Article
Multidisciplinary Sciences
Yingchun Xia, Ziyuan Song, Zhengzhong Tan, Tianrui Xue, Shiqi Wei, Lingyang Zhu, Yingfeng Yang, Hailin Fu, Yunjiang Jiang, Yao Lin, Yanbing Lu, Andrew L. Ferguson, Jianjun Cheng
Summary: Recent advances in accelerated polymerization of N-carboxyanhydrides (NCAs) have enriched the toolbox for preparing well-defined polypeptide materials. The use of crown ethers to catalyze NCA polymerization enables efficient preparation of functionalized polypeptides, while also guiding catalyst design.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Yanchao Wang, Maosheng Li, Shixue Wang, Youhua Tao, Xianhong Wang
Summary: SCA monomers derived from amino acids are more reactive than thiolactones for ultrafast and selective ROP, resulting in controlled molecular weight, low dispersities, and retained stereoregularity of the synthesized polythioesters.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Medicinal
Timothy P. Enright, Dominic L. Garcia, Gia Storti, Jason E. Heindl, Alexander Sidorenko
Summary: Infections caused by multidrug-resistant Gram-negative bacteria are a urgent global health threat and efforts are being made to develop new antibiotics and understand resistance mechanisms. Anti-Microbial Peptides (AMPs) are being explored as a novel drug design strategy due to their broad spectrum activity and efficacy against resistant organisms. However, naturally occurring AMPs have limitations, leading to the development of synthetic analogs with optimal selectivity. This study focuses on the development of chitosan-graft-polypeptide structures as novel antimicrobial agents, which showed activity against clinically significant pathogens and disrupted biofilm formation.
Article
Polymer Science
Dilhan Kandemir, Serter Luleburgaz, Ufuk Saim Gunay, Hakan Durmaz, Volkan Kumbaraci
Summary: This study introduces an organocatalyst-mediated method for the synthesis of poly(disulfide), which is rapid, robust, and practical. By screening various organocatalysts, the best catalyst with a low loading amount was identified to produce poly(disulfide) with varying molecular weights in just 1 minute. The optimum conditions for polymerization were determined using triphenylphosphine as the suitable catalyst. Moreover, successful synthesis of poly(disulfide) with molecular weights up to 85.6 kDa was achieved. The study also attempted a catalyst-free approach and found that polymer synthesis is possible under certain conditions, with increasing temperature leading to higher molecular weights.
Article
Biochemistry & Molecular Biology
Qiang Zhang, Yuanyuan Liu, Yucheng Fei, Jiguo Xie, Xiaofei Zhao, Zhiyuan Zhong, Chao Deng
Summary: The study presents a novel synthesis method for phenylboronic acid-functionalized copolypeptides based on an L-boronophenylalanine N-carboxyanhydride (BPA-NCA) monomer, and demonstrates their potential for co-encapsulation and responsive release of dual anticancer drugs. The synthesized copolypeptides show controlled compositions and can self-assemble into uniform micellar nanoparticles for drug delivery. The resulting nanoparticles exhibit enhanced anticancer effects and have potential applications in smart cancer nanomedicines.
Article
Polymer Science
Meiyao Wang, Lili Xu, Min Lin, Zhibo Li, Jing Sun
Summary: The block copolymer PEG-b-P(Lys-TPE) with reversible pH-responsive AIE characteristics was synthesized via imine bonds. The reversible detachment of TPE residues from polypeptides with pH variation in the presence of organic solvents led to reversible variation of fluorescence intensity. This work provides a convenient and universal strategy to efficiently construct AIEgens with reversible stimuli-responsive properties, serving as potential candidates for new generations of smart fluorescent nanomaterials.
Article
Multidisciplinary Sciences
Fei Han, Songyun Gu, Aleks Klimas, Ni Zhao, Yongxin Zhao, Shih-Chi Chen
Summary: A major challenge in nanotechnology is the fabrication of complex 3D structures with desired materials. This study presents a strategy using a library of materials to fabricate arbitrary 3D nanostructures. By using hydrogel templates and fine-tuning exposure strategies, high-resolution 2D and 3D structures are achieved. Fabricated nanodevices demonstrate their designed functionality and precision, offering further possibilities for nanodevice design.
