@misc{song_corrosion_inhibition_2024, author={Song, C., Wang, C., Mercier, D., Vaghenfinazari, B., Seyeux, A., Snihirova, D., Wieland, F.D.C., Marcus, P., Zheludkevich, M.L., Lamaka, S.V.}, title={Corrosion inhibition mechanism of 2,6-pyridinedicarboxylate depending on magnesium surface treatment}, year={2024}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.corsci.2024.111867}, abstract = {2,6-pyridinedicarboxylate (2,6-PDC) was studied as corrosion inhibitor for pure magnesium. The surface was prepared either by polishing or polishing followed by treatment with 1 M NaOH solution. The results show that 2,6-PDC promotes the formation of a denser protective oxide/hydroxide layer poor in PDC. The mechanism proposed includes forming weak PDC-Mg complexes that lower the free Mg2+ concentration available for the formation of Mg(OH)2. This leads to growth of smaller Mg(OH)2 platelets that are more densely packed and hence form a more protective layer. The highest inhibition efficiency of 2,6-PDC was achieved for samples with surface hydroxylated by NaOH treatment.}, note = {Online available at: \url{https://doi.org/10.1016/j.corsci.2024.111867} (DOI). Song, C.; Wang, C.; Mercier, D.; Vaghenfinazari, B.; Seyeux, A.; Snihirova, D.; Wieland, F.; Marcus, P.; Zheludkevich, M.; Lamaka, S.: Corrosion inhibition mechanism of 2,6-pyridinedicarboxylate depending on magnesium surface treatment. Corrosion Science. 2024. vol. 229, 111867. DOI: 10.1016/j.corsci.2024.111867}} @misc{yeshmanova_effect_of_2024, author={Yeshmanova, G., Blawert, C., Serdechnova, M., Wieland, F.D.C., Starykevich, M., Gazenbiller, E., Höche, D., Smagulov, D., Zheludkevich, M.L.}, title={Effect of electrolyte composition on the formation of PEO coatings on AA2024 aluminium alloy}, year={2024}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.surfin.2023.103797}, abstract = {Since the electrolyte composition plays a crucial role in the plasma electrolytic oxidation (PEO) coating formation process, a systematic and in-depth study was proposed to identify an electrolyte composition for fast PEO coating growth on AA2024 alloy. Different concentration ratios of mixed alkaline electrolytes (hydroxide, silicate and phosphate) were investigated. PEO process was conducted at low constant current density of 50 mA/cm2, which is intended for lowering the energy consumption. Results demonstrated that the breakdown voltage of PEO coatings is directly proportional to the logarithm of electrolyte resistivity. The coating growth mechanism showed two main directions. The thickening of the coating mainly depends on the rapid deposition of electrolyte compounds in Si-based electrolyte, and the coating growth occurs mainly towards the electrolyte/coating interface. Contrary, in OH-, and P-based electrolytes, the inward coating growth was dominating mainly by substrate oxidation. A variety of phases as a function of different electrolyte compositions and final voltages were observed. With high final voltages (over 470 V) for coatings produced in mixed electrolytes with low concentrations of hydroxide, silicate or phosphate (2 and 6 g/L), γ-Al2O3 crystalline phase predominates in the PEO layer composition. However, only a low efficiency of coating growth can be reached. In the electrolytes with high silicate concentrations accompanied by an increase of phosphate concentration, the final voltage is around 455 V and the coating composition is dominated by an amorphous phase in combination with crystalline mullite and γ-Al2O3. High silicate-phosphate contents (18–24 g/L) in mixed electrolytes with low final voltages of about 360 V results in a fully amorphous PEO layer and significantly increases coating thickness. A combination of low content of hydroxide, high silicate with increasing content of phosphate in mixed electrolyte increases the coating thickness, and improves the density and uniformity of the overall PEO layers.}, note = {Online available at: \url{https://doi.org/10.1016/j.surfin.2023.103797} (DOI). Yeshmanova, G.; Blawert, C.; Serdechnova, M.; Wieland, F.; Starykevich, M.; Gazenbiller, E.; Höche, D.; Smagulov, D.; Zheludkevich, M.: Effect of electrolyte composition on the formation of PEO coatings on AA2024 aluminium alloy. Surfaces and Interfaces. 2024. vol. 44, 103797. DOI: 10.1016/j.surfin.2023.103797}} @misc{kasneryk_controllable_recrystallization_2024, author={Kasneryk, V., Wu, T., Rohr, H., Serdechnova, M., Mojsilovi , K., Wieland, F.D.C., Davydok, A., Gazenbiller, E., Vasili , R., Blawert, C., Stock, N., Zheludkevich, M.L.