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C.P. Duif

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15 records found

Journal article (2026) - Eleonora Olsmats, Adrian R. Rennie, Jeroen Plomp, Michel Thijs, Coen Fransen, Chris Duif, Wim Bouwman
Hypothesis: Pea proteins can act not only as interfacial stabilizers of oil-in-water emulsions but also as gelling agents in the continuous phase. Protein gelation, rather than droplet jamming, may be the main mechanism of emulsion stability, providing a physical explanation for the creaminess of high-protein plant-based emulsions. Experimental: Spin-echo small angle neutron scattering (SESANS) with D2O/H2O contrast variation was used to study 15% pea protein dispersions and emulsions with 40–60% rapeseed oil, 7.5% protein at pH 3 to 6.5. SESANS investigates length scales up to tens of micrometres, enabling simultaneous analysis of protein networks and oil droplets without dilution. Complementary small angle X-ray/neutron scattering were used to validate protein aggregate size, and hydration. Findings: Protein dispersions at neutral pH formed mass fractal networks with small individual building blocks (radius ∼38 Å, hydration ∼70%). Emulsions consisted of oil droplets embedded in these networks, with droplet radii decreasing at higher oil fractions due to an effective higher protein concentration in the continuous phase, creating a denser network. Dispersions and emulsions at lower pH contained aggregated clusters of denatured proteins. These coarse and inhomogeneous networks gave increasing droplet radii at lower pH. Contrast variation enabled the separation of protein and oil droplet scattering, demonstrating that protein gelation rather than droplet jamming is the main mechanism of stability. This gives a physical explanation of the high viscosity of high-protein plant-based emulsions and is promising for these plant materials to be used as gelling agents in food applications. ...
Journal article (2025) - Fumiaki Funama, Gregory N. Smith, Steven R. Parnell, Chris P. Duif, Wim G. Bouwman, Roger Pynn, Robert M. Dalgliesh, Fankang Li
Spin-echo small-angle neutron scattering (SESANS) is a unique method to measure structures of materials in real space with length scales from ∼ 30 μm to ∼20 µm [1]. As shown in Figure 1, the accessible length scale of SESANS is given by its ability to encode the momentum transfer into the Larmor phase, namely Φ = →δ . →Q, where →Q is the momentum transfer and →δ is the encoding vector of the setup and its projection along Q (δQ) is called spin-echo length (SEL). [...] ...

Influence of particle properties on network formation

Journal article (2025) - Annika Feichtinger, Ahmed Jarray, Wim G. Bouwman, Chris P. Duif, Maria C. Valverde-Ayllon, Karlijn Heerkens, Renee Rooijakkers, Jasper Landman, Elke Scholten
Capillary suspensions are unique materials, in which the rheological properties can be tuned by controlling the particle network through capillary interactions. To gain insights into the influence of particle properties on the network formation and accompanying gel strength for water-absorbing, biopolymeric particles, protein particles of two different sizes and water absorption capacities (WACs) were prepared. Utilizing SESANS, we describe a novel approach towards detecting changes in water distribution between and within particles. While effects of WAC seemed to be overpowered by concurrent variations in surface roughness, a larger particle size or lower roughness led to a lower initial gel strength and a subsequent much larger relative increase in gel strength upon water addition. Even though similar maximum gel strengths were obtained, indicating that particle properties had a comparably small influence once capillary forces dominated the systems, particle size played a critical role for network collapse with increasing particle clustering at larger water volumes. The results pinpoint subsequent knowledge gaps in the existing literature and demonstrate the tunability of biopolymer-based capillary suspensions over a wide gel strength range by adjustment of particle properties. These insights offer exciting opportunities for application of capillary-force controlled systems in the food, pharmaceutical and cosmetic industries. ...
Journal article (2024) - L.V. Tiihonen, M.P. Weir, A.J. Parnell, S.C. Boothroyd, D.W. Johnson, M. Bleuel, C.P. Duif, W.G. Bouwman, S.R. Parnell, More authors...
We have used spin-echo small-angle neutron scattering (SESANS) to probe the hierarchy of structures present in polymer–carbon nanocomposites, with length scales spanning over three orders of magnitude, from 10 nm to 16 μm. The data processing and reduction show a unified approach across two SESANS instruments (TU Delft and Larmor at the ISIS neutron source) and yield consistent data that are able to be modelled using well-established hierarchical models in freely available software such as SasView. Using this approach, we are able to extend the measured length scales by over an order of magnitude compared to traditional scattering methods. This yields information about the structure in the bulk that is inaccessible with conventional scattering techniques (SANS/SAXS) and points to a way for interrogating and investigating polymer nanocomposites routinely across multiple length scales. ...
