Article
Chemistry, Analytical
Teng Zhou, Juncheng Zhao, Xiaohan He, Liuyong Shi, Liping Wen
Summary: Functionalized nanoparticles and nanochannels are widely used in various fields due to their unique properties. In this study, we established a theoretical model to investigate the impact of brush layer roughness on the charge density of nanoparticles. Our results show that as roughness increases, the charge density decreases, and as the concentration increases, the charge density tends to normalize. Additionally, the grafting density has little effect on the charge density. These findings provide valuable theoretical support for the application of nano-modification technology.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2023)
Article
Engineering, Environmental
Anshuman Satpathy, Qihuang Wang, Daniel E. Giammar, Zimeng Wang
Summary: The study compared different SCMs models and found that there were differences in performance when covering a broader range of conditions with experimental data, highlighting the need to develop a more reliable model. Through a systematic roadmap, it was found that the goethite-uranyl-carbonate ternary surface complexes were crucial in every model. The advanced triple-plane model provided the best fit.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2021)
Article
Chemistry, Multidisciplinary
Raju Lunkad, Fernando L. Barroso da Silva, Peter Kosovan
Summary: The mechanism of protein-polyelectrolyte complexation on the wrong side of the isoelectric point has puzzled researchers for a long time. Through simulation experiments, we found that both charge patch and charge regulation can lead to adsorption on the wrong side of the pI value. Their simultaneous presence enhances adsorption, while their absence prevents adsorption.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Polymer Science
Christopher Hill, Wasiu Abdullahi, Robert Dalgliesh, Martin Crossman, Peter Charles Griffiths
Summary: The study explores the phase space of oppositely charged polymer-surfactant complexes through interactions between charge-modified cationic hydroxyethyl cellulose polymers and sodium dodecylsulfate surfactant. Significant interactions were observed between the charge-modified polymers and SDS, leading to an increase in the size of the formed complexes with increasing Z.
Article
Chemistry, Physical
Chunlian Peng, Lili Song, Lian Wang, Fan Yang, Jianjun Ding, Fangzhi Huang, Yuqiao Wang
Summary: This study visually described the effect of surface charge distribution of phosphorus-doped MoS2 on hydrogen evolution by mapping the differential charge density. Through density functional theory calculations, the changes in electronic structure and atom interactions of MoS2 after phosphorus doping, as well as the bond strength between S and H atoms, were identified. Phosphorus doping improved the charge gradient distribution of MoS2, reduced the hydrogen adsorption energy on the surface, and effectively lowered the free energy of hydrogen evolution.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Nanoscience & Nanotechnology
Chixuan Liu, Yen Wah Tong
Summary: Bioprinting is a precise manufacturing technology for customized 3D biological constructs utilizing biomaterials, cells, and sometimes growth factors. However, its translational application is hindered by the lack of efficient techniques for blood vessel fabrications. In this report, an efficient blood vessel bioprinting technique based on interfacial polyelectrolyte complexation was proposed and investigated. This technique demonstrated clear vascular features and the study on peptide sequencing's effect on the biocompatibility of the polyelectrolyte-peptide amphiphile complex is also interesting and relevant for vascular structure fabrication research.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Engineering, Chemical
Ettore Virga, Klara Zvab, Wiebe M. de Vos
Summary: This study investigates the effect of membrane surface chemistry on fouling in surface water treatment for polyelectrolyte multilayer based nanofiltration membranes. Different surface chemistries were found to affect the adsorption of various foulants, with zwitterionic phosphatidylcholine surface chemistry demonstrating excellent fouling resistance.
JOURNAL OF MEMBRANE SCIENCE
(2021)
Article
Biochemistry & Molecular Biology
Magdalena Ptak-Kaczor, Mateusz Banach, Katarzyna Stapor, Piotr Fabian, Leszek Konieczny, Irena Roterman
Summary: Protein solubility relies on the compatibility of protein surface with polar water environment, influenced by the distribution of polar and hydrophobic residues. The fuzzy oil drop model quantifies the compatibility of hydrophobic distribution in proteins and predicts interactions with molecules of different polarity. Analyzing protein solubility helps in understanding protein folding and complex formation.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2021)
Article
Biochemistry & Molecular Biology
Hezhong Wang, Maren Roman
Summary: This study aimed to investigate the effects of chitosan molecular weight and degree of deacetylation on the formation of chitosan-cellulose nanocrystal polyelectrolyte-macroion complexes. The results showed that chitosan molecular weight had no significant effect on complex formation, but had a minor impact on particle shape and size. Lower sulfate group density and larger hydrodynamic diameter of CNCs, as well as higher degree of deacetylation of chitosan, resulted in higher turbidity levels, indicating the need for more CNCs for charge compensation.
