Review
Biotechnology & Applied Microbiology
M. Artico, C. Roux, F. Peruch, A. -F. Mingotaud, C. Y. Montanier
Summary: This review addresses the challenges and methods of grafting proteins onto synthetic polymer surfaces. The sensitivity of polymers to aqueous media and the differences in chemical functions and physical properties make protein grafting on synthetic polymers a unique process. The review discusses various routes of covalently bonding proteins onto polymeric substrates and highlights the concern of potential loss of function. The characterization methods used to determine grafting efficiency and enzyme behavior are also examined. Furthermore, the review considers the industrial applications and future prospects of protein grafting, emphasizing the importance of sustainable processes based on green chemistry.
BIOTECHNOLOGY ADVANCES
(2023)
Article
Materials Science, Multidisciplinary
Wenfu Zhang, Liang Liu, Rui Bao, Jianhong Yi, Yajie Yang, Caiju Li, Xiaofeng Chen, Shengda Guo
Summary: Tailoring the structural design of reinforcement is an effective strategy to achieve homogeneous dispersion and robust interface bonding in CNTs/Cu composites. A novel zero-dimensional carbonized polymer dots (CPD) were synthesized and grafted onto the surfaces of CNTs via a one-step hydrothermal method. The resulting CPD@CNTs reinforcement showed good dispersibility due to the abundant polar functional groups on CPD. In addition, the interface adhesion was improved by the in-situ formation of Cu2O transient phase. The CPD@CNTs/Cu composite demonstrated outstanding mechanical performances with increased yield strength and tensile strength, while maintaining excellent ductility. Moreover, the electrical conductivity of the composite remained high. Our findings suggest that adjusting the structural configuration of reinforcement is a feasible approach to optimize dispersion and interfacial structure.
DIAMOND AND RELATED MATERIALS
(2023)
Article
Chemistry, Applied
Caroline Pereira, Jean-Sebastien Baumann, Vincent Humblot, Celine Falentin-Daudre
Summary: This study aimed to improve the adhesion and differentiation of osteoblast cells on titanium surfaces by grafting poly(VBP). The results showed that poly(VBP) grafted on titanium surfaces significantly improved the interaction between osteoblast cells and the surface.
REACTIVE & FUNCTIONAL POLYMERS
(2022)
Article
Chemistry, Physical
Haifeng Zhou, Bowu Zhang, Weihua Liu, Yanling Xue, Changwei Zhao, Xiaodong Zhang, Xiuhai Cui, Zhongfeng Tang
Summary: In this study, a new method was explored to graft glycidyl methacrylate (GMA) onto the surface of high-modulus carbon fiber (HMCF), which has extremely high chemical inertness. GMA was successfully grafted onto HMCF after acid activation synergized with ionization radiation, with a grafting degree of 22%. The hydrophilicity of the fiber was effectively improved after acid activation and grafting, and it showed good dispersibility in water. The surface structure of the fiber became highly disordered after grafting GMA. This work provides a new pathway for the modification of HMCF and is beneficial for obtaining high performance HMCF composites.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Analytical
Seunghwa Yang
Summary: In this study, the effects of grafting single-walled and multi-walled carbon nanotubes onto polymer matrices were systematically investigated using molecular dynamics simulations. Key material properties such as interfacial load transfer, alteration of nanotube properties, and dispersion of nanotubes in the polymer matrix were specifically studied. The results show that covalent grafting has two rivalling effects, improving interfacial load transfer in nanocomposites and altering nanotube properties through enhanced interface. Additionally, covalent functionalization with PET molecules can alter nanotube solubility and enhance dispersibility in the polymer matrix.
Article
Chemistry, Physical
Eric Osei-Agyemang, Arish Dasan, Romain Lucas, Sylvie Foucaud, Sylvain Cristol, Etienne Laborde
Summary: This study focuses on grafting polymeric precursors onto functionalized ZrC surfaces to synthesize ZrC/SiC core/shell composites. The surface modification and subsequent grafting reactions were found to be favorable and promising for the synthesis of organic macromolecules on ZrC/SiC interfaces.
APPLIED SURFACE SCIENCE
(2022)
Article
Multidisciplinary Sciences
Tatsuya Arai, Akari Yamauchi, Yue Yang, Shiv Mohan Singh, Yuji C. Sasaki, Sakae Tsuda
Summary: In cold environments, many microorganisms can survive by synthesizing ice-binding proteins (IBPs). Two isoforms of IBP from Psychromyces glacialis were found to have moderate thermal hysteresis (TH) activity and high ice recrystallization inhibition (IRI) activity. These isoforms have weaker binding ability to the whole surface of an ice crystal compared to hyperactive IBP species.