Journal article (2023) - E.G. Iashina, W.G. Bouwman, C.P. Duif, Robert M. Dalgliesh, Elena Y. Varfolomeeva, Rimma A. Pantina, Roman A. Kovalev, Natalia D. Fedorova, S. V. Grigoriev
The organization of chromatin in the nuclei of rat lymphocyte was studied by time-of-flight spin-echo small-angle neutron scattering (ToF-SESANS). The procedures of the measurements in ToF and monochromatic SESANS modes were compared. It is shown that the sensitivity of the ToF method is significantly higher than that of the monochromatic mode. As a result, the SESANS correlation function can always be extracted from the ToF measurement of polarization, while this is not always the case with the monochromatic mode. The applicability of SESANS to fractal objects at the micrometre scale is demonstrated. The SESANS correlation function is well fitted by the exponential decay G(z) = exp(−z/ξ) with the correlation length ξ = 3.7 ± 0.1 µm. The exponential decay of the SESANS correlation function can be connected to the logarithmic correlation function γ(r) = ln(r/ξ) and the cubic law of the scattering intensity I(Q) = Q−3, which is in agreement with the concept of scattering from fractal objects. This finding is interpreted as evidence of a very specific logarithmic fractal structure of the large-scale organization of chromatin. The model of the logarithmic fractal is visualized as a hierarchical object obeying the volume-conservation principle at different scales. ...
Journal article (2022) - Mary O'Kane, Joel Smith, Rachel C. Kilbride, Emma L.K. Spooner, C.P. Duif, Thomas E. Catley, Adam Washington, Stephen M. King, S.R. Parnell, Andrew J. Parnell
Tailoring the solution chemistry of metal halide perovskites requires a detailed understanding of precursor aggregation and coordination. In this work, we use various scattering techniques, including dynamic light scattering (DLS), small angle neutron scattering (SANS), and spin-echo SANS (SESANS) to probe the nanostructures from 1 nm to 10 μm within two different lead-halide perovskite solution inks (MAPbI 3and a triple-cation mixed-halide perovskite). We find that DLS can misrepresent the size distribution of the colloidal dispersion and use SANS/SESANS to confirm that these perovskite solutions are mostly comprised of 1-2 nm-sized particles. We further conclude that if there are larger colloids present, their concentration must be <0.005% of the total dispersion volume. With SANS, we apply a simple fitting model for two component microemulsions (Teubner-Strey), demonstrating this as a potential method to investigate the structure, chemical composition, and colloidal stability of perovskite solutions, and we here show that MAPbI 3solutions age more drastically than triple cation solutions. ...
Journal article (2021) - Gregory N. Smith, Erik Brok, Martin Schmiele, Kell Mortensen, Wim G. Bouwman, Chris P. Duif, Tue Hassenkam, Martin Alm, Peter Thomsen, Lise Arleth
By introducing hydrophilic polymers into silicone medical devices, highly beneficial biomedical properties can be realized. An established solution to introduce hydrophilic polymers is to form an interpenetrating polymer network (IPN) by performing the hydrogel synthesis in the presence of silicone swollen in supercritical carbon dioxide. The precise distribution of the two polymers is not known, and determining this is the goal of this study. Neutron scattering and microscopy were used to determine the distribution of the hydrophilic guest polymer. Atomic force microscopy revealed that the important length scale on the surface of these materials is 10–100 nm, and spin-echo small-angle neutron scattering (SESANS) on IPNs submerged in D2O revealed structures of the same scale within the interior and enabled quantification of their size. SESANS with hydration by D2O proved to be the only scattering technique that could determine the structure of the bulk of these types of materials, and it should be used as an important tool for characterizing polymer medical devices. ...
Journal article (2020) - Julien Schmitt, Jan Joost Zeeuw, Jan Joost Zeeuw, Jeroen Plomp, Wim G. Bouwman, Adam L. Washington, Chris P. Duif, Michel A. Thijs, Steven R. Parnell, More Authors...
The initial formation stages of surfactant-templated silica thin films which grow at the air-water interface were studied using combined spin-echo modulated small-angle neutron scattering (SEMSANS) and small-angle neutron scattering (SANS). The films are formed from either a cationic surfactant or nonionic surfactant (C16EO8) in a dilute acidic solution by the addition of tetramethoxysilane. Previous work has suggested a two stage formation mechanism with mesostructured particle formation in the bulk solution driving film formation at the solution surface. From the SEMSANS data, it is possible to pinpoint accurately the time associated with the formation of large particles in solution that go on to form the film and to show their emergence is concomitant with the appearance of Bragg peaks in the SANS pattern, associated with the two-dimensional hexagonal order. The combination of SANS and SEMSANS allows a complete depiction of the steps of the synthesis that occur in the subphase. ...