Article
Chemistry, Physical
Yousef A. Alsunni, Charles B. Musgrave
Summary: In this study, grand canonical density functional theory (GC-DFT) was used to predict the surface energies, Wulff shapes, charge distributions, and catalytically active sites of different metal surfaces under electrochemical conditions. The results showed that solvation had a slight effect on the Wulff shape, while applied potentials significantly affected the surface energies and corresponding Wulff shapes. Bader charge analysis revealed that the electron density distribution on the surface atoms was uneven under applied potential, with atoms more exposed to the solvent being more sensitive to bias. The most sensitive atom to bias could be used to identify the most favorable adsorption site and the active sites of electrochemical reactions.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Alexey Rayevsky, Mohsen Sharifi, Eugeniy Demianenko, Dmitriy Volochnyuk, Michael Tukalo
Summary: The use of RESP method to obtain atomic charges can accurately predict the properties of post-transfer editing reaction observed in the AaRS system, showing better results compared to simulations with approximate charges and able to predict key properties induced by mutations.
Article
Cell Biology
Leixin Ouyang, Rubia Shaik, Ruiting Xu, Ge Zhang, Jiang Zhe
Summary: This article presents a method of mapping cell surface charge distribution via electrostatic cell-nanoparticle interactions, using fluorescent nanoparticles as markers. By establishing a relationship between fluorescent light intensity and number of nanoparticles, cells' surface charge distribution can be quantified. This method can be used for rapid surface charge mapping of single particles or cells, and yields results in good agreement with standard electrophoretic light scattering measurements.
Article
Biochemistry & Molecular Biology
Antonella Di Savino, Johannes M. Foerster, G. Matthias Ullmann, Marcellus Ubbink
Summary: Formation of protein complexes heavily relies on electrostatic interactions, which guide recognition and binding through optimized charge distributions on the surface of redox proteins. Investigating the interactions between cytochrome c peroxidase (CcP) and cytochrome c (Cc), it was found that additional charge patches can either enhance or disrupt productive complex formation depending on the presence of negative residues in the regular binding site.
Review
Chemistry, Physical
Maria Bonto, Ali A. Eftekhari, Hamidreza M. Nick
Summary: The surface charge of calcite plays a crucial role in various industrial and environmental applications. This paper reviews different surface complexation models proposed to explain the effects of surface interactions on calcite's zeta potential and discusses their main differences. The study reveals that the discrepancies between the models and experimental data can be explained by different levels of disequilibrium.
ADVANCES IN COLLOID AND INTERFACE SCIENCE
(2022)
Article
Chemistry, Physical
Florent Voisin, Gerald Lelong, Jean Michel Guigner, Thomas Bizien, Jean Maurice Mallet, Florent Carn
Summary: This article demonstrates the stabilizing effect of polyelectrolyte chains on globally neutral aggregates formed through electrostatic complexation. These stabilized complexes, composed of citrate-stabilized gold particles and quater-nized chitosan, are able to retain their nanometric size and stability in saline environment and cell culture media. The plasmonic coupling in these complexes allows for maximized optical absorption.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Celestine Hong, Osaid Alser, Anthony Gebran, Yanpu He, Wontae Joo, Nikolaos Kokoroskos, George Velmahos, Bradley D. Olsen, Paula T. Hammond
Summary: In this study, the interaction between nanoparticles and platelets was systematically evaluated in vitro and in vivo, showing that particle size plays a crucial role. Smaller particles were found to bind a larger percentage of platelets, while intermediate particles recruited more platelets to the wound, leading to enhanced hemostasis. Furthermore, smaller and intermediate nanoparticles exhibited longer circulation lifetimes, while larger nanoparticles accumulated more in the lungs. These findings highlight the importance of platelet content in aggregates and extended nanoparticle circulation lifetimes in enhancing hemostasis, providing useful insights for engineering particulate hemostats.