}, title={Controllable recrystallization of ZnO/ZnAl2O4 based PEO into ZIF-8 as a route for the formation of multifunctional coatings}, year={2024}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.jiec.2023.11.033}, abstract = {Nowadays, plasma electrolytic oxidation (PEO) has become widespread as an effective method for preparation of multifunctional coatings. However, the PEO coatings have numerous pores. On the one hand, their presence restricts their broad application; on the other hand, they represent an excellent platform for post-sealing allowing creating coatings with peculiar properties. In the current work, the possibility of controllable recrystallization of ZnO/ZnAl2O4 based PEO preformed on Zn Z1 alloy into ZIF-8@PEO composite coating was demonstrated for the first time. It was found that the corrosion protection, photocatalytic and photoluminescence properties of the final coatings can be modified by varying the conditions of the post-modification process, which include the amount of the organic linker (2-methylimidazole) and treatment time. This study opens an innovative approach for the formation of multifunctional coatings.}, note = {Online available at: \url{https://doi.org/10.1016/j.jiec.2023.11.033} (DOI). Kasneryk, V.; Wu, T.; Rohr, H.; Serdechnova, M.; Mojsilovi, K.; Wieland, F.; Davydok, A.; Gazenbiller, E.; Vasili, R.; Blawert, C.; Stock, N.; Zheludkevich, M.: Controllable recrystallization of ZnO/ZnAl2O4 based PEO into ZIF-8 as a route for the formation of multifunctional coatings. Journal of Industrial and Engineering Chemistry. 2024. vol. 263, 119538. DOI: 10.1016/j.jiec.2023.11.033}} @misc{sefa_multiscale_morphological_2023, author={Sefa, S., Espiritu, J., Ćwieka, H., Greving, I., Flenner, S., Will, O., Beuer, S., Wieland, D.C.F., Willumeit-Römer, R., Zeller-Plumhoff, B.}, title={Multiscale morphological analysis of bone microarchitecture around Mg-10Gd implants}, year={2023}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.bioactmat.2023.07.017}, abstract = {The utilization of biodegradable magnesium (Mg)-based implants for restoration of bone function following trauma represents a transformative approach in orthopaedic application. One such alloy, magnesium-10 weight percent gadolinium (Mg-10Gd), has been specifically developed to address the rapid degradation of Mg while enhancing its mechanical properties to promote bone healing. Previous studies have demonstrated that Mg-10Gd exhibits favorable osseointegration; however, it exhibits distinct ultrastructural adaptation in comparison to conventional implants like titanium (Ti). A crucial aspect that remains unexplored is the impact of Mg-10Gd degradation on the bone microarchitecture. To address this, we employed hierarchical three-dimensional imaging using synchrotron radiation in conjunction with image-based finite element modelling. By using the methods outlined, the vascular porosity, lacunar porosity and the lacunar-canaliculi network (LCN) morphology of bone around Mg-10Gd in comparison to Ti in a rat model from 4 weeks to 20 weeks post-implantation was investigated. Our investigation revealed that within our observation period, the degradation of Mg-10Gd implants was associated with significantly lower (p < 0.05) lacunar density in the surrounding bone, compared to Ti. Remarkably, the LCN morphology and the fluid flow analysis did not significantly differ for both implant types. In summary, a more pronounced lower lacunae distribution rather than their morphological changes was detected in the surrounding bone upon the degradation of Mg-10Gd implants. This implies potential disparities in bone remodelling rates when compared to Ti implants. Our findings shed light on the intricate relationship between Mg-10Gd degradation and bone microarchitecture, contributing to a deeper understanding of the implications for successful osseointegration.}, note = {Online available at: \url{https://doi.org/10.1016/j.bioactmat.2023.07.017} (DOI). Sefa, S.; Espiritu, J.; Ćwieka, H.; Greving, I.; Flenner, S.; Will, O.; Beuer, S.; Wieland, D.; Willumeit-Römer, R.; Zeller-Plumhoff, B.: Multiscale morphological analysis of bone microarchitecture around Mg-10Gd implants. Bioactive Materials. 2023. vol. 30, 154-168. DOI: 10.1016/j.bioactmat.2023.07.017}} @misc{bruns_on_the_2023, author={Bruns, S., Krüger, D., Galli, S., Wieland, D.C.F., Hammel, J.U., Beckmann, F., Wennerberg, A., Willumeit-Römer, R., Zeller-Plumhoff, B., Moosmann, J.}, title={On the material dependency of peri-implant morphology and stability in healing bone}, year={2023}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.bioactmat.2023.05.006}, abstract = {The microstructural architecture of remodeled bone in the peri-implant region of screw implants plays a vital role in the distribution of strain energy and implant stability. We present a study in which screw implants made from titanium, polyetheretherketone and biodegradable magnesium-gadolinium alloys were implanted into rat tibia and subjected to a push-out test four, eight and twelve weeks after implantation. Screws were 4 mm in length and with an M2 thread. The loading experiment was accompanied by simultaneous three-dimensional imaging using synchrotron-radiation microcomputed tomography at 5 μm resolution. Bone deformation and strains were tracked by applying optical flow-based digital volume correlation to the recorded image sequences. Implant