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
Chemistry, Multidisciplinary
Vusala Ibrahimova, Hang Zhao, Emmanuel Ibarboure, Elisabeth Garanger, Sebastien Lecommandoux
Summary: A new class of hybrid lipoprotein mimics was designed using chemical post-modification reactions, allowing the formation of biomimetic vesicles with controlled permeability, correlated to the temperature-responsiveness of ELPs.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Biochemistry & Molecular Biology
Chloe Grazon, Elisabeth Garanger, Pierre Lalanne, Emmanuel Ibarboure, James E. Galagan, Mark W. Grinstaff, Sebastien Lecommandoux
Summary: Polymeric micelles based on natural diblocks, such as elastin-like polypeptide (ELP) and oligonucleotide (ON), have advantageous properties in terms of molecular recognition, biocompatibility, and biodegradability. This study reports a straightforward synthesis of ON-b-ELP diblock bioconjugates through copper-catalyzed azide-alkyne cycloaddition. The resulting micelles self-assemble above their critical micelle temperature (CMT) to form stable structures, and they retain their stability and temperature sensitivity when binding with proteins.
Article
Chemistry, Multidisciplinary
Jolinde van Strien, Oscar Escalona-Rayo, Wim Jiskoot, Bram Slutter, Alexander Kros
Summary: ELP-based nanomaterials, particularly micelles assembled from amphiphilic ELP diblock copolymers, show great potential as drug delivery systems due to their biodegradability and the ability to control particle design. The cargo can be shielded inside the micelle core or reside in the corona through site-specific attachment to the hydrophobic or hydrophilic block of the ELP. Various types of cargo, including protein, peptide, and small molecule drugs, can be loaded onto or entrapped inside the micelles.
JOURNAL OF CONTROLLED RELEASE
(2023)
Review
Materials Science, Multidisciplinary
Lubinda Mbundi, Miguel Gonzalez-Perez, Fernando Gonzalez-Perez, Diana Juanes-Gusano, Jose Carlos Rodriguez-Cabello
Summary: Porous biomaterials are crucial for biomedical applications, enabling nutrient diffusion, waste removal, and the development of complex structures. Tailoring the physicochemical characteristics of biomaterials is necessary for optimal customized applications. Elastin-like polypeptides play an increasing role in developing porous biomaterials for various tissue applications.
FRONTIERS IN MATERIALS
(2021)
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
Polymer Science
Wen-Wen Song, Zhi-Gang Qian, Hao Liu, Hai-Feng Chen, David L. Kaplan, Xiao-Xia Xia
Summary: This study presents a genetic fusion strategy to regulate the dual thermal transitions of the C-terminal domain of spider major ampullate spidroin 1, enabling the construction of hydrogels with potential applications in cell preservation and delivery.
Article
Nanoscience & Nanotechnology
Robbert J. de Haas, Ketan A. Ganar, Siddharth Deshpande, Renko de Vries
Summary: Biomolecular condensates are macromolecular complexes formed by liquid-liquid phase separation that regulate key biological functions. Designing stimuli-responsive synthetic condensates is crucial for engineering compartmentalized synthetic cells that can mimic spatiotemporal control over biochemical reactions.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Biochemical Research Methods
Daniela S. Strugach, Dagan Hadar, Miriam Amiram
Summary: This study found a photoswitch with suitable light-responsive properties that can be incorporated into proteins, enabling light-responsive behavior. The method allows for multisite incorporation of the photoswitch at the polypeptide level, providing a general approach for designing proteins and polymers with robust light-responsive behavior.
ACS SYNTHETIC BIOLOGY
(2023)
Article
Polymer Science
Yani Zhao, Kurt Kremer
Summary: ELPs are proline-rich stimulus-responsive polymers with applications in drug delivery and green chemistry. Proline isomerization can regulate the conformational behavior of ELPs in aqueous ethanol mixtures without changing the solvation free energy. It affects the affinity of the peptide to both solvent and cosolvent molecules.