Journal article (2019) - Ekaterina G. Iashina, Mikhail V. Filatov, Rimma A. Pantina, Elena Y. Varfolomeeva, Wim G. Bouwman, Chris P. Duif, Dirk Honecker, Vitaliy Pipich, Sergey V. Grigoriev
This paper reports on the two-scale fractal structure of chromatin organization in the nucleus of the HeLa cell. Two neutron scattering methods, small-angle neutron scattering (SANS) and spin-echo SANS, are used to unambiguously identify the large-scale structure as being a logarithmic fractal with the correlation function (r) - ln(r/E). The smaller-scale structural level is shown to be a volume fractal with dimension DF = 2.41. By definition, the volume fractal is self-similar at different scales, while the logarithmic fractal is hierarchically changed upon scaling. As a result, the logarithmic fractal is more compact than the volume fractal but still has a rather high surface area, which provides accessibility at all length scales. Apparently such bi-fractal chromatin organization is the result of an evolutionary process of optimizing the compactness and accessibility of gene packing. As they are in a water solution, the HeLa nuclei tend to agglomerate over time. The large-scale logarithmic fractal structure of chromatin provides the HeLa nucleus with the possibility of penetrating deeply into the adjacent nucleus during the agglomeration process. The interpenetration phenomenon of the HeLa nuclei shows that the chromatin-free space of one nucleus is not negligible but is as large as the volume occupied by chromatin itself. It is speculated that it is the logarithmic fractal architecture of chromatin that provides a comfortable compartment for this most important function of the cell. ...
Journal article (2019) - Hugo Gaspar, Raquel Santos, Paulo Teixeira, Loic Hilliou, Michael P. Weir, Chris P. Duif, Wim G. Bouwman, Steven R. Parnell, Stephen M. King, More authors...
We investigate the morphological development of polystyrene (PS)-C 60 nanocomposites along the length of a prototype co-rotating twin-screw extruder with sampling capabilities. The effects of C 60 concentration and output on the morphological evolution along the extruder are studied employing a suite of characterization techniques covering a wide range of length-scales, thereby shedding new light on the dispersion mechanism in this model system. We show that the relatively new spin-echo small-angle neutron scattering (SESANS) technique is well suited to probe both the distribution and the dispersion of C 60 . SESANS complements optical microscopy (OM) data as it covers sampling areas several orders of magnitude larger than OM. The multi-scale morphological information conveyed by OM, SESANS, SANS and rheological data shows that for larger outputs, C 60 agglomerates are eroded as they travel along the extruder, resulting in C 60 dispersion and distribution at both molecular and micrometric levels. The picture is more complex when smaller feed rates are used, as the evolution of C 60 dispersion depends on the C 60 loading. For larger C 60 contents, agglomeration develops along the extruder, whereas dispersion is improved for smaller C 60 contents. Overall, it is concluded that an over-high feed rate in extrusion does not necessarily result in a bigger size of the nanoparticle agglomerates because of the complex interplay between stresses and residence time. ...
Journal article (2018) - R.P. Harti, J. Valsecchi, P. Trtik, D. Mannes, C. Carminati, Markus Strobl, Jeroen Plomp, Chris Duif, Christian Grünzweig
Structural properties of cohesive powders are dominated by their microstructural composition. Powders with a fractal microstructure show particularly interesting properties during compaction where a microstructural transition and a fractal breakdown happen before compaction and force transport. The study of this phenomenon has been challenging due to its long-range effect and the subsequent necessity to characterize these microstructural changes on a macroscopic scale. For the detailed investigation of the complex nature of powder compaction for various densification states along with the heterogeneous breakdown of the fractal microstructure we applied neutron dark-field imaging in combination with a variety of supporting techniques with various spatial resolutions, field-of-views and information depths. We used scanning electron microscopy to image the surface microstructure in a small field-of-view and X-ray tomography to image density variations in 3D with lower spatial resolution. Non-local spin-echo small-angle neutron scattering results are used to evaluate fitting models later used as input parameters for the neutron dark-field imaging data analysis. Finally, neutron dark-field imaging results in combination with supporting measurements using scanning electron microscopy, X-ray tomography and spin-echo small angle scattering allowed us to comprehensively study the heterogeneous transition from a fractal to a homogeneous microstructure of a cohesive powder in a quantitative manner. ...