SCIENTIFIC REPORTS
(2022)
Article
Chemistry, Physical
Shengshen Gu, Aleksei N. Marianov, Yijiao Jiang
Summary: This study investigates the electrocatalytic activity of amino-substituted Co porphyrin for CO2ERR, showing that the covalently grafted complex CoTAP-cov is one of the best catalysts to date. The presence of NH2 groups and covalent grafting are essential for maximizing the activity and efficiency of the catalyst.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Physical
Melissa K. Stanfield, Jerome Medard, Philippe Decorse, Catherine Combellas, Frederic Kanoufi, Luke C. Henderson, David J. Hayne, Filip Stojcevski, Fetah Podvorica, Jean Pinson
Summary: Electrografting of different polymers directly on various materials without a primary layer is achieved using a radical initiator, 2,6-dimethylbenzenediazonium. This one-step process allows for the polymerization of the vinylic monomer by an electrochemically reduced aryl radical, which reacts with the surface. Polymethyl methacrylate, poly1H,1H-perfluorooctyl methacrylate, polyglycidyl methacrylate, polyacrylic acid, poly(ethyleneglycol) diacrylate, and vinylferrocene were tested as the polymers. Experimental analysis confirms successful surface functionalization. Electrografting of carbon fibers enhances the mechanical properties of carbon-epoxy composites, as demonstrated by increased tensile strength, Young's modulus, and interfacial shear strength.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Benjamin F. Bachman, Zachary R. Jones, Gabriel R. Jaffe, Jad Salman, Raymond Wambold, Zhaoning Yu, Jennifer T. Choy, Shimon J. Kolkowitz, Mark A. Eriksson, Mikhail A. Kats, Robert J. Hamers
Summary: This study demonstrates a highly controlled approach to functionalizing diamond surfaces with carboxylic acid groups through all-carbon tethers of different lengths, followed by covalent chemistry to yield high-quality TEMPO-modified surfaces. The estimated surface densities of 4-amino-TEMPO on nanodiamond and planar diamond are higher than those reported previously using other functionalization methods. The zeta-potential of nanodiamonds was used to track reaction progress and elucidate the regioselectivity of the reaction.
Article
Biochemistry & Molecular Biology
Inho Kim, Yohan Kim, Sung Min Kang
Summary: Grafting zwitterionic molecules onto solid surfaces is an important method for reducing the unwanted adsorption of biomolecules. Various approaches have been used, including zwitterionic monolayer/multilayer formation and surface-initiated polymerization. Recently, a coordination-driven approach has been discovered to be effective. However, the resistance against bacterial adhesion and other fouling organisms has not been fully explored. In this study, the coordination-driven surface zwitteration is systematically investigated using different molecular weights of sulfobetaine polymers. The high molecular weight polymer is found to be crucial for achieving strong resistance to protein adsorption and marine fouling.
MACROMOLECULAR BIOSCIENCE
(2022)
Article
Chemistry, Physical
Pei-Hua Chen, Chan-Pong Iun, Jung-Chin Tsai, Muoi Tang
Summary: Supercritical carbon dioxide (SCCO2) was used to modify the surface of polyacrylonitrile (PAN) membrane by grafting the hydrophilic monomer, 2-hydroxyethyl methacrylate (HEMA). The grafting reaction was achieved using a two-step process in SCCO2, resulting in a significantly improved hydrophilicity of the modified PAN surface.
JOURNAL OF SUPERCRITICAL FLUIDS
(2022)
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, Physical
Jojibabu Panta, Andrew N. Rider, John Wang, Richard Yang, Narelle Brack, Y. X. Zhang
Summary: Incorporating branched polyethyleneimine dendrimer (PEI) functionalized carbon nanotubes (CNTs) and a phase-separated triblock copolymer significantly enhanced the lap shear strength of epoxy-based adhesive. The level of PEI grafting was controlled by adjusting the CNT to PEI dispersion ratio and led to grafting percentages ranging from 5% to 51%. The highest grafting ratios improved the dispersion of CNTs, but heterogeneous curing reactions and localised stress concentrations caused a reduction in lap shear strength.
APPLIED SURFACE SCIENCE
(2023)
Article
Materials Science, Multidisciplinary
Lina Yang, Ping Han, Zheng Gu
Summary: Grafting hyperbranched polymer onto the carbon fiber surface can significantly enhance the interfacial properties of carbon fiber/epoxy composites, improving the mechanical performance and thermal stability of the composites.
