Nonequilibrium Uptake Kinetics of Molecular Cargo into Hollow Hydrogels Tuned by Electrosteric Interactions

Moncho-Jordá, A.; Germán-Bellod, Alicia; Angioletti‐Uberti, Stefano; Adroher‐Benítez, Irene; Dzubiella, Joachim

doi:10.1021/acsnano.8b07609

Cited by 22 publications

(28 citation statements)

References 79 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…19) to include the cooperative effect more completely to consistently describe the total binding equilibrium. Similar models, additionally including Born self-energy terms and dipolar contributions, albeit neglecting the G b term, were devised for proteins binding to hydrogels in equilibrium [51,67] as well as for protein sorption kinetics to core-shell hydrogels [68] and molecular cargo to hollow hydrogels [69].…”

Section: Electrostatic Excess Contributions and Cooperativitymentioning

confidence: 99%

Probing the protein corona around charged macromolecules: interpretation of isothermal titration calorimetry by binding models and computer simulations

Dzubiella

2020

Colloid Polym Sci

Self Cite

View full text Add to dashboard Cite

Isothermal titration calorimetry (ITC) is a widely used tool to experimentally probe the heat signal of the formation of the protein corona around macromolecules or nanoparticles. If an appropriate binding model is applied to the ITC data, the heat of binding and the binding stoichiometry as well as the binding affinity per protein can be quantified and interpreted. However, the binding of the protein to the macromolecule is governed by complex microscopic interactions. In particular, due to the steric and electrostatic protein–protein interactions within the corona as well as cooperative, charge renormalization effects of the total complex, the application of standard (e.g., Langmuir) binding models is questionable and the development of more appropriate binding models is very challenging. Here, we discuss recent developments in the interpretation of the Langmuir model applied to ITC data of protein corona formation, exemplified for the well-defined case of lysozyme coating highly charged dendritic polyglycerol sulfate (dPGS), and demonstrate that meaningful data can be extracted from the fits if properly analyzed. As we show, this is particular useful for the interpretation of ITC data by molecular computer simulations where binding affinities can be calculated but it is often not clear how to consistently compare them with the ITC data. Moreover, we discuss the connection of Langmuir models to continuum binding models (where no discrete binding sites have to be assumed) and their possible extensions toward the inclusion of leading order cooperative electrostatic effects.

show abstract

Section: Electrostatic Excess Contributions and Cooperativitymentioning

confidence: 99%

Probing the protein corona around charged macromolecules: interpretation of isothermal titration calorimetry by binding models and computer simulations

Dzubiella

2020

Colloid Polym Sci

Self Cite

View full text Add to dashboard Cite

show abstract

“…Observations 49 show that distribution of polymer chains in the reference state of a microgel is uniform except for thin layers near the surfaces R = R 1 and R = R 2 . To reduce the number of adjustable parameters, we disregard this inhomogeneity and treat the degree of swelling in the reference state Q 0 as a quantity independent of spatial coordinates.…”

Section: Modelmentioning

confidence: 99%

Equilibrium swelling of thermo‐responsive core‐shell microgels

Drozdov

Christiansen

2020

J of Applied Polymer Sci

View full text Add to dashboard Cite

Design of new routes for preparation of hydrogels with fast response and enhanced mechanical and physical properties requires adequate modeling of their swelling. A model is developed for the equilibrium swelling of thermo‐responsive gels. A characteristic feature of the model is that it accounts for a strong increase in the elastic moduli above the volume phase transition temperature Tc driven by aggregation of hydrophobic segments into clusters that serve as extra physical bonds between chains. The model is applied to the analysis of swelling diagrams on poly(N‐isopropylacrylamide) macroscopic gels, microgel latices, and core‐shell microgels with rigid cores. Good agreement is shown between the experimental data and results of simulation. It is demonstrated that the elastic moduli of microgels are higher, while their degrees of swelling in the stress‐free state are lower compared with those of macroscopic gels.

show abstract

“…Dzubiella et al (2003) have formulated the DDFT concept based on the mean-field (quadratic in density) free energy functional. DDFT has been used to describe protein adsorption on polymer-coated nanoparticles (Angioletti-Uberti et al, 2014 and the uptake kinetics of molecular cargo into hollow hydrogels (Moncho-Jorda et al, 2019). DDFT has been applied to lane formation in oppositely driven binary mixtures (Chakrabarti et al, 2003(Chakrabarti et al, , 2004.…”

Section: H Approximate Free Energy Functionalsmentioning

confidence: 99%

“…A time-dependent version of classical DFT or "dynamical DFT" was proposed by Evans (1979) and later much advocated by Marconi and Tarazona (1999) and by Archer and Evans (2004). Selected examples of insightful dynamical DFT studies include the uptake kinetics of molecular cargo into hollow hydrogels (Moncho-Jorda et al, 2019), the particle-scale resolved non-equilibrium sedimentation of colloids (Royall et al, 2007), the bulk dynamics of colloidal Brownian hard disks (Stopper et al, 2018), the pair dynamics in inhomogeneous liquids and glasses (Archer et al, 2007;Hopkins et al, 2010), and the growth of monolayers of hard rods on planar substrates (Klopotek et al, 2017). The dynamical DFT can be viewed as being based on the approximation that the nonequilibrium dynamics are represented as a sequence of "adiabatic states" that each are taken to be in equilibrium.…”

Section: Introduction a Soft Matter Dynamicsmentioning

confidence: 99%

Power functional theory for Newtonian many-body dynamics

Schmidt

2018

The Journal of Chemical Physics

View full text Add to dashboard Cite

We construct a variational theory for the inertial dynamics of classical many-body systems out of equilibrium. The governing (power rate) functional depends on three time- and space-dependent one-body distributions, namely, the density, the particle current, and the time derivative of the particle current. The functional is minimized by the true time derivative of the current. Together with the continuity equation, the corresponding Euler-Lagrange equation uniquely determines the time evolution of the system. An adiabatic approximation introduces both the free energy functional and the Brownian free power functional, as is relevant for liquids governed by molecular dynamics at constant temperature. The forces beyond the Brownian power functional are generated from a superpower (above the overdamped Brownian) functional.

show abstract

Nonequilibrium Uptake Kinetics of Molecular Cargo into Hollow Hydrogels Tuned by Electrosteric Interactions

Cited by 22 publications

References 79 publications

Probing the protein corona around charged macromolecules: interpretation of isothermal titration calorimetry by binding models and computer simulations

Probing the protein corona around charged macromolecules: interpretation of isothermal titration calorimetry by binding models and computer simulations

Equilibrium swelling of thermo‐responsive core‐shell microgels

Power functional theory for Newtonian many-body dynamics

Contact Info

Product

Resources

About