Journal article (2017) - E.G. Iashina, W. G. Bouwman, C. P. Duif, M.V. Filatov, S. V. Grigoriev
Spin-echo small-angle scattering (SESANS) technique is a method to measure the structure of materials from nano- to micrmeter length scales. This method could be important for studying the packaging of DNA in the eukaryotic cell. We measured the SESANS function from chicken erythrocyte nuclei which is well fitted by the exponential function G(z) = exp(-z/ξ), where ξ is the correlation length of a nucleus (in experimental data ξ = 3, 3 μm). The exponential decay of G(z) corresponds to the logarithmic pair correlation function γ(r) = ln(ξ/r). As the sensitivity of the SESANS signal depends on the neutron wavelength, we propose the SESANS setup with the changeable wavelength in the range from 2 to 12 Å. Such option allows one to study in great detail the internal structure of the biological cell in the length scale from 10-2 μm to 10 μm. ...
Journal article (2017) - Evgenii Velichko, A.L. Buyanov, N.N. Saprykina, Yu.O. Chetverikov, Chris Duif, Wim Bouwman, R.Yu. Smyslov
Submicron- and micron-scale structures of composite hydrogels based on bacterial cellulose (BC) and polyacrylamide (PAAm) were studied by spin-echo small-angle neutron scattering (SESANS) and cryo-scanning electron microscopy (cryo-SEM). These hydrogels possessing the structure of interpenetrating polymer network were synthesized via free-radical polymerization of acrylamide carried out in the pellicle of BC swollen in the reaction solution. No neutron scattering was observed for the samples swollen in heavy water to the equilibrium state, but the SESANS signal appeared when TbCl3 salt was added to the solvent. It is the unusual effect, which may be very helpful for SESANS studying of other hydrogel systems. The SESANS dependences obtained for these samples revealed the anisotropy of mesostructure for the hydrogels under investigation. Density inhomogeneities on the characteristic scale of 11.5 ± 0.5 μm were detected in one fixed orientation of the sample, i.e., with the growth plane of BC parallel to the plane formed by the neutron beam and the spin-echo length. The uniaxial anisotropy revealed agrees with a recently proposed model, which attributes this behavior to the existence of tunnel-like oriented structures inside BC. The evidence of such type of mesostructure anisotropy of BC and BC-PAAm hydrogels was obtained by using the cryo-SEM method. ...
Journal article (2017) - K. A. Pavlov, E. V. Velichko, V. N. Zabenkin, W. H. Kraan, C. P. Duif, W. G. Bouwman, Z. A. Mikhailovskaya, E. S. Buyanova, S. V. Grigoriev
The closed porous structure in ceramic materials is investigated by spin-echo small-angle neutron scattering. A series of ceramic samples of oxygen–ion conductors based on bismuth molybdate with the general formula Bi12.8X0.2Mo5O34 ± δ (X = Mg, Ba, Ca, Sr) is obtained by powder sintering for 6−45 h at a temperature close to the melting point. The samples are characterized by scanning electron microscopy and X-ray fluorescence analysis. It is found that they had a stoichiometric chemical composition, are singlephase, and contain clean pores between crystal grains. The pore size is determined by spin-echo small-angle neutron scattering and ranges from 2.2 to 3.5 μm. It is demonstrated that longer sintering times correspond to larger pores (the increase in their average diameter is as large as 30%). It is found that the studied materials lack a fractal pore structure. ...
Journal article (2017) - E.G. Iashina, Evgenii Velichko, M.V. Filatov, Wim Bouwman, Chris Duif, A. Brulet, S. V. Grigoriev
Small-angle neutron scattering (SANS) on nuclei of chicken erythrocytes demonstrates the cubic dependence of the scattering intensity Q−3 in the range of momentum transfer Q∈10−3–10−2nm−1. Independent spin-echo SANS measurements give the spin-echo function, which is well described by the exponential law in a range of sizes (3×102)–(3×104) nm. Both experimental dependences reflect the nature of the structural organization of chromatin in the nucleus of a living cell, which corresponds to the correlation function γ(r)=ln(ξ/r) for r<ξ, where ξ=(3.69±0.07)×103 nm, the size of the nucleus. It has the specific scaling property of the logarithmic fractal γ(r/a)=γ(r)+ln(a), i.e., the scaling down by a gives an additive constant to the correlation function, which distinguishes it from the mass fractal, which is characterized by multiplicative constant. ...