MATERIALS & DESIGN
(2021)
Article
Chemistry, Multidisciplinary
Robert J. Hamers, Desiree M. Bates, Kristopher Jose Aguayo Barragan, Danica G. Gressel, Beau S. Schweitzer, Jairo Villalona, Cheri A. Barta, Judith Burstyn, Andrew E. Greenberg, Michael P. Schwartz
Summary: This study describes programs at the University of Wisconsin-Madison Department of Chemistry aimed at increasing representation and improving outcomes for graduate students from underrepresented minority groups. The experiences have yielded both successes and failures, providing direction for future improvements and efforts.
JOURNAL OF CHEMICAL EDUCATION
(2022)
Article
Chemistry, Multidisciplinary
Fangjia Li, Hugh D. Mitchell, Arielle C. Mensch, Dehong Hu, Elizabeth D. Laudadio, Jenny K. Hedlund Orbeck, Robert J. Hamers, Galya Orr
Summary: This study utilized single-cell analysis to investigate individual cell responses to lithium cobalt oxide nanoparticles, revealing significant variability in gene expression levels between neighboring cells under the same exposure conditions, as well as a prioritization of gene expression for restoring energy balance in individual cells.
Article
Nanoscience & Nanotechnology
Becky J. Curtis, Nicholas J. Niemuth, Evan Bennett, Angela Schmoldt, Olaf Mueller, Aurash A. Mohaimani, Elizabeth D. Laudadio, Yu Shen, Jason C. White, Robert J. Hamers, Rebecca D. Klaper
Summary: The physico-chemical characteristics of engineered nanomaterials play a crucial role in their impact on organisms, but the sensitivity of different species also contributes to the effects. Various factors, such as differences in biochemical responses, exposure, and uptake, may cause the sensitivity to vary significantly across species. A comparison of three model species revealed that their different sensitivities to lithium cobalt oxide nanosheets can be attributed to variations in immune-response, iron-sulfur protein, and central nervous system pathways. Nanomaterial uptake and dissolution do not fully explain the differences between species.
NATURE NANOTECHNOLOGY
(2022)
Article
Chemistry, Physical
Hugo Nolan, Christian Schroder, Marc Brunet-Cabre, Filippo Pota, Niall McEvoy, Kim McKelvey, Tatiana S. Perova, Paula E. Colavita
Summary: The study investigates the effects of N-functionalities on MoS2 supported on carbon for hydrogen evolution reaction (HER) performance. It is found that the presence of pyridinic-N groups at the carbon support suppresses HER activity at high pH due to the modulation of deprotonation and lone-pair availability. This suggests important implications for the design of heterostructured electrocatalysts to control performance in HER electrocatalysis by exploiting synergistic/inhibitory behaviors.
Article
Multidisciplinary Sciences
Marc Brunet Cabre, Dahnan Spurling, Pietro Martinuz, Mariangela Longhi, Christian Schroder, Hugo Nolan, Valeria Nicolosi, Paula E. Colavita, Kim McKelvey
Summary: Through unique experimental configuration, researchers found that the pseudocapacitive charge storage in Ti3C2Tx MXenes in acid electrolytes involves proton intercalation/deintercalation, redox switching of the Ti centres, and protonation/deprotonation of oxygen functional groups. They also observed pseudocapacitive charging outside the electrochemical contact area, suggesting a fast transport of protons mechanism across the MXene surface. These findings provide new insights into the surface chemistry of MXenes.
NATURE COMMUNICATIONS
(2023)
Editorial Material
Chemistry, Multidisciplinary
Anke Krueger, Nianjun Yang, Robert J. Hamers
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Electrochemistry
L. V. Morris, C. A. Ortiz-Ledon, R. J. Hamers
Summary: A new class of organosilicon additives was introduced to explore their effect on the electrochemistry of Si anode surfaces during the first cycle. EQCM and EIS were used to investigate the impedance of the cells and XPS was used to analyze the composition of the SEI layers. The results showed that the organosilicon-treated cells had an increase in impedance and thinner SEI layers richer in LiF and with less organic material.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Nanoscience & Nanotechnology
Paige C. Kinsley, Curtis M. Green, Jaya Borgatta, Catherine E. Kruszynski Earl, Elizabeth D. Laudadio, Robert J. Hamers
Summary: We have developed a method to control the behavior of metal oxide nanoparticles in aqueous media by producing nanometer-thin carbon shells on their surface, allowing subsequent covalent chemical functionalization with molecular ligands. This approach enables the nanoparticles to acquire specific molecular properties in aqueous media, utilizing the strong and stable C-C interfacial bonds between the surface ligands and the carbon shell.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Physical
Michelle P. Browne, Carlota Dominguez, Can Kaplan, Michael E. G. Lyons, Emiliano Fonda, Paula E. Colavita
Summary: By using X-ray photoelectron spectroscopy and X-ray absorption spectroscopy, it is found that the Mn content influences the active site of Mn/Ru oxide materials for the oxygen evolution reaction (OER), which may enhance the activity by changing the oxygen coordination environment of Ru sites.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Deepti Sharan, Daniel Wolfson, Curtis M. Green, Paul Lemke, Alessandra G. Gavin, Robert J. Hamers, Z. Vivian Feng, Erin E. Carlson
Summary: The use of complex metal oxide nanoparticles has increased significantly in recent years, particularly in electric vehicle batteries. However, our understanding of their impact on environmental organisms has not kept pace with their usage. This study examines the effects of chronic exposure to nanoscale lithiated nickel manganese cobalt oxide (NMC) on the bacterium Shewanella oneidensis. The results show that chronic exposure to NMC leads to genetic-level variation in the bacteria, including the production of reactive oxygen species (ROS) and DNA damage.
