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- ItemExploring the atmospheric chemistry of nitrous acid (HONO) at a rural site in Southern China(München : European Geopyhsical Union, 2012) Li, X.; Brauers, T.; Häseler, R.; Bohn, B.; Fuchs, H.; Hofzumahaus, A.; Holland, F.; Lou, S.; Lu, K.D.; Rohrer, F.; Hu, M.; Zeng, L.M.; Zhang, Y.H.; Garland, R.M.; Su, H.; Nowak, A.; Wiedensohler, A.; Takegawa, N.; Shao, M.; Wahner, A.We performed measurements of nitrous acid (HONO) during the PRIDE-PRD2006 campaign in the Pearl River Delta region 60 km north of Guangzhou, China, for 4 weeks in June 2006. HONO was measured by a LOPAP in-situ instrument which was setup in one of the campaign supersites along with a variety of instruments measuring hydroxyl radicals, trace gases, aerosols, and meteorological parameters. Maximum diurnal HONO mixing ratios of 1–5 ppb were observed during the nights. We found that the nighttime build-up of HONO can be attributed to the heterogeneous NO2 to HONO conversion on ground surfaces and the OH + NO reaction. In addition to elevated nighttime mixing ratios, measured noontime values of ≈200 ppt indicate the existence of a daytime source higher than the OH + NO→HONO reaction. Using the simultaneously recorded OH, NO, and HONO photolysis frequency, a daytime additional source strength of HONO (PM) was calculated to be 0.77 ppb h−1 on average. This value compares well to previous measurements in other environments. Our analysis of PM provides evidence that the photolysis of HNO3 adsorbed on ground surfaces contributes to the HONO formation.
- ItemDesign and performance of an automatic regenerating adsorption aerosol dryer for continuous operation at monitoring sites(München : European Geopyhsical Union, 2009) Tuch, T.M.; Haudek, A.; Müller, T.; Nowak, A.; Wex, H.; Wiedensohler, A.Sizes of aerosol particles depend on the relative humidity of their carrier gas. Most monitoring networks require therefore that the aerosol is dried to a relative humidity below 50% r.H. to ensure comparability of measurements at different sites. Commercially available aerosol dryers are often not suitable for this purpose at remote monitoring sites. Adsorption dryers need to be regenerated frequently and maintenance-free single column Nafion dryers are not designed for high aerosol flow rates. We therefore developed an automatic regenerating adsorption aerosol dryer with a design flow rate of 1 m3/h. Particle transmission efficiency of this dryer has been determined during a 3 week experiment. The lower 50% cut-off was found to be smaller than 3 nm at the design flow rate of the instrument. Measured transmission efficiencies are in good agreement with theoretical calculations. One dryer has been successfully deployed in the Amazon river basin. We present data from this monitoring site for the first 6 months of measurements (February 2008–August 2008). Apart from one unscheduled service, this dryer did not require any maintenance during this time period. The average relative humidity of the dried aerosol was 27.1+/−7.5% r.H. compared to an average ambient relative humidity of nearly 80% and temperatures around 30°C. This initial deployment demonstrated that these dryers are well suitable for continuous operation at remote monitoring sites under adverse ambient conditions.
- ItemHydrophilic non-precious metal nitrogen-doped carbon electrocatalysts for enhanced efficiency in oxygen reduction reaction(Cambridge : Royal Society of Chemistry, 2015) Hao, Guang-Ping; Sahraie, Nastaran Ranjbar; Zhang, Qiang; Krause, Simon; Oschatz, Martin; Bachmatiuk, Alicja; Strasser, Peter; Kaskel, StefanExploring the role of surface hydrophilicity of non-precious metal N-doped carbon electrocatalysts in electrocatalysis is challenging. Herein we discover an ultra-hydrophilic non-precious carbon electrocatalyst, showing enhanced catalysis efficiency on both gravimetric and areal basis for oxygen reduction reaction due to a high dispersion of active centres.
- ItemUniversal emulsion stabilization from the arrested adsorption of rough particles at liquid-liquid interfaces([London] : Nature Publishing Group UK, 2017) Zanini, Michele; Marschelke, Claudia; Anachkov, Svetoslav E.; Marini, Emanuele; Synytska, Alla; Isa, LucioSurface heterogeneities, including roughness, significantly affect the adsorption, motion and interactions of particles at fluid interfaces. However, a systematic experimental study, linking surface roughness to particle wettability at a microscopic level, is currently missing. Here we synthesize a library of all-silica microparticles with uniform surface chemistry, but tuneable surface roughness and study their spontaneous adsorption at oil-water interfaces. We demonstrate that surface roughness strongly pins the particles' contact lines and arrests their adsorption in long-lived metastable positions, and we directly measure the roughness-induced interface deformations around isolated particles. Pinning imparts tremendous contact angle hysteresis, which can practically invert the particle wettability for sufficient roughness, irrespective of their chemical nature. As a unique consequence, the same rough particles stabilize both water-in-oil and oil-in-water emulsions depending on the phase they are initially dispersed in. These results both shed light on fundamental phenomena concerning particle adsorption at fluid interfaces and indicate future design rules for particle-based emulsifiers.