MACROMOLECULAR RAPID COMMUNICATIONS
(2022)
Article
Biotechnology & Applied Microbiology
Zihang Su, ChulOong Kim, Julie N. Renner
Summary: In this study, short elastin-like peptides (ELPs) with varying hydrophobicity and sequence length were designed for gold attachment, and a quantitative model was developed to describe the relationship between ELP effective surface coverage and mean hydrophobicity and mass loading. The results showed that precise control of surface properties can be achieved by tuning the ELP sequence, which is useful for designing surface-bound ELP sequences with desired effective surface coverage for electrochemical and biomaterial applications.
BIOCHEMICAL ENGINEERING JOURNAL
(2021)
Review
Engineering, Biomedical
Irene C. Jenkins, Joshua J. Milligan, Ashutosh Chilkoti
Summary: Elastin-like polypeptides (ELPs) are thermally responsive biopolymers that can be harnessed to produce stimuli-responsive biomaterials, such as nanoparticles or injectable drug delivery depots. ELPs can be loaded with drugs to create controlled, intelligent drug delivery systems. ELPs are biodegradable, nonimmunogenic, and tolerant of therapeutic additives.
ADVANCED HEALTHCARE MATERIALS
(2021)
Article
Biochemistry & Molecular Biology
Jingjing Ji, Md Shahadat Hossain, Emily N. Krueger, Zhe Zhang, Shivangi Nangia, Britnie Carpentier, Mae Martel, Shikha Nangia, Davoud Mozhdehi
Summary: Lipidated proteins are hybrid biomaterials that combine the functional capabilities of proteins with precisely engineered nano-biomaterials. The thermoresponsive behavior of fatty-acid-modified elastin-like polypeptides (FAMEs) and the structural changes induced by temperature and molecular syntax were investigated using computational nanoscopy, spectroscopy, scattering, and microscopy. These findings provide insights into the biophysical consequences of lipidation in biology and facilitate the rational design of biomaterials and therapeutics.
Article
Engineering, Environmental
Zhongwei Guo, Yuanyuan Xu, Lina Dong, Malav S. Desai, Jingjing Xia, Mujiao Liang, Seung-Wuk Lee, Shengli Mi, Wei Sun
Summary: In this study, we designed and synthesized genetically encoded materials called elastin-like polypeptides (ELPs) that can undergo temperature-induced phase transition and photo-crosslinking due to modification with methacrylate groups. The degree of methacrylate functionalization can be controlled by adjusting the reactant ratio. By combining hydrogel fabrication strategy, the methacrylated ELPs (ELP-MA) can be engineered into different physical forms such as coacervates and hydrogels, functioning as light transmittance regulators and elastic adhesives. The physical properties of the hydrogels can be controlled by the degree of methacrylation and ELP-MA concentration. The resulting ELP-MA hydrogels showed good biocompatibility when implanted subcutaneously in mice.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Polymer Science
Tingting Zhang, Frederic Peruch, Anne-Laure Wirotius, Emmanuel Ibarboure, Frederic Rosu, Christophe Schatz, Bertrand Garbay
Summary: New biomaterials were developed by combining biocompatible blocks of polyisoprene and elastin-like polypeptide, which self-assemble into nanoparticles and can be used as drug delivery systems for various hydrophobic drugs.
