparable, MgHA-containing bioinks promoted osteogenic differentiation of osteoblasts, shown by increased Runx2 expression, ALP activity, and biomineralization. These findings suggest that the combined incorporation of NDs and MgHA within the TO-CNFs-GelMA-SA matrix provides a promising platform with robust printability and enhanced bioactivity, addressing the current trade-offs in the design of bioinks for comprehensive BTE. © 2025,

关键词： Bone

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Sharma et al. Reply:

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Physical Review Letters 2022年第21期128卷 219602-219602页

作者： Keshav Sharma Nathalia L. Costa Yoong Ahm Kim Hiroyuki Muramatsu Newton M. Barbosa Neto Luiz G. P. Martins Jing Kong Alexandre Rocha Paschoal Paulo T. Araujo Department of Physics and Astronomy University of Alabama Tuscaloosa 35487 Alabama USA Department of Physics Federal University of Ceara Fortaleza 60455-760 Ceara Brazil Department of Polymer Engineering School of Polymer Science and Engineering and Alan G. MacDiarmid Energy Research Institute Chonnam National University 77 Yongbong-ro Buk-gu Gwangju 61186 Republic of Korea Research Institute for Supra-Materials Shinshu University 4-17-1 Wakasato 380-8553 Nagano Japan Institute of Natural Sciences Graduate Program in Physics Federal University of Para Belem 66075-110 Brazil Department of Physics Massachusetts Institute of Technology Cambridge 02139 Massachusetts USA Department of Electrical Engineering and Computer Science Massachusetts Institute of Technology Cambridge 02139 Massachusetts USA

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Dynamic Covalent Bonds Enabled Carbon Fiber Reinforced polymers Recyclability and Material Circularity

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Angewandte Chemie 2024年第40期136卷

作者： Xiaotong Fan Jie Zheng Jayven Chee Chuan Yeo Sheng Wang Ke Li Joseph Kinyanjui Muiruri Nikos Hadjichristidis Zibiao Li Institute of Sustainability for Chemicals Energy and Environment (ISCE2) Agency for Science Technology and Research (A*STAR) 1 Pesek Road Jurong Island Singapore 627833 Republic of Singapore Institute of Materials Research and Engineering (IMRE) Agency for Science Technology and Research (A*STAR) 2 Fusionopolis Way Innovis #08-03 Singapore 138634 Republic of Singapore Polymer Synthesis Laboratory Chemistry Program KAUST Catalysis Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology (KAUST) Thuwal 23955 Saudi Arabia Department of Materials Science & Engineering National University of Singapore 9 Engineering Drive 1 Singapore 117575 Republic of Singapore

Due to their remarkable features of lightweight, high strength, stiffness, high-temperature resistance, and corrosion resistance, carbon fiber reinforced polymers (CFRPs) are extensively used in sports equipment, vehicles, aircraft, windmill blades, and other sectors. The urging need to develop a resource-saving and environmentally responsible society requires the recycling of CFRPs. Traditional CFRPs, on the other hand, are difficult to recycle due to the permanent covalent crosslinking of polymer matrices. The combination of covalent adaptable networks (CANs) with carbon fibers (CFs) marks a new development path for closed-loop recyclable CFRPs and polymer resins. In this review, we summarize the most recent developments of closed-loop recyclable CFRPs from the unique paradigm of dynamic crosslinking polymers, CANs. These sophisticated materials with diverse functions, oriented towards CFs recycling and resin sustainability, are further categorized into several active domains of dynamic covalent bonds, including ester bonds, imine bonds, disulfide bonds, boronic ester bonds, and acetal linkages, etc. Finally, the possible strategies for the future design of recyclable CFPRs by combining dynamic covalent chemistry innovation with materials interface science are proposed.

关键词： dynamic covalent bonds carbon fiber reinforced polymers recyclability materials circularity

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Effect of TPU hard segment content on TPU’s bead foaming behavior

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AIP Conference Proceedings 2020年第1期2205卷

作者： Emine Bursa Kucuk Bige Batı Mohammadreza Nofar 1Polymer Science and Technology Program Istanbul Technical University Maslak Istanbul 34469 Turkey 2Metallurgical & Materials Engineering Department Faculty of Chemical and Metallurgical Engineering Istanbul Technical University Maslak Istanbul 34469 Turkey

A lab-scale bead foaming reactor was used to investigate the foaming behavior of thermoplastic polyurethane (TPU) samples with different hard segment contents of around 39 %, 49 % and 57%. The saturation temperature, pressure, and time differently influenced the formation of hard segment crystals with different close-packed structures and sizes. Consequently, with the increase in hard segment crystallization during the saturation the heterogeneous cell nucleation was improved and the foam expansion was controlled by the stiffness of the TPU/CO2 mixture, solubility of CO2, and final shrinkage of the foamed samples. As the saturation temperature increased, the expansion ratio tended to increase with a tendency to shrink more due to the reduced crystallites content. This is while the cell density decreased due to the reduced hard segment crystallites generated during the saturation. Increase in pressure also improved the CO2 solubility and hence the expansion ratio was increased more significantly. The saturation time also influenced the amount and perfection degree of hard segment crystals. The interrelation between the crystallization behavior of the TPU bead foams and process conditions was reported using differential scanning calorimetry (DSC) and scanning electron microscope (SEM) analysis.