Article
Chemistry, Multidisciplinary
Dylan J. Walsh, Timo N. Schneider, Bradley D. Olsen, Klavs F. Jensen
Summary: This paper presents a design of a versatile, uniform light platform for photochemistry to improve the performance and reproducibility of high throughput experiments. The design is based on the development of an open-source ray tracing light simulation package and is experimentally validated using radiometry. The usefulness of the platform is demonstrated through its application in photoinduced electron transfer-reversible addition-fragmentation chain transfer polymerization of methyl acrylate.
REACTION CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Physical
Melody A. Morris, Rogerio A. Bataglioli, Danielle J. Mai, Yun Jung Yang, Justin M. Paloni, Carolyn E. Mills, Zachary D. Schmitz, Erika A. Ding, Allison C. Huske, Bradley D. Olsen
Summary: Protein materials have unique properties that make them suitable for various applications. This article introduces an automated platform for protein expression, which allows testing of different combinations of DNA vectors and Escherichia coli strains. Within a week, high-yield expression conditions can be determined.
MOLECULAR SYSTEMS DESIGN & ENGINEERING
(2023)
Article
Biochemistry & Molecular Biology
Rogerio A. Bataglioli, Bruno S. Leao, Carolyn E. Mills, Joao Batista M. Rocha Neto, Thiago B. Taketa, Bradley D. Olsen, Marisa M. Beppu
Summary: The self-assembled layer-by-layer technique is a popular method for engineering biofunctional surfaces. This paper introduces an automated, high-throughput approach to depositing polyelectrolyte multilayers (PEMs) in multiwell plates, allowing for screening of numerous film formulations simultaneously. The method was successfully validated by studying the deposition of different types of films and analyzing their properties. This study demonstrates the challenges associated with predicting the growth and properties of multilayer films and highlights the importance of the high-throughput layer-by-layer method in accelerating film development.
Article
Multidisciplinary Sciences
Katharina A. Fransen, Sarah H. M. Av-Ron, Tess R. Buchanan, Dylan J. Walsh, Dechen T. Rota, Lana Van Note, Bradley D. Olsen
Summary: The development of biodegradable plastics has been driven by the increasing plastic pollution. However, limited research on polymer biodegradation has hindered innovation due to costly and slow measurement methods. To tackle this issue, a high-throughput polymer synthesis and biodegradation method were utilized to generate a dataset for 642 chemically distinct polyesters and polycarbonates. The results showed that biodegradability depended on the length of the aliphatic repeat unit, with shorter chains and side chains improving biodegradability. Aromatic backbone groups generally hindered biodegradability, but ortho- and para-substituted benzene rings were more degradable than meta-substituted rings. In addition, ether groups in the backbone improved biodegradability.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Polymer Science
Haley K. Beech, Jeremiah A. Johnson, Bradley D. Olsen
Summary: Small angle neutron scattering was used to measure the single chain radii of gyration of end-linked polymer gels before and after cross-linking. The prestrain, which is the ratio of the average chain size in a cross-linked network to that of a free chain in solution, increased as gel synthesis concentration decreased near the overlap concentration. Dilute gels with higher loop fractions were found to be spatially homogeneous. The results provide a reference for network theories that rely on prestrain for the calculation of mechanical properties.
Article
Chemistry, Medicinal
Nathan J. Rebello, Tzyy-Shyang Lin, Heeba Nazeer, Bradley D. Olsen
Summary: Molecular search is essential in various fields, including chemistry, biology, and informatics. However, the search algorithms for polymers are less developed compared to small molecules due to the challenges in polymer naming and limited substructure search. This study introduces a novel query language and graph traversal search algorithm for polymers, which can fully capture all chemical structures in polymers. The algorithm has been validated against hundreds of target chemistries and topologies, demonstrating its effectiveness in matching monomer connectivity and polymer topology.