Article
Chemistry, Multidisciplinary
Benjamin P. Allen, Zoe M. Wright, Hailey F. Taylor, Thomas J. Oweida, Sabila Kader-Pinky, Emily F. Patteson, Kara M. Bucci, Caleb A. Cox, Abishec Sundar Senthilvel, Yaroslava G. Yingling, Abigail S. Knight
Summary: This study presents a systematic investigation of the structure-assembly relationships of peptide-polymer amphiphiles (PPAs). The study reveals that the molecular weight and hydrophilicity of the oligomer control the morphology of the PPAs, while the dispersity and charge density of the peptide affect the particle size. These findings provide important benchmarks for the rational design of PPAs with enhanced biomimetic functionality.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Akhlak U. Mahmood, Yaroslava G. Yingling
Summary: Magnetic nanoparticles (MNPs) can self-assemble into ordered structures with unique geometries. A new atomistic molecular dynamics simulation method is proposed to study the dynamics, self-assembly, structure, and properties of MNPs under different core sizes and shapes, ligand chemistry, solvent properties, and external fields. The simulation of oleic acid ligand-functionalized magnetite (Fe3O4) nanoparticles shows that electrostatic interactions favor the formation of chains over rings, ligands promote cluster growth, and solvents reduce rotational diffusion. The parallelized algorithm can be used as a plugin for LAMMPS to gain insights into the physics and chemistry of magnetic assembly processes.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Biophysics
Jessica A. Nash, Matthew D. Manning, Alexey V. Gulyuk, Aleksey E. Kuznetsov, Yaroslava G. Yingling
Summary: RNA-based therapeutics have great potential in treating various diseases. This study used simulations to investigate the ability of cationic ligand functionalized gold nanoparticles to bend dsRNA and designed nanoparticles with controlled internal binding to RNA's major groove. The findings have important implications in packaging nucleic acids for nanotechnology and gene delivery.
Article
Chemistry, Physical
Sabila K. Pinky, Albert L. Kwansa, Buang Zhang, Adrienne D. Stiff-Roberts, Yaroslava G. Yingling
Summary: The morphology of conjugated polymer thin films is influenced by the emulsion characteristics, but the understanding of how these characteristics control the film properties and device performance is still unclear. In this study, molecular dynamics simulations were conducted on emulsions containing polyfluorene (PFO) polymer and various solvents to investigate the relationship between emulsion properties and the morphology of deposited PFO thin films. The results showed that a primary solvent with low solubility-in-water and high non-bonded interaction energy ratio among the solvent, polymer, and water produced smoother and denser films.
Article
Materials Science, Biomaterials
Atrouli Chatterjee, Preeta Pratakshya, Albert L. Kwansa, Nikhil Kaimal, Andrew H. Cannon, Barbara Sartori, Benedetta Marmiroli, Helen Orins, Zhijing Feng, Samantha Drake, Justin Couvrette, LeAnn Le, Sigrid Bernstorff, Yaroslava G. Yingling, Alon A. Gorodetsky
Summary: By combining experimental and computational methods, we systematically mapped the three-dimensional refractive index distributions of model self-assembled reflectin-based structures, which can improve understanding of squid skin cell functionality and enhance characterization of protein-based optical materials.
ACS BIOMATERIALS SCIENCE & ENGINEERING
(2023)
Article
Nanoscience & Nanotechnology
Buang Zhang, Sabila K. Pinky, Albert L. Kwansa, Spencer Ferguson, Yaroslava G. Yingling, Adrienne D. Stiff-Roberts
Summary: Thin films of polyfluorene (PFO) were successfully deposited using the emulsion based resonant infrared, matrix-assisted pulsed laser evaporation (RIR-MAPLE) method. It was found that the selection of surfactant can increase the crystalline-fi phase content and improve the color purity of light emission. Comparison of blue light-emitting diodes (LEDs) with different surfactants showed the significant impact of surfactant on device performance.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Akhlak U. Mahmood, Mehedi H. Rizvi, Joseph B. Tracy, Yaroslava G. Yingling
Summary: Inorganic colloidal nanoparticle (NP) properties can be controlled by stripping stabilizing ligands using a poor solvent. This study investigates the stripping process of oleylamine ligands from magnetite (Fe3O4) NPs in different ethanol/hexane mixtures. The results reveal the complex interactions between ethanol and system components, and suggest the existence of a threshold concentration of ethanol for effective ligand stripping. The study provides insights into the ligand-solvent interactions and offers a computational approach for studying ligand stripping from colloidal NPs.
