Article
Chemistry, Multidisciplinary
Jan Pille, Antonio Aloi, Duc H. T. Le, Ilia Vialshin, Nathalie van de Laar, Kirsten Kevenaar, Maarten Merkx, Ilja K. Voets, Jan C. M. van Hest
Summary: This study introduces a novel pathway-dependent assembly method based on stimulus-responsive polymers, which can form monodisperse and stable polymeric particles under specific heating conditions. This method shows high efficiency in encapsulating cargo, such as fluorescent proteins and bioluminescent enzymes, and maintaining their function within cells.
Article
Polymer Science
Haohui Huo, Jie Liu, Senthil Kannan, Long Chen, Yimin Zhao, Lei Zhang, Gang Chang, Qilu Zhang, Feng Liu
Summary: This study presents the first example of protein-like multicompartment nanoparticles formed via self-assembly of a specifically designed 21-arm star polymer, PEG(PAA-b-PS)(20). The morphology of the MCNs is determined by the volume ratio of PS to PAA, and unique string structures composed of one-dimensional alignment of single-star polymers were observed for the first time. A new mechanism for the assembly of star polymers was proposed based on investigations under different conditions, suggesting potential applications in drug delivery and catalysis.
Article
Polymer Science
Jordan T. Lovegrove, Ben A. Humphreys, Chin Ken Wong, Liliana de Campo, Anna Wang, Christopher J. Garvey, Martina H. Stenzel
Summary: This article investigates a synthetic pathway to produce biologically compatible, crosslinked, multicompartment worms (MCWs) in aqueous solution by incorporating thermoresponsive poly-N-isopropylacrylamide (PNIPAM) to direct assembly above the lower critical solution temperature (LCST). The self-assembly process and mechanism of MCWs starting from primary micelles were observed and controlled by adjusting the temperature.
Article
Polymer Science
Michele Dai, Evangelos Georgilis, Guillaume Goudounet, Bertrand Garbay, Jan Pille, Jan C. M. van Hest, Xavier Schultze, Elisabeth Garanger, Sebastien Lecommandoux
Summary: This study reports the design and study of an ELP diblock library based on ELP-[M1V3-i]-[I-j], which showed a thermal phase transition with three distinct regimes by selectively oxidizing methionines of ELP-[M1V3-i] within the different diblocks structures.
Article
Materials Science, Multidisciplinary
Dan Zhao, Rui Liu, Cheng Luo, Yang Guo, Chengyi Hou, Qinghong Zhang, Yaogang Li, Wei Jia, Hongzhi Wang
Summary: The study focuses on the in-situ assembly of carbon nanotubes (CNTs) using macroscopic dielectrophoresis, overcoming the limitation of small size in traditional manipulation methods. Through optimizing voltage and frequency, ordered CNTs chains can be obtained under the action of alternating current dielectrophoresis, which can restore immediately upon powering up after being damaged. Different conductive patterns on non-woven fabric can be achieved by controlling the position of the electrodes in a wet environment.
ADVANCED FIBER MATERIALS
(2021)
Article
Polymer Science
Zhengwei Zhou, Daihong Wan, Junwei Zhou, Yixin Zhang, Rong Wang
Summary: In this work, the self-assembly behavior of surfactin-like polymer in selective solvents was studied using dissipative particle dynamics. Different structures such as vesicles, disk-like micelles, worm-like micelles, sphere-like micelles, and ring-like micelles were obtained by changing interaction parameters, the size of the hydrophilic ring, the length of the hydrophobic tail chain, and the concentration. The formation paths of vesicles and ring-like micelles were explored, and the mechanism of sphere-like micelle formation at lower concentration was explained. The study provides insights into the self-assembly behavior of surfactin-like polymers and has implications for their practical application.
POLYMER INTERNATIONAL
(2023)
Review
Chemistry, Multidisciplinary
Hiroaki Kitagishi, Koji Kano
Summary: Myoglobin (Mb) is an optimal system for capturing molecular oxygen in aqueous solution, but stable O-2 adducts are challenging to obtain due to immediate autoxidation by water molecules. HemoCD1, a supramolecule, satisfies the challenging requirements for an artificial O-2 receptor and is capable of function in aqueous solution. This research has expanded to include synthesizing analogues, modeling enzymatic reactions, developing artificial oxygen carriers, and selective binding/removal of toxic small molecules in living organisms.