stabilities measured for screws of biodegradable alloys were comparable to pins whereas non-degradable biomaterials experienced additional mechanical stabilization. Peri-implant bone morphology and strain transfer from the loaded implant site depended heavily on the biomaterial utilized. Titanium implants stimulated rapid callus formation displaying a consistent monomodal strain profile whereas the bone volume fraction in the vicinity of magnesium-gadolinium alloys exhibited a minimum close to the interface of the implant and less ordered strain transfer. Correlations in our data suggest that implant stability benefits from disparate bone morphological properties depending on the biomaterial utilized. This leaves the choice of biomaterial as situational depending on local tissue properties.}, note = {Online available at: \url{https://doi.org/10.1016/j.bioactmat.2023.05.006} (DOI). Bruns, S.; Krüger, D.; Galli, S.; Wieland, D.; Hammel, J.; Beckmann, F.; Wennerberg, A.; Willumeit-Römer, R.; Zeller-Plumhoff, B.; Moosmann, J.: On the material dependency of peri-implant morphology and stability in healing bone. Bioactive Materials. 2023. vol. 28, 155-166. DOI: 10.1016/j.bioactmat.2023.05.006}} @misc{kasneryk_formation_and_2022, author={Kasneryk, V., Poschmann, M.P.M., Serdechnova, M., Dovzhenko, G., Wieland, D.C.F., Karlova, P., Naacke, T., Starykevich, M., Blawert, C., Stock, N., Zheludkevich, M.L.}, title={Formation and structure of ZIF-8@PEO coating on the surface of zinc}, year={2022}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.surfcoat.2022.128733}, abstract = {Recently, plasma electrolytic oxidation (PEO) found broad application as a multi-purpose process to create effective corrosion and wear resistant coatings on various metallic substrates. The exceptional properties of metal organic frameworks (MOFs) put them also in focus as perspective materials for corrosion protection. In this work, the formation of a novel ZIF-8@PEO coating is reported for the first time. It was synthesized by controllable recrystallization of a PEO layer formed on zinc alloy Z1 into ZIF-8 in the presence of 2-methylimidazole organic linkers. The multi-stage mechanism of PEO to ZIF-8 rearrangement is proposed. Cross section, glow discharge optical emission spectroscopy and nano-focused synchrotron X-ray diffraction demonstrated that varying of synthesis parameters, the ZIF-8@PEO coating with different distribution of ZIF-8 through PEO layer can be prepared. Based on the results of laser scanning microscopy, the surface smoothing was observed with increasing the degree of the PEO-to-ZIF-8 rearrangement. Containing two components, the novel ZIF-8@PEO coating is expected to combine admirable physical-chemical properties of both PEO and ZIF-8. Such a feature can open the way for its potential application not only for corrosion protection, but also for photo- and heterogeneous catalysis.}, note = {Online available at: \url{https://doi.org/10.1016/j.surfcoat.2022.128733} (DOI). Kasneryk, V.; Poschmann, M.; Serdechnova, M.; Dovzhenko, G.; Wieland, D.; Karlova, P.; Naacke, T.; Starykevich, M.; Blawert, C.; Stock, N.; Zheludkevich, M.: Formation and structure of ZIF-8@PEO coating on the surface of zinc. Surface and Coatings Technology. 2022. vol. 445, 128733. DOI: 10.1016/j.surfcoat.2022.128733}} @misc{vaghefinazari_exploring_the_2022, author={Vaghefinazari, B., Lamaka, S.V., Blawert, C., Serdechnova, M., Scharnagl, N., Karlova, P., Wieland, D.C.F., Zheludkevich, M.L.}, title={Exploring the corrosion inhibition mechanism of 8-hydroxyquinoline for a PEO-coated magnesium alloy}, year={2022}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.corsci.2022.110344}, abstract = {In this study, the corrosion inhibition effect of 8-hydroxyquinoline (8HQ) on a PEO-coated AZ21 magnesium alloy is explored. The interaction of 8HQ molecules with both bare AZ21 and PEO layer was thoroughly scrutinized during the exposure to a corrosive NaCl electrolyte using different characterization methods, including EIS, SEM, Raman spectroscopy, and XRD. The corrosion inhibition mechanism stems from the extensive precipitation of the insoluble complex between 8HQ molecules and Mg2+ on top of the PEO layer, which leads to subsequently inhibition-enhancing phenomena, including modification of the corrosion products and re-precipitation of the PEO amorphous phase.}, note = {Online available at: \url{https://doi.org/10.1016/j.corsci.2022.110344} (DOI). Vaghefinazari, B.; Lamaka, S.; Blawert, C.; Serdechnova, M.; Scharnagl, N.; Karlova, P.; Wieland, D.; Zheludkevich, M.: Exploring the corrosion inhibition mechanism of 8-hydroxyquinoline for a PEO-coated magnesium alloy. Corrosion Science. 2022. vol. 203, 110344. DOI: 10.1016/j.corsci.2022.110344}} @misc{ignjatovi_formation_of_2021, author={Ignjatović, S., Blawert, C., Serdechnova, M., Karpushenkov, S., Damjanović, M., Karlova, P., Wieland, D.C.F., Starykevich, M., Stojanović, S., Damjanović-Vasilić, L., Zheludkevich, M.L.