Article
Chemistry, Multidisciplinary
Junliang Zhu, Yunjie He, Chenglong Ge, Wenting Si, Ziyuan Song, Lichen Yin
Summary: In this study, a rapid and efficient method for preparing polypeptide-based inorganic/organic nano-hybrids was reported. The accelerated ring-opening polymerization of N-carboxyanhydrides (NCAs) was achieved using amine-modified mesoporous silica nanoparticles (MSN-NH2) as nano-initiators in a dichloromethane/water biphasic system. The resulting nano-hybrids exhibited spherical morphology and uniform size distribution. Moreover, this strategy can be applied to various types of NCAs and inorganic nano-initiators. The research provides a convenient approach for the synthesis of inorganic/organic nano-hybrids and promotes their potential applications in the biomedical field.
CHINESE JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Nicholas J. Chan, Sarah Lentz, Paul A. Gurr, Shereen Tan, Thomas Scheibel, Greg G. Qiao
Summary: In this study, densely crosslinked polypeptide films with unusually high random coil content were successfully fabricated through continuous assembly polymerization. The method shows great potential for applications in drug delivery and tissue engineering.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Liyang Fu, Yanxue Che, Yanjun Gong, Hongwei Ji, Yifan Zhang, Ling Zang, Jincai Zhao, Yanke Che
Summary: We report a tunable 2D living self-assembly method for controlling the geometric shape variety and mechanical properties of uniform 2D platelets. The approach involves using n-alkyl alcohols to form a 2D network via hydrogen bonding, resulting in three effects: maintaining the same optical properties and thermal stability, generating alcohol-dependent 2D shape variety, and varying the mechanical properties through the interactions of different alcohol tail lengths.
CHEMISTRY OF MATERIALS
(2023)
Article
Polymer Science
Christopher B. Keller, Susan E. Walley, Curtis W. Jarand, Jibao He, Muhammad Ejaz, Daniel A. Savin, Scott M. Grayson
Summary: By grafting linear-bottlebrush amphiphilic copolymers onto the surface of silica nanoparticles, nanoparticle micelles with the ability to encapsulate and stabilize non-polar structures in aqueous media were successfully formed. These nanoparticles not only enhance oil encapsulation, but also provide an alternative dispersant system to address oil pollution in the environment.
Article
Chemistry, Multidisciplinary
Jiadong Tang, Maosheng Li, Xianhong Wang, Youhua Tao
Summary: We have achieved the one-pot production of sequence-controlled block copolymer from mixed monomers using a switchable catalyst. The method allows for chemoselective and efficient polymerization reactions, resulting in a high conversion rate of CO2.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Polymer Science
Rui Chen, Ying Wang, Linlin Zhu, Zhen Zhang
Summary: An ultrafast method for controlled synthesis of polysulfonamides through organocatalytic anionic ring-opening polymerization (ROP) in the melt has been established. Using N,N,N',N'',N''-pentamethyldiethylenetriamine (PMDETA) as catalyst, poly(2-methyl-N-tosylaziridine) with molecular weight over 100 kg/mol can be synthesized in less than 90 s. Various initiators can be applied to achieve molecular weight and end-group controlled polymers under open-flask conditions.
JOURNAL OF POLYMER SCIENCE
(2021)
Article
Polymer Science
Fang Yin, Pascale Laborie, Barbara Lonetti, Yannick Coppel, Nancy Lauth-de Viguerie, Jean-Daniel Marty, Stephane Gineste
Summary: Doubly thermo-and pH-responsive PNIPAM-b-PDEAEAM polymers were synthesized by RAFT polymerization. The properties of these polymers and corresponding homopolymers in solution depend on pH and the protonation degree of the diethylamino moiety. The behavior of the polymers is also influenced by the nature of the polymer chain ends. At pH 10, both PNIPAM and PDEAEAM blocks contribute to phase transition and form stable spherical nanoobjects. At pH 4, PNIPAM-b-PDEAEAM with longer PDEAEAM length exhibits a two-step thermoresponsive behavior and forms large aggregates with a positively charged shell.
Article
Biochemistry & Molecular Biology
Basma Mahi, Mario Gauthier, Nikos Hadjichristidis
Summary: This paper reports the synthesis and characterization of novel hybrid arborescent polypeptides based on poly(gamma-benzyl L-glutamate)-co-poly(gamma-tert-butyl L-glutamate)-g-polysarcosine, which has potential applications as drug carriers. The study demonstrates the successful synthesis of different functionalized polymers and the effectiveness of RGD decoration in preventing micelle aggregation.
