Go with the flow for high-throughput electrochemistry
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Bipolar electrochemistry-driven wireless drug loading and energy harvesting in conductive hybrid hydrogels
Bipolar electrochemistry enables wireless and spatially controlled redox reactions on (semi)conductive objects immersed in an electrolyte. Here, we investigate advanced bipolar electrochemistry applications using flexible bipolar electrodes coated with hybrid films of conductive polymer poly(3,4-ethylenedioxythiophene) and alginate hydrogels. These coatings allow for the wireless creation of reversible redox and chemical gradients, providing targeted drug loading and energy harvesting opportunities. We use cyclic voltammetry, electrochemical impedance spectroscopy, Raman microscopy, and X-ray photoelectron spectroscopy to characterize distinct redox regions within the bipolar electrode. The wireless and selective loading of a model drug, fluorescein, into the hydrogel, demonstrated control over drug distribution, suggesting an alternative to conventional uniform doping techniques. Furthermore, cutting the gradient-encoded bipolar electrode and closing an external circuit between the halves, enables energy recovery through a concentration cell mechanism. Our findings illustrate the potential of bipolar electrochemistry in creating versatile platforms that bridge materials science, electrochemistry, and bioelectronics for innovative biomedical and energy applications.
Revealing the molecular interplay of coverage, wettability, and capacitive response at the Pt(111)-water solution interface under bias
While electrified interfaces are crucial for electrocatalysis and corrosion, their molecular morphology remains largely unknown. Through highly realistic ab initio molecular dynamics simulations of the Pt(111)-water solution interface in reducing conditions, we reveal a deep interconnection among electrode coverage, wettability, capacitive response, and catalytic activity. We identify computationally the experimentally hypothesised states for adsorbed hydrogen on Pt, HUPD and HOPD, revealing their role in governing interfacial water reorientation and hydrogen evolution. The transition between these two H states with increasing potential, induces a shift from a hydrophobic to a hydrophilic interface and correlates with a change in the primary electrode screening mechanism. This results in a slope change in differential capacitance, marking the onset of the experimentally observed peak around the potential of zero charge. Our work produces crucial insights for advancing electrocatalytic energy conversion, developing deep understanding of electrified interfaces.
Phosphorylation of endothelial histone H3.3 serine 31 by PKN1 links flow-induced signaling to proatherogenic gene expression
Atherosclerotic lesions develop preferentially in arterial regions exposed to disturbed blood flow, where endothelial cells acquire an inflammatory phenotype. How disturbed flow induces endothelial cell inflammation is incompletely understood. Here we show that histone H3.3 phosphorylation at serine 31 (H3.3S31) regulates disturbed-flow-induced endothelial inflammation by allowing rapid induction of FOS and FOSB, required for inflammatory gene expression. We identified protein kinase N1 (PKN1) as the kinase responsible for disturbed-flow-induced H3.3S31 phosphorylation. Disturbed flow activates PKN1 in an integrin α5β1-dependent manner and induces its translocation into the nucleus, and PKN1 is also involved in the phosphorylation of the AP-1 transcription factor JUN. Mice with endothelium-specific PKN1 loss or endothelial expression of S31 phosphorylation-deficient H.3.3 mutants show reduced endothelial inflammation and disturbed-flow-induced vascular remodeling in vitro and in vivo. Together, we identified a pathway whereby disturbed flow through PKN1-mediated histone phosphorylation and FOS/FOSB induction promotes inflammatory gene expression and vascular inflammation.
High-throughput multiplexed serology via the mass-spectrometric analysis of isotopically barcoded beads
In serology, each sample is typically tested individually, one antigen at a time. This is costly and time consuming. Serology techniques should ideally allow recurrent measurements in parallel in small sample volumes and be inexpensive and fast. Here we show that mass cytometry can be used to scale up multiplexed serology testing by leveraging polystyrene beads uniformly loaded with combinations of stable isotopes. We generated 18,480 unique isotopically barcoded beads to simultaneously detect, in a single tube with 924 serum samples, the levels of immunoglobulins G and M against 19 proteins from SARS-CoV-2 (a total of 36,960 tests in 400 nl of sample volume and 30 μl of reaction volume). As a rapid, high-throughput and cost-effective technique, serology by mass cytometry may contribute to the effective management of public health emergencies originating from infectious diseases.
An artificial market model for the forex market
As financial markets have transitioned toward electronic trading, there has been a corresponding increase in the number of algorithmic strategies and degree of transaction frequency. This move to high-frequency trading at the millisecond level, propelled by algorithmic strategies, has brought to the forefront short-term market reactions, like market impact, which were previously negligible in low-frequency trading scenarios. Such evolution necessitates a new framework for analyzing and developing algorithmic strategies in these rapidly evolving markets. Employing artificial markets stands out as a solution to this problem. This study aims to construct an artificial foreign exchange market referencing market microstructure theory, without relying on the assumption of information or technical traders. Furthermore, it endeavors to validate the model by replicating stylized facts, such as fat tails, which exhibit a higher degree of kurtosis in the return distribution than that predicted by normal distribution models. The validated artificial market model will be used to simulate market dynamics and algorithm strategies; its generated rates could also be applied to pricing and risk management for currency options and other foreign exchange derivatives. Moreover, this work explores the importance of order flow and the underlying factors of stylized facts within the artificial market model.
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