}, title={Formation of multi-functional TiO2 surfaces on AA2024 alloy using plasma electrolytic oxidation}, year={2021}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.apsusc.2020.148875}, abstract = {It was found that the coating thickness and surface morphology are strongly dependent on the PEO processing time. However, the phase composition is not much affected by the treatment time and the main coating phase is rutile with a smaller amount of anatase. Adding additional anatase in the form of particles increases the amount of anatase in the coatings. The additional particle addition has only minor effect on the corrosion resistance, but reduces the wear resistance remarkably. Interestingly, the addition of anatase particles and the PEO treatment time are not effective in increasing the photocatalytic activities of the samples.}, note = {Online available at: \url{https://doi.org/10.1016/j.apsusc.2020.148875} (DOI). Ignjatović, S.; Blawert, C.; Serdechnova, M.; Karpushenkov, S.; Damjanović, M.; Karlova, P.; Wieland, D.; Starykevich, M.; Stojanović, S.; Damjanović-Vasilić, L.; Zheludkevich, M.: Formation of multi-functional TiO2 surfaces on AA2024 alloy using plasma electrolytic oxidation. Applied Surface Science. 2021. vol. 544, 148875. DOI: 10.1016/j.apsusc.2020.148875}} @misc{zellerplumhoff_analysis_of_2020, author={Zeller-Plumhoff, B., Malich, C., Krueger, D., Campbell, G., Wiese, B., Galli, S., Wennerberg, A., Willumeit-Römer, R., Wieland, D.C.F.}, title={Analysis of the bone ultrastructure around biodegradable Mg–xGd implants using small angle X-ray scattering and X-ray diffraction}, year={2020}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.actbio.2019.11.030}, abstract = {Magnesium alloys are increasingly researched as temporary biodegradable metal implants in bone applications due to their mechanical properties which are more similar to bone than conventional implant metals and the fact that Magnesium occurs naturally within the body. However, the degradation processes in vivo and in particular the interaction of the bone with the degrading material need to be further investigated. In this study we are presenting the first quantitative comparison of the bone ultrastructure formed at the interface of biodegradable Mg–5Gd and Mg–10Gd implants and titanium and PEEK implants after 4, 8 and 12 weeks healing time using two-dimensional small angle X-ray scattering and X-ray diffraction. Differences in mineralization, orientation and thickness of the hydroxyapatite are assessed. We find statistically significant (p < 0.05) differences for the lattice spacing of the (310)-reflex of hydroxyapatite between titanium and Mg–xGd materials, as well as for the (310) crystal size between titanium and Mg–5Gd, indicating a possible deposition of Mg within the bone matrix. The (310) lattice spacing and crystallite size further differ significantly between implant degradation layer and surrounding bone (p < 0.001 for Mg–10Gd), suggesting apatite formation with significant amounts of Gd and Mg within the degradation layer.}, note = {Online available at: \url{https://doi.org/10.1016/j.actbio.2019.11.030} (DOI). Zeller-Plumhoff, B.; Malich, C.; Krueger, D.; Campbell, G.; Wiese, B.; Galli, S.; Wennerberg, A.; Willumeit-Römer, R.; Wieland, D.: Analysis of the bone ultrastructure around biodegradable Mg–xGd implants using small angle X-ray scattering and X-ray diffraction. Acta Biomaterialia. 2020. vol. 101, 637-645. DOI: 10.1016/j.actbio.2019.11.030}} @misc{kalanda_smallangle_neutron_2019, author={Kalanda, N., Haramus, V.M., Avdeev, M., Zheludkevich, M.L., Yarmolich, M., Serdechnova, M., Wieland, D.C.F., Petrov, A., Zhaludkevich, A., Sobolev, N.}, title={Small‐Angle Neutron Scattering and Magnetically Heterogeneous State in Sr2FeMoO6–δ}, year={2019}, howpublished = {journal article}, doi = {https://doi.org/10.1002/pssb.201800428}, abstract = {Single‐phase strontium ferromolybdate (Sr2FeMoO6–δ) samples with different degrees of the superstructural ordering of the Fe/Mo cations (P) are obtained from partially reduced SrFeO3–х, SrMoO4 precursors by the solid‐state technology. The study of the temperature dependences of the magnetization measured in the field‐cooling and zero‐field‐cooling modes indicated an inhomogeneous magnetic state of the samples. The presence of magnetic regions of different nature has also been revealed by the small‐angle neutron scattering. For the Sr2FeMoO6–δ samples with different P values and for all values of the magnetic field induction up to 1.5 T and of the scattering vector in the interval 0.1 > q > 0.002 Å−1, the analytical dependence I ∼ q–α obeys the Porod law (α ≈ 4), which corresponds to an object with a smooth and well‐marked surface and polydisperse grain size. Deviations from the Porod law in the q > 0.1 Å−1 region and a weakening of the neutron scattering in applied magnetic fields may be ascribed to magnetic inhomogeneities with diameters D < 6 nm, which are partially destroyed/oriented by magnetic fields В ≥ 1.5 T. It is established that the magnetic homogeneity of the Sr2FeMoO6–δ compound is enhanced with increasing superstructural ordering of the Fe/Mo cations.