CHEMICAL COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Xingyun Li, Sai Zhang, Yuan Chen, Shanshan Wang, Qingchi Xu, Jun Xu
Summary: In this work, a novel gold nanocapsule with an anisotropic ellipsoidal shape and cavity structure was successfully prepared by self-assembly of ultrathin Au nanowires. The assembly mechanism was studied by tuning the assembly conditions, and the nanocapsules showed great drug loading ability and pH-responsive drug release behavior.
Article
Materials Science, Ceramics
James E. John, Shizhi Qian, Dipankar Ghosh
Summary: The role of high-frequency alternating current (AC) electric field in the assembly of alumina particles in aqueous media was investigated. Field-particle interactions were in situ investigated for coarse and fine powder particles in very dilute suspensions. For both coarse and fine particles, AC field-induced assembly led to the formation of chains of particles within a minute, which were aligned in the field direction. However, a much finer network of particle chains evolved in fine particle suspensions. Threshold field strength for chain formation was also lower for fine particles (28 V/mm) than for coarse particles (50 V/mm), suggesting stronger interactions for finer particles. Chain length increased with both field strength and field duration. Chain formation was attributed to mutual dielectrophoretic (DEP) interaction forces. Increase in DEP forces with field strength resulted in enhanced interactions. For finer particles, decreasing interparticle distance might have favored stronger interactions. Suspension microstructure was disrupted as soon as the field was removed. However, higher field duration was associated with an improved pattern stability and retention following the field removal. Finally, particle motion was studied in deliberately applied spatially nonuniform AC field, which revealed different mechanisms of chain formation for coarse (negative-DEP) and fine (positive-DEP) particles.
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
(2022)
Article
Polymer Science
K. J. Winchell, Patrick Y. Yee, Yolanda L. Li, Alexander F. Simafranca, Julia Chang, Christian Beren, Xinyu Liu, Diego Garcia Vidales, Robert J. Thompson, Charlene Z. Salamat, Quynh M. Duong, Robert S. Jordan, Benjamin J. Schwartz, William M. Gelbart, Yves Rubin, Sarah H. Tolbert
Summary: Semiconducting polymers are important materials for (opto)electronic applications, but their disorder and poor conductivities limit their performance. This study presents a method to straighten polymer chains using amphiphilic conjugated polyelectrolytes (CPEs) that self-assemble into worm-like micelles. By synthesizing and characterizing a micelle-forming polymer called PCT, it is found that the lack of steric hindrance between its subunits leads to significant chain straightening and the formation of rod-like micelles. This work expands the availability of micelle-forming semiconducting polymers and suggests possibilities for obtaining homogeneous nanostructured polymer assemblies.
Article
Chemistry, Physical
Aida Jover, Francisco Fraga, Francisco Meijide, Jose Vazquez Tato, Jacopo Cautela, Alessandra Del Giudice, Maria Chiara di Gregorio
Summary: Sodium deoxycholate exhibits various self-assembled structures in water, with novel phases and reversible transitions observed under conditions suitable for physiological working environment. These findings enhance the understanding of its diversity and help clarify its role in vivo.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2021)
Article
Multidisciplinary Sciences
Thais C. Neves-Martins, Nathane C. Mebus-Antunes, Carlos H. G. Neto, Glauce M. Barbosa, Fabio C. L. Almeida, Icaro P. Caruso, Andrea T. Da Poian
Summary: The researchers designed a mutant of the dengue virus capsid protein (DENVC) by replacing a positively charged spot with a cysteine residue, resulting in the self-assembly of capsid-like particles (CLP) in solution without nucleic acids.
