Article
Chemistry, Multidisciplinary
Gustav Ferrand-Drake Castillo, Maria Kyriakidou, Zeynep Adali, Kunli Xiong, Rebekah L. N. Hailes, Andreas Dahlin
Summary: This study presents the first interface that can be electrically switched between a high-capacity protein binding state and a completely non-fouling state. The technology offers various applications, such as zero fouling on demand, protein patterning or separation, and controlled release of biologics in a physiological environment.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Leonid I. Klushin, Alexander M. Skvortsov, Alexey A. Polotsky, Anna S. Ivanova, Friederike Schmid
Summary: A novel class of responsive polymer brushes with controllable grafting density has been proposed in this study, using end-grafted polymer chains that have an affinity to the substrate. The dense layer and the outer brush can be seen as coexisting microphases, with the effective grafting density controlled by adsorption strength. Numerical self-consistent field calculations and scaling arguments demonstrate the reversible and controlled changes in grafting density in response to environmental parameters.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Nanoscience & Nanotechnology
Neslihan Torun, Ilker Torun, Menekse Sakir, Mustafa Kalay, M. Serdar Onses
Summary: There is a strong demand for encoded surfaces with multiple security layers that are prepared by stochastic processes and are adaptable to deterministic fabrication approaches. Dewetting instabilities in nanoscopic polymer films present a suitable platform for fabricating unclonable surfaces, with the thermal annealing-induced dewetting of P2VP enabling fabrication of randomly positioned functional features that are separated at a microscopic length scale. The patterning of P2VP films presents opportunities for fabricating hybrid security labels, which can be resolved through both stochastic and deterministic pathways, offering key opportunities in encoding applications.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Review
Materials Science, Multidisciplinary
Adnan Murad Bhayo, Yang Yang, Xiangming He
Summary: Polymer brushes are thin films consisting of polymer chains attached to a solid interface by one end. These highly branched polymers exhibit unique characteristics and properties compared to their linear counterparts, making them widely used in fields such as drug delivery and tissue engineering. Surface-initiated controlled radical polymerization has provided a robust method to tailor the chemical and physical properties of surfaces and interfaces, leading to significant innovations in surface and interface engineering.
PROGRESS IN MATERIALS SCIENCE
(2022)
Article
Polymer Science
Riccardo Chiarcos, Diego Antonioli, Valentina Gianotti, Michele Laus, Gianmarco Munao, Giuseppe Milano, Antonio De Nicola, Michele Perego
Summary: In this study, two copolymers were thermally grafted from melt to a silicon wafer, and it was observed that the lower molecular weight component of the blend preferentially grafted to the polymeric brush layer. The enrichment of short chains in the brush layer was found to be independent of time. Molecular dynamics simulations supported this observation, providing insights for further investigation and control of brush layer characteristics.
Article
Polymer Science
Yu-Min Wang, Anna Kalosi, Yuriy Halahovets, Iryna Romanenko, Jiri Slaby, Jiri Homola, Jan Svoboda, Andres de los Santos Pereira, Ognen Pop-Georgievski
Summary: This study compared the anti-fouling properties of poly(HPMA) brushes prepared by chemisorption and surface-initiated polymerization methods, finding that the latter exhibited better anti-fouling performance due to higher grafting density.
Review
Engineering, Biomedical
Danyang Li, Lizhou Xu, Jing Wang, Julien E. Gautrot
Summary: Responsive polymer brushes are capable of conformational and chemical changes in response to external stimuli, offering unique opportunities for the control of bio-nano interactions. They can be designed on a wide range of nanomaterial surfaces without compromising their physical and imaging properties. Research on the use of responsive brushes as smart delivery systems is still in its early stages.
ADVANCED HEALTHCARE MATERIALS
(2021)
Article
Chemistry, Physical
Xiyong Li, Xuan Li, Wenqin Wang
Summary: Poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) brushes were grafted onto graphene oxide (GO) film using the self-initiated photografting and photopolymerization (SIPGP) method. Silver nanosheet-assembled microspheres were spontaneously grown on the GO-g-PDMAEMA film in [Ag(NH3)2]OH solution. The shape and size of the microspheres could be easily controlled by adjusting reaction time and the concentration of [Ag(NH3)2]OH solution. The obtained GO-g-PDMAEMA/Ag film exhibited excellent surface-enhanced Raman scattering (SERS) performances, with a limit of detection (LOD) of 10-16 M for 4-ATP and 10 ng/mL for thiram.