}, note = {Online available at: \url{https://doi.org/10.1002/pssb.201800428} (DOI). Kalanda, N.; Haramus, V.; Avdeev, M.; Zheludkevich, M.; Yarmolich, M.; Serdechnova, M.; Wieland, D.; Petrov, A.; Zhaludkevich, A.; Sobolev, N.: Small‐Angle Neutron Scattering and Magnetically Heterogeneous State in Sr2FeMoO6–δ. Physica Status Solidi B. 2019. vol. 256, no. 5, 1800428. DOI: 10.1002/pssb.201800428}} @misc{zander_influence_of_2019, author={Zander, T., Wieland, D.C.F., Raj, A., Salmen, P., Dogan, S., Dedinaite, A., Haramus, V.M., Schreyer, A., Claesson, P.M., Willumeit-Römer, R.}, title={Influence of high hydrostatic pressure on solid supported DPPC bilayers with hyaluronan in the presence of Ca2+ ions}, year={2019}, howpublished = {journal article}, doi = {https://doi.org/10.1039/C9SM01066A}, abstract = {The molecular mechanisms responsible for outstanding lubrication of natural systems, like articular joints, have been the focus of scientific research for several decades. One essential aspect is the lubrication under pressure, where it is important to understand how the lubricating entities adapt under dynamic working conditions in order to fulfill their function. We made a structural investigation of a model system consisting of two of the molecules present at the cartilage interface, 1,2-dipalmitoyl-sn-glycero-3-phosphocholine and hyaluronan, at high hydrostatic pressure. Phospholipid layers are found at the cartilage surfaces and are able to considerably reduce friction. Their behavior under load and varied solution conditions is important as pressures of 180 bar are encountered during daily life activities. We focus on how divalent ions, like Ca2+, affect the interaction between DPPC and hyaluronan, as other investigations have indicated that calcium ions influence their interaction. It could be shown that already low amounts of Ca2+ strongly influence the interaction of hyaluronan with DPPC. Our results suggest that the calcium ions increase the amount of adsorbed hyaluronan indicating an increased electrostatic interaction. Most importantly, we observe a modification of the DPPC phase diagram as hyaluronan absorbs to the bilayer which results in an Lα-like structure at low temperatures and a decoupling of the leaflets forming an asymmetric bilayer structure.}, note = {Online available at: \url{https://doi.org/10.1039/C9SM01066A} (DOI). Zander, T.; Wieland, D.; Raj, A.; Salmen, P.; Dogan, S.; Dedinaite, A.; Haramus, V.; Schreyer, A.; Claesson, P.; Willumeit-Römer, R.: Influence of high hydrostatic pressure on solid supported DPPC bilayers with hyaluronan in the presence of Ca2+ ions. Soft Matter. 2019. vol. 15, no. 36, 7295-7304. DOI: 10.1039/C9SM01066A}} @misc{bouali_layered_double_2019, author={Bouali, A.C., Straumal, E.A., Serdechnova, M., Wieland, D.C.F., Starykevich, M., Blawert, C., Hammel, J.U., Lermontov, S.A., Ferreira, M.G.S., Zheludkevich, M.L.}, title={Layered double hydroxide based active corrosion protective sealing of plasma electrolytic oxidation/sol-gel composite coating on AA2024}, year={2019}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.apsusc.2019.07.117}, abstract = {This work reports a novel approach for growing layered double hydroxide (LDH) films on any plasma electrolytic oxidation (PEO) coated AA2024 independently of the nature of the PEO coating. The specific PEO coating chosen to carry out this work is considered to be not suitable for direct LDH growth because of phase composition and morphological features. In this paper, we describe a new methodology that consists of covering the PEO coating with a thin layer of aluminum oxide based xerogel as the source of aluminate ions for subsequent in-situ LDH growth. X-ray diffraction (XRD) and scanning electron microscope (SEM) images showed a successful formation of LDHs on the surface. An improvement in terms of active corrosion protection was also demonstrated by electrochemical impedance spectroscopy (EIS) and scanning vibrating electrode technique (SVET).}, note = {Online available at: \url{https://doi.org/10.1016/j.apsusc.2019.07.117} (DOI). Bouali, A.; Straumal, E.; Serdechnova, M.; Wieland, D.; Starykevich, M.; Blawert, C.; Hammel, J.; Lermontov, S.; Ferreira, M.; Zheludkevich, M.: Layered double hydroxide based active corrosion protective sealing of plasma electrolytic oxidation/sol-gel composite coating on AA2024. Applied Surface Science. 2019. vol. 494, 829-840. DOI: 10.1016/j.apsusc.2019.07.117}} @misc{dedinaite_biolubrication_synergy_2019, author={Dedinaite, A., Wieland, D.C.F., Beldowski, P., Claesson, P.M.