Review
Pharmacology & Pharmacy
Yunjiang Jiang, Yingying Chen, Ziyuan Song, Zhengzhong Tan, Jianjun Cheng
Summary: AMPs and SMAMPs have attracted significant enthusiasm in the past thirty years due to their unique membrane-active antimicrobial mechanism and broad-spectrum antimicrobial activity. Despite challenges inherent to current design strategies slowing down the clinical translational development of AMPs and SMAMPs, these challenges have triggered efforts to redesign and repurpose AMPs.
ADVANCED DRUG DELIVERY REVIEWS
(2021)
Article
Multidisciplinary Sciences
Yingchun Xia, Ziyuan Song, Zhengzhong Tan, Tianrui Xue, Shiqi Wei, Lingyang Zhu, Yingfeng Yang, Hailin Fu, Yunjiang Jiang, Yao Lin, Yanbing Lu, Andrew L. Ferguson, Jianjun Cheng
Summary: Recent advances in accelerated polymerization of N-carboxyanhydrides (NCAs) have enriched the toolbox for preparing well-defined polypeptide materials. The use of crown ethers to catalyze NCA polymerization enables efficient preparation of functionalized polypeptides, while also guiding catalyst design.
NATURE COMMUNICATIONS
(2021)
Article
Engineering, Biomedical
Xu Wang, Ziyuan Song, Shiqi Wei, Guonan Ji, Xuetao Zheng, Zihuan Fu, Jianjun Cheng
Summary: Recent years have witnessed increasing interest in using ring-opening polymerization of NCAs to prepare synthetic polypeptides for various biomedical applications. Polypeptides, with their rich side-chain functionalities, diverse hydrophilicity/hydrophobicity profiles, and stable secondary structures, can assemble into well-organized nano-structures that offer unique advantages in drug delivery and controlled release. This review focuses on the design and use of polypeptide-based drug delivery systems derived from NCA chemistry, discussing their potential to change the landscape of next-generation therapeutics and diagnosis.
Article
Biochemistry & Molecular Biology
Tianjian Yang, Kyle Benson, Hailin Fu, Tianrui Xue, Ziyuan Song, Hanyi Duan, Hongwei Xia, Ankarao Kalluri, Jie He, Jianjun Cheng, Challa Kumar, Yao Lin
Summary: This study demonstrates the accelerated assembly of synthetic poly(L-glutamic acid) into amyloid-like fibrils catalyzed by cationic silica nanoparticle clusters as artificial nucleation factors. The charge-charge interactions and surface functionalities effectively facilitate the conformational change of macromolecular monomers and control the rates of nucleation for fibril growth. This approach inspires the development of novel materials through biomimetic supramolecular polymerizations.
Article
Materials Science, Ceramics
Shen J. Dillon, Yu-Feng Shen, Gregory S. Rohrer
Summary: By investigating the variation of grain boundary energy, the characteristics of grain boundaries in 8% yttria-stabilized zirconia were identified, with a focus on the impact of [100] orientation and [100] twist boundaries. The study results indicate that by manipulating the microstructure to increase the relative areas of [100] twist boundaries, the oxygen ion conductivity of the material can be enhanced.
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
(2022)
Article
Chemistry, Physical
Bhaskar Soman, Yoo Kyung Go, Chengtian Shen, Cecilia Leal, Christopher M. Evans
Summary: Vitrimers, dynamic polymer networks with topology conserving exchange reactions, have shown to have a long induction period for crystallization and exhibit evolving crystal morphologies over time due to the impact of bond exchange.
Article
Polymer Science
Hailin Fu, Ryan Baumgartner, Ziyuan Song, Chongyi Chen, Jianjun Cheng, Yao Lin
Summary: This article introduces a simple kinetic model to describe the cooperativity in covalent polymerizations. By treating the growing polymer chain as both a cooperative system and a primitive enzyme, and incorporating a Michaelis-Menten-like equation, the model accurately describes the binding of monomers to the polymer chain. The application of this model can help polymer chemists discover similar cooperative mechanisms in nonpolypeptide systems and utilize them to create covalent analogues of natural cooperative systems.
Article
Polymer Science
Fangping Yang, Zhiwei Liu, Wenting Si, Ziyuan Song, Lichen Yin, Haoyu Tang
Summary: Polysaccharide-polypeptide conjugates have shown great potential for biomedical applications by mimicking the structure and bioactivity of peptidoglycans or proteoglycans. However, the efficient and precise preparation of these conjugates remains challenging. In this study, we present a facile and efficient strategy to prepare conjugates with well-controlled polypeptide chain length from unmodified polysaccharides. The effect of polypeptide chain length on the surface antibacterial properties was also investigated.