CHEMICAL PHYSICS LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Biao Zuo, Cheng Li, Quanyin Xu, Katelyn Randazzo, Naisheng Jiang, Xinping Wang, Rodney D. Priestley
Summary: This study demonstrates that polymer brushes with ultrahigh grafting density exhibit significantly improved thermal stability, overcoming confinement and interfacial effects to control thin-film material properties. The dense packing and molecular ordering in the amorphous state of ultradense brushes prepared by surface-initiated atom transfer radical polymerization in combination with a self-assembled monolayer of initiators play a crucial role in enhancing the thermal stability of polymer films.
Article
Chemistry, Physical
Barbara Capone, Christos N. Likos, Ivan Coluzza
Summary: Through multiscale molecular simulation, it is shown that solvophilic-solvophobic AB diblock copolymer brushes exhibit a re-entrant disorder/order/disorder transition in the semi-dilute regime. This transition is fully controllable through adjustments to the grafting density and the solvophobic to solvophilic ratio of the tethered macromolecules. The transition from order to disorder is explained by the density dependent shrinkage of aggregates, which is caused by entropic/enthalpic competition during hierarchical self-assembly of the brush.
Article
Polymer Science
Diego Antonioli, Riccardo Chiarcos, Valentina Gianotti, Margherita Terragno, Michele Laus, Gianmarco Munao, Giuseppe Milano, Antonio De Nicola, Michele Perego
Summary: In this study, the grafting reaction of copolymers with different compositions onto a silicon wafer showed that lower molecular weight components are selectively incorporated into the polymeric brush. The time, temperature, and composition of blends were found to systematically affect the final brush layer composition. Hybrid particle-field simulations suggested that the preference of short chains to react with the silicon surface is influenced by the number of chains in contact with silica and the substrate surface area occupied by a single chain.
Article
Chemistry, Applied
Thi Nguyet Tran, Arnaud Nourry, Pamela Pasetto, Guillaume Brotons
Summary: A new methodology for covalently grafting polyisoprene onto various surfaces has been developed, achieving high glass surface coverage density and strong covalent bonding. This method allows for the formation of versatile polymeric constituents and represents a new family of sustainable coatings.
PROGRESS IN ORGANIC COATINGS
(2021)
Article
Chemistry, Multidisciplinary
Jean-Francois Berret, Alain Graillot
Summary: In this feature article, the authors provide an overview of their research on using statistical copolymers as a coating material for metal oxide nanoparticles and surfaces. They develop a polymer-based coating platform that shares features with self-assembled monolayer and layer-by-layer deposition techniques. The synthesized copolymers containing phosphonic acid groups show strong affinity to metals and experimental evidence of colloidal stability of the coated particles. Applications in nanomaterials and nanomedicine are also discussed, including the beneficial effects of coatings on nanopowders, contrast agents, and stimuli-responsive particles.
Article
Materials Science, Multidisciplinary
Ruchun Zhou, Rana Mhanna, Ming Jin, Haiyan Pan, Decheng Wan, Davy-Louis Versace, Constance Thomas, Fabrice Morlet-Savary, Olivier Soppera, Jean-Pierre Malval
Summary: This study describes an original structure-reactivity relationship within a series of type II photoinitiators based on a multibranched molecular engineering strategy. It was found that the photoinitiating efficiency of these multipolar derivatives is mainly modulated by a solvent-mediated interplay between intersystem crossing and intramolecular charge transfer processes at the excited singlet state. This balancing mechanism significantly enhances the photoinitiation performance by more than 1 order of magnitude in the series.
ACS APPLIED POLYMER MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Jade Poisson, Alexander M. Polgar, Michele Fromel, Christian W. Pester, Zachary M. Hudson
Summary: An oxygen-tolerant approach has been introduced for preparing surface-tethered polymer films of organic semiconductors directly from electrode substrates. The PET-RAFT method was used to prepare multiblock polymer architectures resembling multi-layer OLEDs, and the preparation of TADF and TAF trilayer OLED architectures was described. The surface-initiated (SI)-PET-RAFT approach allows enhanced control over layer thickness and spatial resolution in polymer brush patterning at low cost utilizing direct photomasking and a digital micromirror device.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Multidisciplinary Sciences
Christopher Vega-Sanchez, Sam Peppou-Chapman, Liwen Zhu, Chiara Neto
Summary: This study reveals that lubricant-infused surfaces can effectively reduce drag in microfluidic flow. The spontaneous nucleation of surface nanobubbles leads to a significant increase in interfacial slip, a mechanism that is likely to occur on most infused surfaces.
