Catalogue Search | MBRL
Search Results Heading
Explore the vast range of titles available.
MBRLSearchResults
-
LanguageLanguage
-
SubjectSubject
-
Item TypeItem Type
-
DisciplineDiscipline
-
YearFrom:-To:
-
More FiltersMore FiltersIs Peer Reviewed
Done
Filters
Reset
65
result(s) for
"Hermans, Thomas M."
Sort by:
Non-equilibrium steady states in supramolecular polymerization
by
Sato, Akihiro
,
Hermans, Thomas M.
,
Leira-Iglesias, Jorge
in
639/638/541/960
,
639/638/541/966
,
Actin
2017
Living systems use fuel-driven supramolecular polymers such as actin to control important cell functions. Fuel molecules like ATP are used to control when and where such polymers should assemble and disassemble. The cell supplies fresh ATP to the cytosol and removes waste products to sustain steady states. Artificial fuel-driven polymers have been developed recently, but keeping them in sustained non-equilibrium steady states (NESS) has proven challenging. Here we show a supramolecular polymer that can be kept in NESS, inside a membrane reactor where ATP is added and waste removed continuously. Assembly and disassembly of our polymer is regulated by phosphorylation and dephosphorylation, respectively. Waste products lead to inhibition, causing the reaction cycle to stop. Inside the membrane reactor, however, waste can be removed leading to long-lived NESS conditions. We anticipate that our approach to obtain NESS can be applied to other stimuli-responsive materials to achieve more life-like behaviour.
Several cell functions are based on the fuel-driven assembly and disassembly of supramolecular polymers under non-equilibrium conditions. Here, the authors show controlled formation and breaking of a supramolecular polymer by enzymatic phosphorylation and dephosphorylation of a building block by continuously adding ATP fuel and removing waste products.
Journal Article
Liquid flow and control without solid walls
2020
When miniaturizing fluidic circuitry, the solid walls of the fluid channels become increasingly important
1
because they limit the flow rates achievable for a given pressure drop, and they are prone to fouling
2
. Approaches for reducing the wall interactions include hydrophobic coatings
3
, liquid-infused porous surfaces
4
–
6
, nanoparticle surfactant jamming
7
, changes to surface electronic structure
8
, electrowetting
9
,
10
, surface tension pinning
11
,
12
and use of atomically flat channels
13
. A better solution may be to avoid the solid walls altogether. Droplet microfluidics and sheath flow achieve this but require continuous flow of the central liquid and the surrounding liquid
1
,
14
. Here we demonstrate an approach in which aqueous liquid channels are surrounded by an immiscible magnetic liquid, both of which are stabilized by a quadrupolar magnetic field. This creates self-healing, non-clogging, anti-fouling and near-frictionless liquid-in-liquid fluidic channels. Manipulation of the field provides flow control, such as valving, splitting, merging and pumping. The latter is achieved by moving permanent magnets that have no physical contact with the liquid channel. We show that this magnetostaltic pumping method can be used to transport whole human blood with very little damage due to shear forces. Haemolysis (rupture of blood cells) is reduced by an order of magnitude compared with traditional peristaltic pumping, in which blood is mechanically squeezed through a plastic tube. Our liquid-in-liquid approach provides new ways to transport delicate liquids, particularly when scaling channels down to the micrometre scale, with no need for high pressures, and could also be used for microfluidic circuitry.
Wall-free liquid channels surrounded by an immiscible magnetic liquid can be used to create liquid circuitry or to transport human blood without damaging the blood cells by moving permanent magnets.
Journal Article
Control of Surface Charges by Radicals as a Principle of Antistatic Polymers Protecting Electronic Circuitry
by
Baytekin, H. Tarik
,
Hermans, Thomas M.