ENVIRONMENTAL SCIENCE-NANO
(2023)
Article
Materials Science, Multidisciplinary
David T. T. Hinds, Samir A. A. Belhout, Paula E. E. Colavita, Andrew D. D. Ward, Susan J. J. Quinn
Summary: In this work, high loading of gold nanoparticles (AuNPs) were assembled on porous carbon microspheres (C mu P) to prepare surface-enhanced Raman scattering (SERS) active materials. The specific surface functionalization of C mu Ps using carboxylic acid and thiol groups allowed for the immobilization of AuNPs. By treating the surface-immobilized gold nanoparticles with hydroquinone, a roughened gold surface with significantly increased Au loading was prepared. Various characterization techniques were used to analyze the materials, and the SERS capacity of individual particles to detect malachite green was investigated. A pinning approach was employed to overcome the challenges in trapping these materials. The porous carbon particles showed great potential as versatile scaffolds for SERS applications.
MATERIALS ADVANCES
(2023)
Article
Chemistry, Multidisciplinary
Shreyasi Sengupta, Swapnil B. Ambade, Tana L. O'Keefe, Falak Tawakalna, Jenny K. Hedlund Orbeck, Robert J. Hamers, Z. Vivian Feng, Christy L. Haynes, Zeev Rosenzweig
Summary: This study investigates the environmental fate of InSe nanosheets and the impact of EGCG-coated nanosheets on bacterial growth.
ENVIRONMENTAL SCIENCE-NANO
(2023)
Article
Chemistry, Multidisciplinary
Thomas R. Kuech, Nasim Ganji, Caroline Anastasia, Marco D. Torelli, Eric S. Melby, Arielle C. Mensch, Emily R. Caudill, Ralf Zimmermann, Robert J. Hamers, Joel A. Pedersen
Summary: The interactions between cationic polymer-wrapped diamond nanoparticles (PAH-DNPs) and lipid bilayers are influenced by the phospholipid composition and surface charge. Electrostatic attractions and repulsions play key roles in the initial attachment and final extent of nanoparticle adhesion. The formation of a lipid corona on PAH-DNPs reduces the effective charge density and affects the adhesion extent. The inclusion of charged phospholipids decreases the attachment efficiency and extent by reducing the electrostatic attraction between PAH-DNPs and the bilayers.
ENVIRONMENTAL SCIENCE-NANO
(2023)
Article
Chemistry, Multidisciplinary
Christian A. Reardon-Lochbaum, Ravithree D. Senanayake, Rocio Amaro Marquez, Kha Trinh, Khoi Nguyen L. Hoang, Tobias Rangel Guillen, Catherine J. Murphy, Robert J. Hamers, Joel A. Pedersen, Rigoberto Hernandez
Summary: Supported lipid bilayers are commonly used as model systems for studying interactions between biological membranes and proteins or nanoparticles. The choice of substrate material, such as gold or SiO2, influences the interactions and adsorption behavior of anionic nanoparticles and cytochrome c to the bilayers. The underlying substrate material plays a role in determining the extent of interaction between nanoscale analytes and supported lipid bilayers.
ENVIRONMENTAL SCIENCE-NANO
(2023)
Article
Chemistry, Physical
Shuo Li, Luca Francaviglia, Daniel D. Kohler, Zachary R. Jones, Eric T. Zhao, D. Frank Ogletree, Alexander Weber-Bargioni, Nicholas A. Melosh, Robert J. Hamers
Summary: This study investigates highly stable silicon-vacancy (SiV) centers in diamond for sensing and quantum information science. The results show that complete encapsulation of Ag nanospheres with SiV centers in a thin diamond coating leads to hybrid core-shell nanostructures with extraordinary chemical and thermal stability and enhanced optical properties. The stability and optical properties of these Ag-diamond core-shell structures make them promising candidates for high-efficiency imaging and quantum-based sensing applications.