- ItemInteraction between immobilized polyelectrolyte complex nanoparticles and human mesenchymal stromal cells(Auckland : DOVE Medical Press, 2014) Woltmann, B.; Torger, B.; Müller, M.; Hempel, U.Background: Implant loosening or deficient osseointegration is a major problem in patients with systemic bone diseases (eg, osteoporosis). For this reason, the stimulation of the regional cell population by local and sustained drug delivery at the bone/implant interface to induce the formation of a mechanical stable bone is promising. The purpose of this study was to investigate the interaction of polymer-based nanoparticles with human bone marrow-derived cells, considering nanoparticles' composition and surface net charge. Materials and methods: Polyelectrolyte complex nanoparticles (PECNPs) composed of the polycations poly(ethyleneimine) (PEI), poly(L-lysine) (PLL), or (N,N-diethylamino)ethyldextran (DEAE) in combination with the polyanions dextran sulfate (DS) or cellulose sulfate (CS) were prepared. PECNPs' physicochemical properties (size, net charge) were characterized by dynamic light scattering and particle charge detector measurements. Biocompatibility was investigated using human mesenchymal stromal cells (hMSCs) cultured on immobilized PECNP films (5-50 nmol·cm-2) by analysis for metabolic activity of hMSCs in dependence of PECNP surface concentration by MTS (3-[4,5-dimethylthiazol-2-yl]-5-[3-carboxymethoxyphenyl]-2-[4-sulfophenyl]-2H-tetrazolium, inner salt) assay, as well as cell morphology (phase contrast microscopy). Results: PECNPs ranging between ~50 nm and 150 nm were prepared. By varying the ratio of polycations and polyanions, PECNPs with a slightly positive (PEC+NP) or negative (PEC-NP) net charge were obtained. The PECNP composition significantly affected cell morphology and metabolic activity, whereas the net charge had a negligible influence. Therefore, we classified PECNPs into "variant systems" featuring a significant dose dependency of metabolic activity (DEAE/CS, PEI/DS) and "invariant systems" lacking such a dependency (DEAE/DS, PEI/CS). Immunofluorescence imaging of fluorescein isothiocyanate isomer I (FITC)-labeled PECNPs suggested internalization into hMSCs remaining stable for 8 days. Conclusion: Our study demonstrated that PECNP composition affects hMSC behavior. In particular, the PEI/CS system showed biocompatibility in a wide concentration range, representing a suitable system for local drug delivery from PECNP-functionalized bone substitute materials.
- ItemLinear and ring polymers in confined geometries(Berlin ; Heidelberg : Springer, 2017) Usatenko, Zoryana; Kuterba, Piotr; Chamati, Hassan; Romeis, DirkA short overview of the theoretical and experimental works on the polymer-colloid mixtures is given. The behaviour of a dilute solution of linear and ring polymers in confined geometries like slit of two parallel walls or in the solution of mesoscopic colloidal particles of big size with different adsorbing or repelling properties in respect to polymers is discussed. Besides, we consider the massive field theory approach in fixed space dimensions d = 3 for the investigation of the interaction between long flexible polymers and mesoscopic colloidal particles of big size and for the calculation of the correspondent depletion interaction potentials and the depletion forces between confining walls. The presented results indicate the interesting and nontrivial behavior of linear and ring polymers in confined geometries and give possibility better to understand the complexity of physical effects arising from confinement and chain topology which plays a significant role in the shaping of individual chromosomes and in the process of their segregation, especially in the case of elongated bacterial cells. The possibility of using linear and ring polymers for production of new types of nano- and micro-electromechanical devices is analyzed.
- ItemThe sequence to hydrogenate coronene cations: A journey guided by magic numbers([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Cazaux, Stéphanie; Boschman, Leon; Rougeau, Nathalie; Reitsma, Geert; Hoekstra, Ronnie; Teillet-Billy, Dominique; Morisset, Sabine; Spaans, Marco; Schlathölter, ThomasThe understanding of hydrogen attachment to carbonaceous surfaces is essential to a wide variety of research fields and technologies such as hydrogen storage for transportation, precise localization of hydrogen in electronic devices and the formation of cosmic H2. For coronene cations as prototypical Polycyclic Aromatic Hydrocarbon (PAH) molecules, the existence of magic numbers upon hydrogenation was uncovered experimentally. Quantum chemistry calculations show that hydrogenation follows a site-specific sequence leading to the appearance of cations having 5, 11, or 17 hydrogen atoms attached, exactly the magic numbers found in the experiments. For these closed-shell cations, further hydrogenation requires appreciable structural changes associated with a high transition barrier. Controlling specific hydrogenation pathways would provide the possibility to tune the location of hydrogen attachment and the stability of the system. The sequence to hydrogenate PAHs, leading to PAHs with magic numbers of H atoms attached, provides clues to understand that carbon in space is mostly aromatic and partially aliphatic in PAHs. PAH hydrogenation is fundamental to assess the contribution of PAHs to the formation of cosmic H2.