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Anharmonicity and Universal Response of Linear Carbon Chain Mechanical Properties under Hydrostatic Pressure

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Physical Review Letters 2020年第10期125卷 105501-105501页

作者： Keshav Sharma Nathalia L. Costa Yoong Ahm Kim Hiroyuki Muramatsu Newton M. Barbosa Neto Luiz G. P. Martins Jing Kong Alexandre Rocha Paschoal Paulo T. Araujo Department of Physics and Astronomy University of Alabama Tuscaloosa Alabama 35487 USA Department of Physics Federal University of Ceara 60455-760 Fortaleza Ceara Brazil Department of Polymer Engineering School of Polymer Science and Engineering and Alan G. MacDiarmid Energy Research Institute Chonnam National University 77 Yongbong-ro Buk-gu Gwangju 61186 Republic of Korea Research Institute for Supra-Materials Shinshu University 4-17-1 Wakasato Nagano Japan Institute of Natural Sciences Graduate Program in Physics Federal University of Para 66075-110 Belem PA Brazil Department of Physics Massachusetts Institute of Technology Cambridge Massachusetts 02139 USA Department of Electrical Engineering and Computer Science Massachusetts Institute of Technology Cambridge Massachusetts 02139 USA

Isolated linear carbon chains (LCCs) encapsulated by multiwalled carbon nanotubes are studied under hydrostatic pressure (P) via resonance Raman scattering. The LCCs’ spectroscopic signature C band around 1850 cm−1 softens linearly with increasing P. A simple anharmonic force-constant model not only describes such softening but also shows that the LCCs’ Young’s modulus (E), Grüneisen parameter (γ), and strain (ϵ) follow universal P−1 and P2 laws, respectively. In particular, γ also presents a unified behavior for all LCCs. To the best of our knowledge, these are the first results reported on such isolated systems and the first work to explore universal P-dependent responses for LCCs’ E, ϵ, and γ.

关键词： Anharmonic lattice dynamics Compressive strength Elasticity Mechanical & acoustical properties Pressure effects Stress 1-dimensional systems Lattice models in condensed matter Pressure techniques Raman spectroscopy

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Confinement and characterization of deep eutectic solvent based on choline chloride:alcohol into nanoporous silica for CO2 capture

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AIP Conference Proceedings 2019年第1期2111卷

作者： Zaitun Ghazali Mohd Ambar Yarmo Rizafizah Othaman 1Polymer Research Centre Faculty of Science and Technology Faculty of Science and Technology Universiti Kebangsaan Malaysia 43600 Bangi Selangor Malaysia 2Catalysis Research Group School of Chemical Sciences and Food Technology Faculty of Science and Technology Universiti Kebangsaan Malaysia 43600 Bangi Selangor Malaysia

Biodegradable nanocomposite adsorbents based on nanoporous silica (NS) and deep eutectic solvents (DESs) mixture of choline chloride:glycerol (ChCl:Gly) and choline chloride:ethylene glycol (ChCl:EG) were synthesized and the ability to adsorb carbon dioxide (CO2) has been studied. All DESs were prepared in mole ratio 1:2 and 10 w/w% were confined into nanoporous silica through sol gel method. The physicochemical properties of the prepared adsorbents have been characterized using Fourier transform infrared attenuated total reflectance (FTIR-ATR) and surface analyzer ASAP 2020. The presence of ChCl:Gly and ChCl:EG in the NS can be detected with the presence sp3 hybridized CH stretching and CH2 bending peaks. Specific surface areas of the NS were significantly reduced with confinement of DESs due to the transformation of micropores to mesopores. The ability of adsorbent to adsorb CO2 was evaluated using isothermal CO2 adsorption by Micromeritic ASAP 2020. ChCl:Gly/NS showed higher CO2 adsorption capacity compared to ChCl:EG/NS which are 20.1 mgCO2/gadsorbent and 18.8 mgCO2/gadsorbent, respectively.

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Mechanical properties of chemically modified Sansevieria trifasciata/natural rubber/high density polyethylene (STF/NR/HDPE) composites: Effect of silane coupling agent

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AIP Conference Proceedings 2018年第1期1940卷

作者： Nurzam Ezdiani Zakaria Azizah Baharum Ishak Ahmad 2School of Chemical Sciences and Food Technology Faculty of Science and Technology National University of Malaysia 43600 UKM Bangi Selangor Malaysia 3Food Processing and Packaging Program Food Science Technology Research Centre Malaysian Agricultural of Research and Development Institute P.O Box 12301 General Post Office 50774 Kuala Lumpur Malaysia 1Polymer Research Center Faculty of Science and Technology National University of Malaysia 43600 UKM Bangi Selangor Malaysia

The main objective of this research is to study the effects of chemical modification on the mechanical properties of treated Sansevieria trifasciata fiber/natural rubber/high density polyethylene (TSTF/NR/HDPE) composites. Processing of STF/NR/HDPE composites was done by using an internal mixer. The processing parameters used were 135°C for temperature and a mixing rotor speed of 55 rpm for 15 minutes. Filler loading was varied from 10% to 40% of STF and the fiber size used was 125 µm. The composite blends obtained then were pressed with a hot press machine to get test samples of 1 mm and 3 mm of thickness. Samples were evaluated via tensile tests, Izod impact test and scanning electron microscopy (SEM). Results showed that tensile strength and strain value decreased while tensile modulus increased when filler loading increased. Impact strength increased when filler loading increased and began to decrease after 10% of filler amount for treated composites. For untreated composites, impact strength began to decrease after 20% of filler loading. Chemical modification by using silane coupling agent has improved certain mechanical properties of the composites such as tensile strength, strain value and tensile modulus. Adding more amount of filler will also increase the viscosity and the stiffness of the materials.

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