Asphaltene molecular size and weight have been of concern since asphaltenes were first isolated from crude oils. Despite previous divergent results on this topic, in recent years, there has been a growing consensus among all mass spectral ionization techniques and all diffusion measurements that asphaltenes are fairly small molecules. In this paper, fluorescence correlation spectroscopy (FCS) is used to determine translational diffusion coefficients of asphaltene and model compounds under a variety of conditions. These FCS studies provide several stringent tests on asphaltene molecular size and architecture. A broad range of concentrations including ultralow concentrations is investigated to ensure the lack of potential aggregation difficulties. Large temperature variations are used to test the application of the simple diffusion equation. FCS results here clearly show the dependence of the diffusion constant on the molecular weight. Finally, FCS results on asphaltenes are in quantitative agreement with those of time-resolved fluorescence depolarization on asphaltenes. A comparison of the results herein with previous FCS and time-resolved fluorescence depolarization (TRFD) results on the same asphaltenes confirms the correlation between molecular size and asphaltene chromophore size; this supports a molecular architecture with one or two polycyclic aromatic hydrocarbons (PAHs) per molecule and counters proposed structures with many PAHs per asphaltene molecule.
Many microfluidic applications require modified surface wettability of the microchannels. Patterning of wettability within enclosed microfluidic structures at high spatial resolution has been challenging in the past. In this paper, we report an improved method for altering the surface wettability in poly(dimethylsiloxane) (PDMS) microchannels by UV-induced graft polymerization of poly(acrylic acid). Our method presents significant improvements in terms of wettability contrast and spatial resolution of the patterned structures as compared to recent literature and is in particular applicable to complex microfluidic structures with a broad range of channel sizes and aspect ratios. A key part of our work is the clear description of the surface treatment process with the identification of key parameters, some of which have been overlooked, neglected, or misinterpreted in previous works. We have studied these key parameters in detail and provide recommended values for each parameter supported by experimental results. This detailed understanding of the treatment process and the effects of the critical parameters on it allowed us to significantly improve quality and reliability of the treatment process.
Following the great success of traditional microfluidic devices across many disciplines, a new class of microfluidic systems emerged in recent years, which features finely tuned, localized surface modifications within the microstructures in order to keep up with the demand for devices of ever increasing complexity (lab on chip, assay on chip, etc.). Graft photopolymerization has become a powerful tool for such localized surface modifications particularly in combination with poly(dimethylsiloxane) (PDMS) devices, as it is compatible with many functional monomers and allows for high spatial resolution. However, application within enclosed PDMS microstructures and in particular well-controlled surface-directed polymerization remains challenging. Detailed understanding of the interaction between photoinitiator, benzophenone (BP), and polymer matrix is needed. We have developed a visualization technique, which allows for observation of reacted BP in situ within the PDMS matrix. We present a detailed study on solvent-driven BP diffusion providing results essential to successful surface treatment. We also identified and investigated photoinitiator inhibition by oxygen and provide appropriate mitigation strategies.
We present a microfluidic apparatus and method for the measurement of asphaltene content in crude-oil samples. The measurement is based on an optical absorption technique, where it was established that asphaltene coloration correlated linearly with asphaltene weight content. The initial absorbance of the oil is measured, and asphaltenes are removed from the oil by the addition of n-alkane, leading to flocculation and subsequent filtration. The absorbance of the deasphalted oil (maltenes) is then measured, and the initial asphaltene content is revealed by the change in absorbance. The asphaltene optical densities correlated linearly with conventional weight measurement results (e.g., ASTM D6560) for 38 crude-oil samples from around the world. Sample measurement repeatability was shown to be within ±2% over several months. Other aspects influencing performance of the system were evaluated, including plug dispersion, flocculation kinetics, membrane degradation, and channel clogging. The microfluidic approach described here permits asphaltene content measurement in less than 30 min as opposed to days required with traditional gravimetric techniques. This many-fold reduction in measurement time will enable more frequent characterization of crude oil samples.
Many plants and insects possess multi‐functional surfaces covered by dense nanohair. Such a nanofur is of high interest for various biomimetic applications like self‐healing, air retention, and oil/water separation. Here, we introduce a highly scalable and competitive molding technique for the fabrication of biomimetic nanofur. With this method, we pull nanofur out of flat polycarbonate and tune its wettability from hydrophilic to superhydrophobic. By mechanically structuring these samples we create various devices suitable for microfluidics. The nanofur can be also used for the fabrication of self‐healing surfaces inspired by pitcher plants as well as for air‐retaining surfaces mimicking the water fern Salvinia minima. Finally, we utilize the nanofur for oil/water separation and the cleaning of oil spills.
Inspired by the white beetle of the genus Cyphochilus, we fabricate ultra-thin, porous PMMA films by foaming with CO2 saturation. Optimising pore diameter and fraction in terms of broad-band reflectance results in very thin films with exceptional whiteness. Already films with 60 µm-thick scattering layer feature a whiteness with a reflectance of 90%. Even 9 µm thin scattering layers appear white with a reflectance above 57%. The transport mean free path in the artificial films is between 3.5 µm and 4 µm being close to the evolutionary optimised natural prototype. The bio-inspired white films do not lose their whiteness during further shaping, allowing for various applications.
3D organoids using stem cells to study development and disease are now widespread. These models are powerful to mimic in vivo situations but are currently associated with high variability and low throughput. For biomedical research, platforms are thus necessary to increase reproducibility and allow high-throughput screens (HTS). Here, we introduce a microwell platform, integrated in standard culture plates, for functional HTS. Using micro-thermoforming, we form round-bottom microwell arrays from optically clear cyclic olefin polymer films, and assemble them with bottom-less 96-well plates. We show that embryonic stem cells aggregate faster and more reproducibly (centricity, circularity) as compared to a state-of-the-art microwell array. We then run a screen of a chemical library to direct differentiation into primitive endoderm (PrE) and, using on-chip high content imaging (HCI), we identify molecules, including regulators of the cAMP pathway, regulating tissue size, morphology and PrE gene activity. We propose that this platform will benefit to the systematic study of organogenesis in vitro.
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