}, title={Biolubrication synergy: Hyaluronan – Phospholipid interactions at interfaces}, year={2019}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.cis.2019.102050}, abstract = {The manner in which nature has solved lubrication issues has fascinated scientists for centuries, in particular when considering that lubrication is achieved in aqueous media. The most outstanding system in this respect is likely the synovial joint, where close to frictionless motion is realized under different loads and shear rates. This review article focuses on two components present in the synovial area, hyaluronan and phospholipids. We recapitulate what has been learned about their interactions at interfaces from recent experiments, with focus on results obtained using reflectivity techniques at large scale facilities. In parallel, modelling experiments have been carried out and from these efforts new detailed knowledge about how hyaluronan and phospholipids interact has been gained. In this review we combine findings from modelling and experiments to gain deeper insight. Finally, we summarize what has been learned of the lubrication performance of mixtures of phospholipids and hyaluronan.}, note = {Online available at: \url{https://doi.org/10.1016/j.cis.2019.102050} (DOI). Dedinaite, A.; Wieland, D.; Beldowski, P.; Claesson, P.: Biolubrication synergy: Hyaluronan – Phospholipid interactions at interfaces. Advances in Colloid and Interface Science. 2019. vol. 274, 102050. DOI: 10.1016/j.cis.2019.102050}} @misc{wieland_complex_solutions_2017, author={Wieland, D.C.F., Zander, T., Haramus, V.M., Krywka, C., Dedinaite, A., Claesson, P., Willumeit-Roemer, R.}, title={Complex solutions under shear and pressure: a rheometer setup for X-ray scattering experiments}, year={2017}, howpublished = {journal article}, doi = {https://doi.org/10.1107/S1600577517002648}, abstract = {A newly developed high-pressure rheometer for in situ X-ray scattering experiments is described. A commercial rheometer was modified in such a way that X-ray scattering experiments can be performed under different pressures and shear. First experiments were carried out on hyaluronan, a ubiquitous biopolymer that is important for different functions in the body such as articular joint lubrication. The data hint at a decreased electrostatic interaction at higher pressure, presumably due to the increase of the dielectric constant of water by 3% and the decrease of the free volume at 300 bar.}, note = {Online available at: \url{https://doi.org/10.1107/S1600577517002648} (DOI). Wieland, D.; Zander, T.; Haramus, V.; Krywka, C.; Dedinaite, A.; Claesson, P.; Willumeit-Roemer, R.: Complex solutions under shear and pressure: a rheometer setup for X-ray scattering experiments. Journal of Synchrotron Radiation. 2017. vol. 24, no. 3, 646-652. DOI: 10.1107/S1600577517002648}} @misc{golub_solution_structure_2017, author={Golub, M., Hejazi, M., Koelsch, A., Lokstein, H., Wieland, D.C.F., Zouni, A., Pieper, J.}, title={Solution structure of monomeric and trimeric photosystem I of Thermosynechococcus elongatus investigated by small-angle X-ray scattering}, year={2017}, howpublished = {journal article}, doi = {https://doi.org/10.1007/s11120-017-0342-6}, abstract = {The structure of monomeric and trimeric photosystem I (PS I) of Thermosynechococcus elongatus BP1 (T. elongatus) was investigated by small-angle X-ray scattering (SAXS). The scattering data reveal that the protein–detergent complexes possess radii of gyration of 58 and 78 Å in the cases of monomeric and trimeric PS I, respectively. The results also show that the samples are monodisperse, virtually free of aggregation, and contain empty detergent micelles. The shape of the protein–detergent complexes can be well approximated by elliptical cylinders with a height of 78 Å. Monomeric PS I in buffer solution exhibits minor and major radii of the elliptical cylinder of about 50 and 85 Å, respectively. In the case of trimeric PS I, both radii are equal to about 110 Å. The latter model can be shown to accommodate three elliptical cylinders equal to those describing monomeric PS I. A structure reconstitution also reveals that the protein–detergent complexes are larger than their respective crystal structures. The reconstituted structures are larger by about 20 Å mainly in the region of the hydrophobic surfaces of the monomeric and trimeric PS I complexes. This seeming contradiction can be resolved by the addition of a detergent belt constituted by a monolayer of dodecyl-β-D-maltoside molecules. Assuming a closest possible packing, a number of roughly 1024 and 1472 detergent molecules can be determined for monomeric and trimeric PS I, respectively. Taking the monolayer of detergent molecules into account, the solution structure can be almost perfectly modeled by the crystal structures of monomeric and trimeric PS I.}, note = {Online available at: \url{https://doi.org/10.1007/s11120-017-0342-6} (DOI). Golub, M.; Hejazi, M.; Koelsch, A.; Lokstein, H.; Wieland, D.; Zouni, A.; Pieper, J.: Solution structure of monomeric and trimeric photosystem I of Thermosynechococcus elongatus investigated by small-angle X-ray scattering. Photosynthesis Research. 