Article
Physics, Applied
Omar Hussein, D. Keith Coffman, Khalid Hattar, Eric Lang, Shen J. Dillon, Fadi Abdeljawad
Summary: In this study, we demonstrate a morphological instability where a polycrystalline nanorod breaks up into isolated domains at grain boundaries. The destabilizing role of grain boundaries is shown, with the critical wavelength for the instability decreasing as the grain boundary energy increases. Phase field simulations predict the temporal evolution of interfacial profiles in quantitative agreement with experimental observations.
APPLIED PHYSICS LETTERS
(2022)
Article
Materials Science, Multidisciplinary
Shen J. Dillon, Yonghui Ma, Jia-hu Oyang, D. Keith Coffman, Omar Hussein, Khalid Hattar, Fadi Abdeljawad
Summary: In situ sintering experiments performed in a transmission electron microscope show that the densification rate can follow interface nucleation rate limited kinetics. This study conducts in situ sintering experiments on immiscible Al2O3-GdAlO3 interfaces, allowing for statistical analysis of sintering at a single interface type as a function of time and temperature. The data provide a measure of the activation energy for the nucleation process, which is asymptotic to 4.8 eV. The development of a new sintering model based on interface nucleation rate limited kinetics demonstrates its effectiveness in predicting various sintering data.
Article
Materials Science, Multidisciplinary
Shen J. Dillon, Eric Lang, Sarah C. Finkeldei, Jia-hu Ouyang, Khalid Hattar
Summary: The motion of grain boundary dislocations is responsible for grain boundary plasticity during processes like creep and stress relaxation. However, creep at low stress levels, known as non-Newtonian grain boundary creep, is not well understood. Previous models for nucleation rate limited creep have not been adequately developed. In this study, a model for nucleation rate limited kinetics is developed and shown to accurately describe existing creep data using realistic materials properties as inputs.
Article
Chemistry, Multidisciplinary
Chenglong Ge, Junliang Zhu, Huan Ye, Yuansong Wei, Yuheng Lei, Renxiang Zhou, Ziyuan Song, Lichen Yin
Summary: In this study, a series of protein-mimetic nano-switches were constructed to control their function based on the flexibility/rigidity of the polymeric chains. When in a dormant state, the polypeptide adopts a flexible, random-coiled conformation, leading to the turn-off of the optically functional molecule. Upon treatment with alkaline phosphatase, the nano-switches are activated due to the coil-to-helix and flexible-to-rigid transition of the polypeptide linker, enabling selective fluorescence imaging or photodynamic therapy in response to ALP overproduced by tumor cells.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Wanying Wang, Hailin Fu, Yao Lin, Jianjun Cheng, Ziyuan Song
Summary: In this paper, we discussed the mechanism and applications of cooperative covalent polymerization (CCP), which can accelerate the polymerization reaction and efficiently synthesize high-molecular-weight polypeptide materials. By studying the initiating systems and kinetic models of CCP, it was found that the secondary structure and molecular interactions played a crucial role in the polymerization rate. The fast kinetics of CCP also minimized side reactions and allowed the synthesis of polypeptides in the presence of an aqueous phase.
ACCOUNTS OF MATERIALS RESEARCH
(2023)
Article
Polymer Science
Qinyuan Li, Yingjia Lan, Wanying Wang, Guonan Ji, Xiaohong Li, Ziyuan Song
Summary: This study reports a method to control the polymerization behavior using a cosolvent system, which alters the polymerization kinetics curve and increases monomer solubility by mixing with chloroform, enabling fast and controlled preparation of polypeptides.
Article
Materials Science, Biomaterials
Ruizhong Xue, Xu Zhang, Yuansong Wei, Ziyin Zhao, Hao Liu, Fangping Yang, Lichen Yin, Ziyuan Song, Shifang Luan, Haoyu Tang
Summary: The study reports an anionic polypeptide coating with various excellent properties, including antibacterial, antifouling, and biocompatibility. The coating, prepared through ring-opening polymerization and subsequent reaction, showed superior antibacterial activity, and in vivo studies demonstrated its good anti-infection and tissue compatibility.
BIOMATERIALS SCIENCE
(2021)