NATURE COMMUNICATIONS
(2022)
Review
Chemistry, Multidisciplinary
Christopher Vega-Sanchez, Chiara Neto
Summary: The correct theoretical definition of boundary conditions for flow is essential for fluid dynamics studies, especially in confined nano- and micro-scale flows. The pressure drop versus flow rate method is useful for detecting microscale interfacial slip and drag reduction. Comparing accurate experiments with theoretical models can provide clarity on slip mechanisms on smooth and structured surfaces.
ADVANCED MATERIALS INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Jun Ki Hong, Kavya Mathur, Alexander M. Ruhoff, Behnam Akhavan, Anna Waterhouse, Chiara Neto
Summary: Tethered-liquid perfluorocarbon (TLP) coatings have shown potential in reducing blood adhesion and delaying thrombosis on blood-contacting medical devices. In this study, a vapor phase silanization reaction was used to create tethered-perfluorocarbon (TP) layers with large bumpy aggregates on top of a uniform coating. The vapor phase method was found to be effective in reproducibly creating slippery coatings with low water sliding angles. The TP layer retained perfluorinated lubricants even under high shear rates and showed reduced fibrin adhesion from human whole blood compared to control surfaces.
ADVANCED MATERIALS INTERFACES
(2022)
Article
Chemistry, Medicinal
Malachy Maher, Veronica Glattauer, Carmine Onofrillo, Serena Duchi, Zhilian Yue, Timothy C. Hughes, John A. M. Ramshaw, Gordon G. Wallace
Summary: This study compares the potential and performance differences of collagen from marine and porcine sources in tissue engineering. Collagen derived from marine sources has lower risk of disease transfer and is more compatible with religious and ethical groups. Although it has inferior mechanical properties and is prone to degradation, marine-derived collagen is still considered a promising biomaterial.
Article
Polymer Science
Malachy Kevin Maher, Jacinta F. White, Veronica Glattauer, Zhilian Yue, Timothy C. Hughes, John A. M. Ramshaw, Gordon G. Wallace
Summary: Collagen, as the most abundant protein in the extracellular matrix, has been extensively studied in tissue engineering and regenerative medicine. Collagen type I is commonly used in laboratory studies. The structure of the collagen fibril network affects cellular proliferation, differentiation, and the modulus of hydrogels. This study compared the network-forming properties of two forms of collagen and investigated the impact of methacrylation on the crosslinking and 3D printing suitability. The results showed that the presence of telopeptides facilitated fibril formation, but methacrylation reduced the self-assembly potential. Crosslinking improved the fibril-like network structure.
Article
Biophysics
Muamer Dervisevic, Esma Dervisevic, Lars Esser, Christopher D. Easton, Victor J. Cadarso, Nicolas H. Voelcker
Summary: Microneedle-based wearable sensors provide an alternative approach for health monitoring and disease diagnostics by detecting pH levels in the skin interstitial fluid. This technology significantly contributes to the advancement of wearable sensors, simplifies the manufacturing process, and improves cost-effectiveness.
BIOSENSORS & BIOELECTRONICS
(2023)
Article
Chemistry, Multidisciplinary
Amane Shiohara, Marcin Wojnilowicz, Quanxia Lyu, Yi Pei, Christopher D. Easton, Yu Chen, Jacinta F. White, Alexander McAuley, Beatriz Prieto-Simon, Helmut Thissen, Nicolas H. Voelcker
Summary: The development of simple, cost-effective, rapid, and quantitative diagnostic tools is crucial for monitoring infectious COVID-19 disease. This study demonstrates a unique approach to fabricate a nanochannel-based electrochemical biosensor that can detect the entire SARS-CoV-2 virus instead of virus fragments. The biosensor shows a low limit of detection and a wide detection range, and is able to differentiate saliva samples with SARS-CoV-2 from those without, showing potential for translation into a point-of-care biosensor product.