2017. vol. 133, no. 1-3, 163-173. DOI: 10.1007/s11120-017-0342-6}} @misc{golub_solution_structure_2017, author={Golub, M., Combet, S., Wieland, D.C.F., Soloviov, D., Kuklin, A., Lokstein, H., Schmitt, F.-J., Olliges, R., Hecht, M., Eckert, H.-J., Pieper, J.}, title={Solution structure and excitation energy transfer in phycobiliproteins of Acaryochloris marina investigated by small angle scattering}, year={2017}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.bbabio.2017.01.010}, abstract = {The structure of phycobiliproteins of the cyanobacterium Acaryochloris marina was investigated in buffer solution at physiological temperatures, i.e. under the same conditions applied in spectroscopic experiments, using small angle neutron scattering. The scattering data of intact phycobiliproteins in buffer solution containing phosphate can be well described using a cylindrical shape with a length of about 225 Å and a diameter of approximately 100 Å. This finding is qualitatively consistent with earlier electron microscopy studies reporting a rod-like shape of the phycobiliproteins with a length of about 250 (M. Chen et al., FEBS Letters 583, 2009, 2535) or 300 Å (J. Marquart et al., FEBS Letters 410, 1997, 428). In contrast, phycobiliproteins dissolved in buffer lacking phosphate revealed a splitting of the rods into cylindrical subunits with a height of 28 Å only, but also a pronounced sample aggregation. Complementary small angle neutron and X-ray scattering experiments on phycocyanin suggest that the cylindrical subunits may represent either trimeric phycocyanin or trimeric allophycocyanin. Our findings are in agreement with the assumption that a phycobiliprotein rod with a total height of about 225 Å can accommodate seven trimeric phycocyanin subunits and one trimeric allophycocyanin subunit, each of which having a height of about 28 Å. The structural information obtained by small angle neutron and X-ray scattering can be used to interpret variations in the low-energy region of the 4.5 K absorption spectra of phycobiliproteins dissolved in buffer solutions containing and lacking phosphate, respectively.}, note = {Online available at: \url{https://doi.org/10.1016/j.bbabio.2017.01.010} (DOI). Golub, M.; Combet, S.; Wieland, D.; Soloviov, D.; Kuklin, A.; Lokstein, H.; Schmitt, F.; Olliges, R.; Hecht, M.; Eckert, H.; Pieper, J.: Solution structure and excitation energy transfer in phycobiliproteins of Acaryochloris marina investigated by small angle scattering. Biochimica et Biophysica Acta: Bioenergetics. 2017. vol. 1858, no. 4, 318-324. DOI: 10.1016/j.bbabio.2017.01.010}} @misc{raj_lubrication_synergy_2017, author={Raj, A., Wang, M., Zander, T., Wieland, D.C.F., Liu, X., An, J., Haramus, V.M., Willumeit-Roemer, R., Fielden, M., Claesson, P.M., Dedinaite, A.}, title={Lubrication synergy: Mixture of hyaluronan and dipalmitoylphosphatidylcholine (DPPC) vesicles}, year={2017}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.jcis.2016.10.091}, abstract = {Phospholipids and hyaluronan have been implied to fulfil important roles in synovial joint lubrication. Since both components are present in synovial fluid, self-assembly structures formed by them should also be present. We demonstrate by small angle X-ray scattering that hyaluronan associates with the outer shell of dipalmitoylphophatidylcholine (DPPC) vesicles in bulk solution. Further, we follow adsorption to silica from mixed hyaluronan/DPPC vesicle solution by Quartz Crystal Microbalance with Dissipation measurements. Atomic Force Microscope imaging visualises the adsorbed layer structure consisting of non-homogeneous phospholipid bilayer with hyaluronan/DPPC aggregates on top. The presence of these aggregates generates a long-range repulsive surface force as two such surfaces are brought together. However, the aggregates are easily deformed, partly rearranged into multilayer structures and partly removed from between the surfaces under high loads. These layers offer very low friction coefficient (<0.01), high load bearing capacity (≈23 MPa), and self-healing ability. Surface bound DPPC/hyaluronan aggregates provide a means for accumulation of lubricating DPPC molecules on sliding surfaces.}, note = {Online available at: \url{https://doi.org/10.1016/j.jcis.2016.10.091} (DOI). Raj, A.; Wang, M.; Zander, T.; Wieland, D.; Liu, X.; An, J.; Haramus, V.; Willumeit-Roemer, R.; Fielden, M.; Claesson, P.; Dedinaite, A.: Lubrication synergy: Mixture of hyaluronan and dipalmitoylphosphatidylcholine (DPPC) vesicles. Journal of Colloid and Interface Science. 2017. vol. 488, 225-233. DOI: 10.1016/j.jcis.2016.10.091}} @misc{nyrow_bulk_sensitive_2016, author={Nyrow, A., Sternemann, C., Tse, J.S., Weis, C., Sahle, C,J., Mende, K., Wieland, D.C.F., Cerantola, V., Gordon, R.A., Spiekermann, G., Regier, T., Wilke, M., Tolan, M.