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1. Studies of Dynamic Binding of Amino Acids to TiO2 Nanoparticle Surfaces by Solution NMR and Molecular Dynamics Simulations

   Mengjun Xue, Janani Sampath (July 2020, Langmuir)

   null (Ed.)

   Adsorption of biomolecules onto material surfaces involves a potentially complex mechanism where molecular species interact to varying degrees with a heterogeneous material surface. Surface adsorption studies by atomic force microscopy, sum frequency generation spectroscopy, and solid-state NMR detect the structures and interactions of biomolecular species that are bound to material surfaces, which, in the absence of a solid–liquid interface, do not exchange rapidly between surface-bound forms and free molecular species in bulk solution. Solution NMR has the potential to complement these techniques by detecting and studying transiently bound biomolecules at the liquid–solid interface. Herein, we show that dark-state exchange saturation transfer (DEST) NMR experiments on gel-stabilized TiO2 nanoparticle (NP) samples detect several forms of biomolecular adsorption onto titanium(IV) oxide surfaces. Specifically, we use the DEST approach to study the interaction of amino acids arginine (Arg), lysine (Lys), leucine (Leu), alanine (Ala), and aspartic acid (Asp) with TiO2 rutile NP surfaces. Whereas Leu, Ala, and Asp display only a single weakly interacting form in the presence of TiO2 NPs, Arg and Lys displayed at least two distinct bound forms: a species that is surface bound and retains a degree of reorientational motion and a second more tightly bound form characterized by broadened DEST profiles upon the addition of TiO2 NPs. Molecular dynamics simulations indicate different surface bound states for both Lys and Arg depending on the degree of TiO2 surface hydroxylation but only a single bound state for Asp regardless of the degree of surface hydroxylation, in agreement with results obtained from the analysis of DEST profiles. 

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2. RNA BioMolecular Electronics: towards new tools for biophysics and biomedicine

   https://doi.org/10.1039/D1TB01141C  

   Pattiya Arachchillage, Keshani G.; Chandra, Subrata; Piso, Angela; Qattan, Tiba; Artes Vivancos, Juan M. (September 2021, Journal of Materials Chemistry B)

   The last half-century has witnessed the birth and development of a new multidisciplinary field at the edge between materials science, nanoscience, engineering, and chemistry known as Molecular Electronics. This field deals with the electronic properties of individual molecules and their integration as active components in electronic circuits and has also been applied to biomolecules, leading to BioMolecular Electronics and opening new perspectives for single-molecule biophysics and biomedicine. Herein, we provide a brief introduction and overview of the BioMolecular electronics field, focusing on nucleic acids and potential applications for these measurements. In particular, we review the recent demonstration of the first single-molecule electrical detection of a biologically-relevant nucleic acid. We also show how this could be used to study biomolecular interactions and applications in liquid biopsy for early cancer detection, among others. Finally, we discuss future perspectives and challenges in the applications of this fascinating research field. 

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3. Peptide-based assembled nanostructures that can direct cellular responses

   https://doi.org/10.1088/1748-605X/ac92b5  

   Huang, Haofu; Kiick, Kristi (September 2022, Biomedical Materials)

   Abstract Natural originated materials have been well-studied over the past several decades owing to their higher biocompatibility compared to the traditional polymers. Peptides, consisting of amino acids, are among the most popular programmable building blocks, which is becoming a growing interest in nanobiotechnology. Structures assembled using those biomimetic peptides allow the exploration of chemical sequences beyond those been routinely used in biology. In this review, we discussed the most recent experimental discoveries on the peptide-based assembled nanostructures and their potential application at the cellular level such as drug delivery. In particular, we explored the fundamental principles of peptide self-assembly and the most recent development in improving their interactions with biological systems. We believe that as the fundamental knowledge of the peptide assemblies evolves, the more sophisticated and versatile nanostructures can be built, with promising biomedical applications. 

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4. Smart Materials by Nanoscale Magnetic Assembly

   https://doi.org/10.1002/adfm.201903467  

   Li, Zhiwei; Yang, Fan; Yin, Yadong (July 2019, Advanced Functional Materials)

   Abstract Magnetic assembly at the nanoscale level holds great potential for producing smart materials with high functional and structural diversity. Generally, the chemical, physical, and mechanical properties of the resulting materials can be engineered or dynamically tuned by controlling external magnetic fields. This Review analyzes the recent research progress on nanoscale magnetic assembly approaches toward the development of smart materials. The magnetic interactions between nanoparticles (both magnetic and nonmagnetic) and the interactions between nanoparticles and external magnetic fields are fully expatiated based on numerical simulations. In particular, the advancements of nanoscale magnetic assembly in responsive optical nanostructures, shape‐morphing systems, and advanced materials with tunable surface properties are introduced in three subsections. The key roles of magnetic interactions in nanoscale assembly toward customizable physical and chemical properties are highlighted, with focus on how to enable direct manipulation of the positional and orientational orders of the building blocks and orientational control of soft matrices through the incorporation of anisotropic magnetic structures. 

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5. Surface Segregation and Self‐Assembly of Block‐Copolymer Separation Layers on Top of Homopolymer Substructures in Asymmetric Ultrafiltration Membranes from a Single Casting Step

   https://doi.org/10.1002/adfm.202009387  

   Hibi, Yusuke; Wiesner, Ulrich (May 2021, Advanced Functional Materials)

   Abstract Surface segregation in blended polymer films has attracted much interest in fundamental research as well as for practical applications. A variety of methodologies have been proposed for controlling surface segregation. They often require long annealing times, however, to achieve thermodynamic equilibrium. Here, a strategy and proof‐of‐principle experiments are described to control surface segregation of thin block‐copolymer (BCP) layers on top of a homopolymer in a single casting step from blended BCP/homopolymer solutions. The surface coverage by the minor constituent BCP (2–10 wt%) is accomplished despite almost identical surface energies of BCP and homopolymer constituents. Immersing this casted solution into water for nonsolvent induced phase separation (NIPS), a nonequilibrium process, affords solidified bilayer ultrafiltration membranes composed of a thin porous surface layer of self‐assembled BCP atop an asymmetric porous homopolymer substructure. Key to successful BCP surface segregation is the choice of a binary solvent system based on careful considerations of solvent surface energies and polymer‐solvent interaction parameters. Furthermore, stabilizing the BCP micellar structure by a divalent metal additive is also essential. The approach provides a cost‐effective method for fabricating bilayer‐type asymmetric ultrafiltration membranes with uniform BCP self‐assembly based selective top surface pore layers in a single casting step. 

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