Article
Chemistry, Physical
Chuheng Cao, Keqin Zhou, Wencheng Du, Cheng Chao Li, Minghui Ye, Yufei Zhang, Yongchao Tang, Xiaoqing Liu
Summary: In this study, a soft solid-like viscoelastic Zn powder composite (ss-ZnP) anode based on a rheological oligomer (E-44) gluing strategy is proposed. The ss-ZnP anode exhibits enhanced ion/electron transport and alleviated volume effect, leading to excellent electrochemical performance in Zn-ion batteries. Furthermore, the excellent malleability of ss-ZnP greatly facilitates the assembly of various types of batteries.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Sugiarto, Jun Shinogi, Masahiro Sadakane
Summary: Through 1H NMR spectroscopy analysis, we identified three distinct Cp*Ir-containing tungsten oxide clusters formed in aqueous mixtures of [(Cp*IrCl)2(mu-Cl)2] and Na2WO4 with varying molar ratios. These species were isolated as Na4[(Cp*Ir)2(mu-OH)3]2[(Cp*Ir)2H2W8O30], [(Cp*Ir)2(mu-OH)3]2[(Cp*Ir)2{Cp*Ir(OH2)}2H2W8O30], and [(Cp*Ir)2{Cp*Ir(OH2)}2{Cp*Ir(OH2)2}2H2W8O30](NO3)2. The results indicate that the octatungstate [H2W8O30]10- anion is the main polyoxotungstate species in the presence of {Cp*Ir}2+ cations, which can bind up to six {Cp*Ir}2+ cations on its surfaces. Moreover, the coordination environment of {Cp*Ir}2+ can be altered by coordinating with pyridine.
INORGANIC CHEMISTRY
(2023)
Review
Biochemistry & Molecular Biology
Qian Han, Fei Tao, Peng Yang
Summary: Protein-based biomaterials are of great interest due to their unique structural and functional properties. A recent development in designing such materials is the regulation of protein structural transformation to ordered aggregation, known as amyloid assembly. This process creates fibril-based nanostructures that can form films at interfaces, with excellent adhesion to substrates. This review highlights the research progress and applications of amyloid-like assembly for film formation, serving as a guide for the utilization of protein-based biomaterials.
MACROMOLECULAR BIOSCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Jianhua Lu, Zhun Xu, Hailin Fu, Yao Lin, Huan Wang, Hua Lu
Summary: The protein-mediated, aggregation-induced polymerization of amphiphilic LPA-derived monomers at room temperature enables low concentration PDS conjugation and enhances protein stability and resistance to enzymatic activity and freeze-thaw treatments. It also allows rapid purification of Cys-bearing proteins and opens up new possibilities for protein delivery, reversible protein engineering, enzyme preservation, and recycling.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Wenhao Dong, Zhimao Yang, Jie He, Chuncai Kong, Zhihong Nie
Summary: This article describes the vesicular self-assembly of shaped nanoparticles, such as gold nanocubes grafted with amphiphilic block copolymers, in selective solvents. The nanocubes assembled within the vesicular membranes exhibit two distinctive packing modes, namely square-like and hexagonal packing, depending on the relative dimensions of the copolymer ligands and nanocubes. The corresponding optical properties of the plasmonic nanovesicles can be tuned by varying the length of the grafted copolymers and the size of the nanocubes. This work provides guidance for the fabrication of functional plasmonic vesicles for applications in catalysis, nanomedicines, and optical devices.
Article
Chemistry, Multidisciplinary
Hanyi Duan, Zhenyang Jia, Maham Liaqat, Matthew D. Mellor, Haiyan Tan, Mu-Ping Nieh, Yao Lin, Stephan Link, Christy F. Landes, Jie He
Summary: Control of interparticle interactions by anisotropic ligand grafting on NP building blocks. Ligand deficiency exchange strategy achieved site-specific polymer grafting of AuNRs. Dumbbell-like AuNRs with controllable surface coverage can be synthesized through surface dewetting and exhibit great colloidal stability.
Article
Biochemistry & Molecular Biology
Honglin Zhu, Sunni Chen, Hanyi Duan, Jie He, Yangchao Luo
Summary: Chitosan (CS)/carboxymethyl cellulose (CMC) porous hydrogels crosslinked by epichlorohydrin and with polyethylene glycol (PEG) as a pore-forming agent were synthesized for removal of anionic (Congo red, CR) and cationic (methylene blue, MB) dyes from aqueous solutions. The addition of PEG significantly increased the adsorption of CR and MB, with optimal performance observed for hydrogels prepared with 2% CS and 2% CMC (CS2/CMC2). The adsorption processes followed pseudosecond-order and pseudo-first-order kinetics models for CR and MB, respectively. Freundlich and Langmuir models were suitable for describing the adsorption isotherms of CR and MB, respectively. The thermodynamic study confirmed that the adsorption of CR and MB by the hydrogels was spontaneous, with CR adsorption being endothermic and MB adsorption being exothermic.