Article
Polymer Science
Albert L. L. Kwansa, Rakhee C. C. Pani, Joseph A. A. DeLoach, Arianna Tieppo, Eric J. J. Moskala, Steven T. T. Perri, Yaroslava G. G. Yingling
Summary: Plasticizers improve the flexibility and durability of polymer materials by reducing glass transition and cold flex temperatures. However, the migration and exudation of plasticizers from polymer materials have hindered the development of efficient and safe plasticizers. This study used molecular dynamics simulations validated by experiment to investigate the molecular mechanism of exudation of different plasticizers from PVC, and found that plasticizer-PVC compatibility was the main determinant of exudation.
News Item
Oncology
Kelsey P. Kubelick, Felipe Garcia Quiroz
Summary: A recent study has revealed the connection between PD-L1 upregulation on cancer cells and IRF1-KAT8 transactivation hubs at PD-L1 loci. Targeting these hubs therapeutically could enhance anti-tumor immunity.
Article
Chemistry, Physical
Juseok Choi, Albert L. Kwansa, Yaroslava G. Yingling, Seong H. Kim
Summary: Vibrational sum frequency generation (SFG) spectroscopy is commonly used to analyze the structural information of molecular functional groups at two-dimensional interfaces in gas or liquid mediums. However, interpreting the measured intensity in terms of molecular orientation with respect to laboratory coordinates is challenging. This study utilized density functional theory to calculate the polarizability and dipole derivative tensors of different molecules, allowing for the theoretical calculation of their SFG intensities in relation to the tilt angle of the CH3 group with respect to the surface normal direction. The findings suggest that the vibrational coupling among neighboring functional groups is significant and should not be ignored in SFG experiments.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Biochemistry & Molecular Biology
Preeti Verma, Albert L. Kwansa, Ruoya Ho, Yaroslava G. Yingling, Jochen Zimmer
Summary: Cellulose, a major component of plant cell walls, is synthesized by cellulose synthase through translocation. In this study, cryogenic electron microscopy structures of the substrate and product bound to cellulose synthase isoform-8 from aspen were presented. UDP-glucose binds to a catalytic pocket adjacent to a transmembrane channel, and the glucosyl unit of the substrate is coordinated by conserved residues and amphipathic interface helices. Mutagenesis of a conserved gating loop revealed its critical role in catalytic activity. Molecular dynamics simulations showed prolonged interactions between the gating loop and the substrate, facilitating proper positioning for glycosyl transfer and cellulose translocation.
Article
Multidisciplinary Sciences
Thomas J. Oweida, Yaroslava G. Yingling
Summary: This study presents a method that integrates experimental small-angle X-ray scattering data and all-atom molecular modeling data using a genetic algorithm method for the determination of the atomistic representation of poly-Thymine DNA in solution. The results validate the performance of various AMBER force fields and implicit solvent models for ssDNA and enable a better understanding of the behavior of ssDNA in solution.
ADVANCED THEORY AND SIMULATIONS
(2023)
Meeting Abstract
Biochemistry & Molecular Biology
Felipe G. Quiroz
Article
Environmental Sciences
James S. Peerless, Alexey Gulyuk, Nina J. B. Milliken, Gyu Dong Kim, Elliot Reid, Jae Woo Lee, Dooil Kim, Zachary Hendren, Young Chul Choi, Yaroslava G. Yingling
Summary: Brine desalination is important for reducing the environmental impact of contaminated wastewater, but current techniques require high energy. We tested 10 organic solvents for solvent-based desalination efficacy using experiments and simulations. Solvents that form partial nanoscale phases effectively remove salt ions and capture water molecules. Our results contribute to the rational design of solvents for efficient desalination and low-cost fresh water production.
Article
Chemistry, Multidisciplinary
Benjamin P. Allen, Zoe M. Wright, Hailey F. Taylor, Thomas J. Oweida, Sabila Kader-Pinky, Emily F. Patteson, Kara M. Bucci, Caleb A. Cox, Abishec Sundar Senthilvel, Yaroslava G. Yingling, Abigail S. Knight
Summary: This study systematically investigates the structure-assembly relationships of PPAs, revealing that oligomer molecular weight and peptide hydrophilicity dictate morphology, while dispersity and peptide charge affect particle size.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)