}, title={Bulk sensitive determination of the Fe3+/FeTot-ratio in minerals by Fe L2/3-edge X-ray Raman scattering}, year={2016}, howpublished = {journal article}, doi = {https://doi.org/10.1039/C5JA00261C}, abstract = {We present the first measurements of the iron L2/3-edge of the compounds FeO, Fe2O3, and Fe3O4 at ambient pressure and of FeCO3 at high pressures of 2.4 and 40 GPa using a diamond anvil cell by X-ray Raman scattering spectroscopy, a bulk sensitive probe of soft X-ray absorption edges making use of hard X-rays. We show that the spectral shape of the Fe L2/3-edge can be analyzed quantitatively to reveal the oxidation state of iron in matter. Consequently, in situ X-ray Raman scattering spectroscopy at the iron L-edge at high pressure and temperature opens exciting perspectives to characterize the local coordination, oxidation, and spin state of iron at high pressure and temperature, conditions that are of relevance for e.g. geological sciences or chemical processing.}, note = {Online available at: \url{https://doi.org/10.1039/C5JA00261C} (DOI). Nyrow, A.; Sternemann, C.; Tse, J.; Weis, C.; Sahle, C.; Mende, K.; Wieland, D.; Cerantola, V.; Gordon, R.; Spiekermann, G.; Regier, T.; Wilke, M.; Tolan, M.: Bulk sensitive determination of the Fe3+/FeTot-ratio in minerals by Fe L2/3-edge X-ray Raman scattering. Journal of Analytical Atomic Spectrometry. 2016. vol. 31, no. 3, 815-820. DOI: 10.1039/C5JA00261C}} @misc{wieland_studying_solutions_2016, author={Wieland, D.C.F., Haramus, V.M., Zander, T., Krywka, C., Wang, M., Dedinaite, A., Claesson, P.M., Willumeit-Roemer, R.}, title={Studying solutions at high shear rates: a dedicated microfluidics setup}, year={2016}, howpublished = {journal article}, doi = {https://doi.org/10.1107/S1600577515024856}, abstract = {The development of a dedicated small-angle X-ray scattering setup for the investigation of complex fluids at different controlled shear conditions is reported. The setup utilizes a microfluidics chip with a narrowing channel. As a consequence, a shear gradient is generated within the channel and the effect of shear rate on structure and interactions is mapped spatially. In a first experiment small-angle X-ray scattering is utilized to investigate highly concentrated protein solutions up to a shear rate of 300000 s-1. These data demonstrate that equilibrium clusters of lysozyme are destabilized at high shear rates.}, note = {Online available at: \url{https://doi.org/10.1107/S1600577515024856} (DOI). Wieland, D.; Haramus, V.; Zander, T.; Krywka, C.; Wang, M.; Dedinaite, A.; Claesson, P.; Willumeit-Roemer, R.: Studying solutions at high shear rates: a dedicated microfluidics setup. Journal of Synchrotron Radiation. 2016. vol. 23, no. 2, 480-486. DOI: 10.1107/S1600577515024856}} @misc{zander_the_influence_2016, author={Zander, T., Wieland, D.C.F., Raj, A., Wang, M., Nowak, B., Krywka, C., Dedinaite, A., Claesson, P.M., Haramus, V.M., Schreyer, A., Willumeit-Roemer, R.}, title={The influence of hyaluronan on the structure of a DPPC—bilayer under high pressures}, year={2016}, howpublished = {journal article}, doi = {https://doi.org/10.1016/j.colsurfb.2016.02.040}, abstract = {The superior lubrication properties of synovial joints have inspired many studies aiming at uncovering the molecular mechanisms which give rise to low friction and wear. However, the mechanisms are not fully understood yet, and, in particular, it has not been elucidated how the biolubricants present at the interface of cartilage respond to high pressures, which arise during high loads of joints. In this study we utilize a simple model system composed of two biomolecules that have been implied as being important for joint lubrication. It consists of a solid supported dipalmitoylphosphatidylcholin (DPPC) bilayer, which was formed via vesicles fusion on a flat Si wafer, and the anionic polysaccharide hyaluronan (HA). We first characterized the structure of the HA layer that adsorbed to the DPPC bilayers at ambient pressure and different temperatures using X-ray reflectivity (XRR) measurements. Next, XRR was utilized to evaluate the response of the system to high hydrostatic pressures, up to 2 kbar (200 MPa), at three different temperatures. By means of fluorescence microscopy images the distribution of DPPC and HA on the surface was visualized. Our data suggest that HA adsorbs to the headgroup region that is oriented towards the water side of the supported bilayer. Phase transitions of the bilayer in response to temperature and pressure changes were also observed in presence and absence of HA. Our results reveal a higher stability against high hydrostatic pressures for DPPC/HA composite layers compared to that of the DPPC bilayer in absence of HA.}, note = {Online available at: \url{https://doi.org/10.1016/j.colsurfb.2016.02.040} (DOI). Zander, T.; Wieland, D.; Raj, A.; Wang, M.; Nowak, B.; Krywka, C.; Dedinaite, A.; Claesson, P.; Haramus, V.; Schreyer, A.; Willumeit-Roemer, R.: The influence of hyaluronan on the structure of a DPPC—bilayer under high pressures. Colloids and Surfaces B. 2016. vol. 142, 230-238. DOI: 10.1016/j.colsurfb.2016.02.040}}