Article
Chemistry, Physical
Anthony Katselas, Isaac J. Gresham, Andrew R. J. Nelson, Chiara Neto
Summary: The capture of moisture from the atmosphere through condensation has the potential to provide a sustainable source of water. This study investigates how water contact angle and contact angle hysteresis affect the rates of water capture during condensation of humid air at low subcooling conditions. The results show that hydrophilic and slippery hydrophilic surfaces are preferable for efficient dew collection applications.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Materials Science, Coatings & Films
George H. H. Major, B. Maxwell Clark, Kevin Cayabyab, Nathan Engel, Christopher D. D. Easton, Jan Cechal, Donald R. R. Baer, Jeff Terry, Matthew R. R. Linford
Summary: This study examines the adequacy of reporting metadata for understanding x-ray photoelectron spectroscopy (XPS) data collection and analysis in scientific literature. Data from papers published in high-quality journals during a six-month period in 2019 and throughout 2021 were evaluated. The study found varying percentages of reported information, including spectrometer (66%), fitting software (15%), x-ray source (40%), etc. The results show good agreement over the two-year survey period, with indications of potential improvement.
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A
(2023)
Article
Chemistry, Physical
Lyndi E. Strange, Mark H. Engelhard, Christopher D. Easton, Ju-Myung Kim, Donald R. Baer
Summary: X-ray photoelectron spectroscopy (XPS) is important for analyzing battery materials, but there are many flaws in the analysis and data in the literature. This paper highlights the challenges analysts face when using XPS for battery materials and discusses recent literature that addresses these issues. One common error is ignoring peak overlaps and interferences, which is significant for battery electrodes composed of multiple elements. The paper uses examples of Li and nickel-manganese-cobalt (NMC) electrodes to illustrate the challenges associated with XPS analysis in battery systems.
SURFACE AND INTERFACE ANALYSIS
(2023)
Article
Chemistry, Multidisciplinary
Isaac J. Gresham, Seamus G. Lilley, Andrew R. J. Nelson, Kaloian Koynov, Chiara Neto
Summary: This study quantifies the properties of a range of PDMS SCALS and elucidates their nanostructure responsible for their properties. The study also shows that the properties of SCALS can be predicted by reducing the grafting density, with the lowest water contact angle hysteresis achieved at a grafting density of approximately 2.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Engineering, Environmental
Fanyi Li, Tao Huang, Paul Pasic, Christopher D. Easton, Nicolas H. Voelcker, Daniel E. Heath, Neil M. O'Brien-Simpson, Andrea J. O'Connor, Helmut Thissen
Summary: All indwelling and implantable medical devices are at risk of infection. Strategies that combine multiple layers of defense, such as a copolymer coating with antimicrobial selenium nanoparticles, show promise in providing effective protection against pathogen colonization and biofilm formation. The antimicrobial coating demonstrated low attachment of bacteria and additional bactericidal functionality against commonly found pathogens. It also exhibited effective inhibition of bacterial growth in areas where the coating had been removed. The research shows the feasibility of modulating the release of selenium nanoparticles from the coating and confirms their superior biocompatibility compared to silver nanoparticles.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Glen McHale, Rodrigo Ledesma-Aguilar, Chiara Neto
Summary: In 1948, Cassie proposed an equation for the wetting of a smooth, heterogeneous surface. This equation uses weighted averages based on the fractional surface areas and cosines of contact angles to predict the contact angle of a droplet on a composite surface. The equation has proven fundamental in understanding the wetting of superhydrophobic and superoleophobic surfaces. However, little attention has been given to the complete wetting of one surface component.
Article
Chemistry, Analytical
Ziqiu Tong, Lars Esser, Peter Galettis, Helmut Thissen, David Rudd, Christopher D. Easton, Azadeh Nilghaz, Bo Peng, Douer Zhu, Jennifer H. Martin, Nicolas H. Voelcker
Summary: This paper explores the use of a synthetic fluoropolymer, Teflon(TM) AF 2400, to functionalize organ-on-chip systems, reducing the absorption of hydrophobic compounds. Using CBD as a test compound, the researchers quantified CBD absorption into PDMS and found that surface modification with the fluoropolymer significantly increased CBD signals. The study also demonstrated the compatibility of fluoropolymer-modified microchannels for cell culture and CBD perfusion experiments.
Meeting Abstract
Cell & Tissue Engineering
Ashley R. Murphy, Grace Lidgerwood, Alice Pebay, Yen B. Truong, Carmel M. O'Brien, Veronica Glattauer
TISSUE ENGINEERING PART A
(2022)