JOURNAL OF CHEMICAL INFORMATION AND MODELING
(2023)
Article
Chemistry, Multidisciplinary
Melody A. Morris, Carolyn E. Mills, Justin M. Paloni, Eric A. Miller, Hadley D. Sikes, Bradley D. Olsen
Summary: Evolution shapes diverse properties of proteins. Incorporating proteins into materials is desired for applications, but high-throughput selection techniques are lacking. This study established a high-throughput platform to assess binding affinity for ordered sensing proteins. Fusion proteins library was constructed, and selected variants showed high binding in films. The assembly of fusion proteins and the functionality of binding protein are key factors in biosensing performance. Integration of directed evolution with assembled systems is necessary for designing better materials.
Article
Materials Science, Multidisciplinary
Ameya Rao, Brian R. Carrick, Helen Yao, Bradley D. Olsen
Summary: This study investigates the effects of transient binding on short-time segmental dynamics in associative polymer gels. The results show that a short-time cooperative diffusion mode is observed in all gels, but the diffusion coefficients decrease with increasing junction density. Additionally, the characteristic length scale of nondecaying chain dynamics is estimated to be smaller than the interjunction spacing but similar to the correlation blob size of the overlapping strands.
PHYSICAL REVIEW MATERIALS
(2023)
Article
Chemistry, Physical
Ameya Rao, Bradley D. D. Olsen
Summary: This study investigates the static gel structure and cooperative multi-chain motion in associative networks using a model system composed of artificial coiled-coil proteins. The results show evidence for three static length scales in all protein gel designs, which are attributed to correlations from blob length, inter-junction spacing, and multi-chain density fluctuations. The self-diffusion measurements reveal a transition between slow and fast diffusive species, occurring on a length scale similar to the neutron scattering observations. The analysis supports the primarily single-chain mechanisms of self-diffusion and the occurrence of single-molecule hopping.
Article
Polymer Science
Haley K. Beech, Shu Wang, Devosmita Sen, Dechen Rota, Tatiana B. Kouznetsova, Akash Arora, Michael Rubinstein, Stephen L. Craig, Bradley D. Olsen
Summary: The study explores reactivity-guided fracture in polymer networks with different compositions of strands. It is found that increasing the content of less reactive strands has a negligible impact on the fracture energy until a certain threshold, after which the fracture energy sharply increases. The study also reveals that the loss of percolated network structure is a necessary criterion for crack propagation in polymer networks.
Article
Polymer Science
Haley K. Beech, Tzyy-Shyang Lin, Devosmita Sen, Dechen Rota, Bradley D. Olsen
Summary: The gel point behavior of end-linked poly-(ethylene glycol) gel was studied through experiments and simulations. Results showed that the forward and reverse gel points diverged as the concentration decreased, suggesting that kinetic effects caused a departure from percolation behavior in defect-rich gels.
Article
Chemistry, Multidisciplinary
Ludwig Schneider, Dylan Walsh, Bradley Olsen, Juan de Pablo
Summary: The enhanced version of BigSMILES notation, called generative BigSMILES, provides a foundational tool for automated polymeric material design. By integrating additional data and utilizing a generative graph algorithm, the notation allows for efficient specification of complex molecular ensembles. The combination of generative BigSMILES with advanced machine learning techniques has the potential to accelerate materials design processes and advance the field of polymer science.
Article
Chemistry, Multidisciplinary
I. Caglar Tanrikulu, Lianna Dang, Lekha Nelavelli, Aubrey J. Ellison, Bradley D. Olsen, Song Jin, Ronald T. Raines
Summary: This study successfully designed synthetic collagen hydrogels by maximizing the interactions of the triple helix structure of collagen. It further explored the relationship between self-assembly of short CMPs and interfiber association.
Article
Engineering, Environmental
Yue Wu, Chen Yuan, Xianjing Jia, Zhiyuan Zheng, Xijiao Yang, Jintao Yang, A. Basak Kayitmazer, Ayyaz Ahmad, Naveed Ramzan, Yisheng Xu
Summary: In this study, stable dye-sensitized upconversion nanoparticles (UCNPs) were prepared using flash nanoprecipitation (FNP) technology for cancer cell imaging and treatment. Compared to traditional methods, UCNPs obtained through FNP exhibited smaller size, narrower size distribution, and higher stability.
CHEMICAL ENGINEERING JOURNAL
(2023)