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
(2023)
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
Nanoscience & Nanotechnology
Maham Liaqat, Rumasha Nipuni Thiruwana Kankanamage, Hanyi Duan, Ryuichi Shimogawa, Jiyu Sun, Monia Nielsen, Ehab Shaaban, Yuanyuan Zhu, Puxian Gao, James F. Rusling, Anatoly I. Frenkel, Jie He
Summary: This paper describes a strategy to catalyze in situ C-H oxidation by combining cobalt (Co) single-atom catalysts (SACs) and horseradish peroxidase (HRP). The Co SACs were synthesized using a Co phthalocyanine complex and were found to be strongly correlated to their reactivity. Increasing the calcination temperature improved catalytic activity, with the Co SACs obtained at 800°C showing superior activity in producing H2O2. The in situ production of H2O2 was further coupled with HRP for selective C-H bond oxidation.
ACS APPLIED MATERIALS & INTERFACES
(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
Chemistry, Multidisciplinary
Qiang Luo, Hanyi Duan, Michael C. McLaughlin, Kecheng Wei, Joseph Tapia, Joseph A. Adewuyi, Seth Shuster, Maham Liaqat, Steven Suib, Gael Ung, Peng Bai, Shouheng Sun, Jie He
Summary: We used polymer N-heterocyclic carbenes (NHCs) to control the microenvironment surrounding metal nanocatalysts, enhancing their catalytic performance in CO2 electroreduction. Three polymer NHC ligands were designed with different hydrophobicity: hydrophilic poly(ethylene oxide) (PEO-NHC), hydrophobic polystyrene (PS-NHC), and amphiphilic block copolymer (PEO-b-PS-NHC). The introduction of hydrophobic PS segments led to a twofold increase in the partial current density for CO formation. The hydrophobic polymers altered the hydrogen bonding structures of water, improving CO2 diffusion and subsequent reduction.
Review
Chemistry, Multidisciplinary
Neeraj Kumar, Jie He, James F. F. Rusling
Summary: Cytochrome P450s (Cyt P450s) and peroxidases are enzymes with iron heme cofactors used as biocatalysts in chemical syntheses. By incorporating them into thin films on electrodes, these enzymes can accept electrons and catalyze organic transformations in a cost-effective way. This paper reviews the electrochemical reactions catalyzed by Cyt P450s and peroxidases, including C-H activation, S-oxidation, epoxidation, N-hydroxylation, and oxidative N- and O-dealkylation. Design aspects of these bioelectrocatalytic reactions are discussed, as well as challenges and future perspectives of these systems.
CHEMICAL SOCIETY REVIEWS
(2023)
Article
Polymer Science
Lijun Wang, Qiang Zhou, Yanfang Chen, Xiaoke Yang, Yangyang Zhang, Hanyi Duan, Haixiang Song, Yanfei Wang, Yongjun Zheng
Summary: The self-assembly of amphiphilic graft copolymers with mechanophores is used to fabricate nanosized aggregates that respond to mechanical stimuli. The presence of dimethylformamide (DMF) in the assembly solutions plays a crucial role in promoting the activation of the mechanophores. The DMF content also influences the mechanochemical reaction characteristics and morphology of the assemblies.
Article
Chemistry, Multidisciplinary
Zichao Wei, Chung-Hao Liu, Qiang Luo, Srinivas Thanneeru, Alfredo M. Angeles-Boza, Mu-Ping Nieh, Jie He
Summary: We investigated the hydrophobicity-enhanced reactivity of Cu2+ ions as an ester hydrolase. By varying the synthetic sequence of amphiphilic block copolymers, we controlled the location of the Cu2+ binding motif in polymer micelles. The hydrophobicity of Cu2+ sites significantly impacted their catalytic efficiency, with as much as 60 times more activity. Our findings highlight the importance of hydrophobic microenvironments in the design of bioinspired catalysts.
MATERIALS CHEMISTRY FRONTIERS
(2023)