,
Kowalczyk, Bartlomiej
in
Addition polymerization
,
Antistatic Agents - chemistry
,
Applied sciences
2013
Even minute quantities of electric charge accumulating on polymer surfaces can cause shocks, explosions, and multibillion-dollar losses to electronic circuitry. This paper demonstrates that to remove static electricity, it is not at all necessary to \"target\" the charges themselves. Instead, the way to discharge a polymer is to remove radicals from its surface. These radicals colocalize with and stabilize the charges; when they are scavenged, the surfaces discharge rapidly. This radical-charge interplay allows for controlling static electricity by doping common polymers with small amounts of radical-scavenging molecules, including the familiar vitamin E. The effectiveness of this approach is demonstrated by rendering common polymers dust-mitigating and also by using them as coatings that prevent the failure of electronic circuitry.
Journal Article
Oscillations, travelling fronts and patterns in a supramolecular system
by
Leira-Iglesias, Jorge
,
Tassoni, Alessandra
,
Adachi, Takuji
in
Anchoring
,
Chemical fuels
,
Communications systems
2018
Supramolecular polymers, such as microtubules, operate under non-equilibrium conditions to drive crucial functions in cells, such as motility, division and organelle transport1. In vivo and in vitro size oscillations of individual microtubules2,3 (dynamic instabilities) and collective oscillations4 have been observed. In addition, dynamic spatial structures, like waves and polygons, can form in non-stirred systems5. Here we describe an artificial supramolecular polymer made of a perylene diimide derivative that displays oscillations, travelling fronts and centimetre-scale self-organized patterns when pushed far from equilibrium by chemical fuels. Oscillations arise from a positive feedback due to nucleation–elongation–fragmentation, and a negative feedback due to size-dependent depolymerization. Travelling fronts and patterns form due to self-assembly induced density differences that cause system-wide convection. In our system, the species responsible for the nonlinear dynamics and those that self-assemble are one and the same. In contrast, other reported oscillating assemblies formed by vesicles6, micelles7 or particles8 rely on the combination of a known chemical oscillator and a stimuli-responsive system, either by communication through the solvent (for example, by changing pH7–9), or by anchoring one of the species covalently (for example, a Belousov–Zhabotinsky catalyst6,10). The design of self-oscillating supramolecular polymers and large-scale dissipative structures brings us closer to the creation of more life-like materials11 that respond to external stimuli similarly to living cells, or to creating artificial autonomous chemical robots12.
Journal Article
Vortex flows impart chirality-specific lift forces
by
Hermans, Thomas M.
,
Grzybowski, Bartosz A.
,
Davis, Stephen H.
in
639/766/189
,
639/766/1960
,
catalysis (homogeneous), solar (photovoltaic), bio-inspired, charge transport, mesostructured materials, materials and chemistry by design, synthesis (novel materials), synthesis (self-assembly)
2015
Recent reports that macroscopic vortex flows can discriminate between chiral molecules or their assemblies sparked considerable scientific interest both for their implications to separations technologies and for their relevance to the origins of biological homochirality. However, these earlier results are inconclusive due to questions arising from instrumental artifacts and/or insufficient experimental control. After a decade of controversy, the question remains unresolved—how do vortex flows interact with different stereoisomers? Here, we implement a model experimental system to show that chiral objects in a Taylor–Couette cell experience a chirality-specific lift force. This force is directed parallel to the shear plane in contrast to previous studies in which helices, bacteria and chiral cubes experience chirality-specific forces perpendicular to the shear plane. We present a quantitative hydrodynamic model that explains how chirality-specific motions arise in non-linear shear flows through the interplay between the shear-induced rotation of the particle and its orbital translation. The scaling laws derived here suggest that rotating flows can be used to achieve chiral separation at the micro- and nanoscales.
The separation of enantiomers by flows holds promise in food and pharmaceutical industries, but the feasibility remains uncertain. Here, Hermans
et al.
separate macroscopic particles of opposite chirality at a liquid interface using shear flows, which provides insights into the mechanism at nanoscale.
Journal Article
Ultrasensitive detection of toxic cations through changes in the tunnelling current across films of striped nanoparticles
by
Hermans, Thomas M.
,
Patashinski, Alexander Z.
,
Glotzer, Sharon C.
in
639/301/1005/1009
,
639/301/357/354
,
Biomaterials
2012
Although multiple methods have been developed to detect metal cations, only a few offer sensitivities below 1 pM, and many require complicated procedures and sophisticated equipment. Here, we describe a class of simple solid-state sensors for the ultrasensitive detection of heavy-metal cations (notably, an unprecedented attomolar limit for the detection of CH
3
Hg
+
in both standardized solutions and environmental samples) through changes in the tunnelling current across films of nanoparticles (NPs) protected with striped monolayers of organic ligands. The sensors are also highly selective because of the ligand–shell organization of the NPs. On binding of metal cations, the electronic structure of the molecular bridges between proximal NPs changes, the tunnelling current increases and highly conductive paths ultimately percolate the entire film. The nanoscale heterogeneity of the structure of the film broadens the range of the cation-binding constants, which leads to wide sensitivity ranges (remarkably, over 18 orders of magnitude in CH
3
Hg
+
concentration).
Solid-state sensors for the detection of heavy-metal cations require for the most part sophisticated chemistry and equipment. It is now shown that toxic cations in environmental samples can be detected with ultrahigh sensitivity and over a broad range of cation concentrations by measuring the tunnelling current across films of nanoparticles decorated with striped monolayers of organic ligands.
Journal Article
Suppressing Interfacial Instability of Immiscible Liquid‐in‐Liquid Flow Using Magnetic Forces
2025
Interfacial instability prevents a liquid jet from flowing indefinitely within air or another liquid. An approach is presented here to suppress interfacial instability by means of a magnetic force applied by a ferrofluid envelope around the jet. The stability limits occurring within a large parameter window are experimentally investigated with length and time scales governed by the magnetic Bond number. Instabilities can be generated by modifying the magnetic force strength externally, with a remarkable return to stability when removing the external stimulus. The current system with soft and slippery interfaces enables investigations of flow systems beyond the limits of standard hydrodynamics allowing for exciting applications in flow chemistry, interface engineering and transport of biological materials.
Journal Article
Droplets Out of Equilibrium
by
Hermans, Thomas M.
,
Stellacci, Francesco
,
Frauenrath, Holger
in
Accessibility
,
Biomaterials
,
Dissipation
2013
Magnetic droplets can be switched between static and dynamic structures.
[Also see Report by
Timonen
et al.
]
Living systems create structures and functions of remarkable complexity by mastering self-assembly in different equilibrium and nonequilibrium states. Three states can be distinguished: equilibrium, nondissipative nonequilibrium (or kinetically trapped), and dissipative (or dynamic) nonequilibrium. On page 253 of this issue, Timonen
et al.
(
1
) report on a model system in which all three states are accessible (see the figure) and show how this leads to a range of well-ordered structures.
Journal Article
Self-assembly of soft nanoparticles with tunable patchiness
by
Hermans, Thomas M.
,
Fytas, George
,
Gomopoulos, Nikos
in
Aqueous solutions
,
Binding sites
,
Chemistry and Materials Science
2009
Details of the forces between nanoparticles determine the ways in which the nanoparticles can self-assemble into larger structures. The use of directed interactions has led to new concepts in self-assembly such as asymmetric dendrons
1
,
2
, Janus particles
3
, patchy colloids
4
,
5
,
6
and colloidal molecules
7
. Recent models that include attractive regions or ‘patches’ on the surface of the nanoparticles predict a wealth of intricate modes of assembly
8
,
9
,
10
,
11
,
12
. Interactions between such particles are also important in a range of phenomena including protein aggregation
13
,
14
and crystallization
15
, re-entrant phase transitions
16
,
17
,
18
, assembly of nanoemulsions
19
and the organization of nanoparticles into nanowires
20
. Here, we report the synthesis of 6-nm nanoparticles with dynamic hydrophobic patches and show that they can form reversible self-assembled structures in aqueous solution that become topologically more connected upon dilution. The organization is based on guest–host supramolecular chemistry with the nanoparticles composed of a hydrophobic dendrimer host molecule and water-soluble hydrophilic guest molecules. The work demonstrates that subtle changes in hierarchal composition and/or concentration can dramatically change mesoscopic ordering.
Nanoparticles with dynamic patches can form reversible self-assembled structures in aqueous solution that become topologically more connected on dilution.
Journal Article