Blomduggan2877

Our results call into question the high efficiency of layered Mn oxides toward OER under alkaline conditions and also elucidate the significant role of Ni and Fe impurities in the electrolyte in the presence of layered Mn oxide toward OER under alkaline conditions. Overall, a computational model supports the conclusions from the experimental structural and electrochemical characterizations. In particular, substitutional doping with Fe decreases the thermodynamic OER overpotential up to 310 mV. Besides, the thermodynamic OER onset potential calculated for the Fe-free structures is higher than 1.7 V (vs RHE) and, thus, not in the stability range of Mn oxides.The cleavage-site specificities for many proteases are not well understood, restricting the utility of supervised classification methods. We present an algorithm and web interface to overcome this limitation through the unsupervised detection of overrepresented patterns in protein sequence data, providing insight into the mixture of protease activities contributing to a complex system. Here, we apply the RObust LInear Motif Deconvolution (RoLiM) algorithm to confidently detect substrate cleavage patterns for SARS-CoV-2 MPro protease in the N-terminome data of an infected human cell line. Using mass spectrometry-based peptide data from a case-control comparison of 341 primary urothelial bladder cancer cases and 110 controls, we identified distinct sequence motifs indicative of increased matrix metallopeptidase activity in urine from cancer patients. The evaluation of N-terminal peptides from patient plasma post-chemotherapy detected novel granzyme B/corin activity. RoLiM will enhance the unbiased investigation of peptide sequences to establish the composition of known and uncharacterized protease activities in biological systems. RoLiM is available at http//langelab.org/rolim/.Dynamic nuclear polarization (DNP) is a powerful method to enhance NMR sensitivity. Much progress has been achieved recently to optimize DNP performance at high magnetic fields in solid-state samples, mostly by utilizing the solid or the cross effect. In liquids, only the Overhauser mechanism is active, which exhibits a DNP field profile matching the EPR line shape of the radical, distinguishable from other DNP mechanisms. Here, we observe DNP enhancements with a field profile indicative of the solid effect and thermal mixing at ∼320 K and a magnetic field of 9.4 T in the fluid phase of 1,2-dimyristoyl-sn-glycero-3-phosphocholine (DMPC) lipid bilayers doped with the radical BDPA (1,3-bis(diphenylene)-2-phenylallyl). This interesting observation might open up new perspectives for DNP applications in macromolecular systems at ambient temperatures.Precisely tailoring the nitrogen defects has been verified to be a promising approach for promoting the photocatalytic efficiency of C3N4. Herein, two-coordinated-N vacancies are selectively introduced into the C3N4 framework by a facile Cl- modification method, whereas its concentration can be facilely tuned by varying Cl- usage in the process of thermal polymerization. Impressively, the optimal defective C3N4 (20 mg) exhibited superior hydrogen and oxygen evolution rates of 48.2 and 21.8 μmol h-1, respectively, in photocatalytic overall water splitting and an apparent quantum efficiency of 6.9% at 420 nm, the highest of reported single-component C3N4 photocatalysts for overall water splitting. Systematic studies including XPS, DFT simulations, and NEXAFS reveal that Cl- modification preferentially facilitates the introduction of two-coordinated-N vacancies through tuning the formation energy and promotes charge carrier separation efficiency, thereby greatly enhancing the photocatalytic efficiency. This work allows for a viable approach to rationally designing defective C3N4 for efficient photocatalysis.The hydrophobicity of nanoparticles (NPs) is one of the most important physicochemical properties that determines their agglomeration state under various environmental conditions. When studying nano-bio interactions, it is found that the hydrophobicity of NPs plays a predominant role in mediating the biological response and toxicity of the NPs. Although many methods have been developed to qualitatively or quantitatively determine hydrophobicity, there is not yet a scientific consensus on the standard of characterizing the hydrophobicity of NPs. We have developed a novel optical method, called the maximum particle dispersion (MPD), for quantitatively characterizing the hydrophobicity of NPs. The principle of measurement of the MPD method lies in the control of the aggregation state of the NPs via manipulating the van der Waals interactions between NPs across a dispersion liquid. We have scrutinized the mechanism of the MPD method using a combination of dynamic light scattering and atomic force microscopy and further verified the MPD method using a completely independent dye adsorption method. The MPD method demonstrated great promise to be developed into an easy-to-use and cost-effective method for quantitatively characterizing the hydrophobicity of NPs.In immunobead-based assays, micro/nanobeads are functionalized with antibodies to capture the target analytes, which can significantly improve the assay's performance. The immunobead-based assays have been recently combined with microfluidic mixing devices and customized for a variety of applications. However, device design and process optimization to achieve the best performance remain a substantial technological challenge. Here, we introduce a computational model that enables the rational design and optimization of the immunobead-based assay in a microfluidic mixing channel. We use numerical methods to examine the effect of the flow rates, channel geometry, bead's trajectory, and the analyte and reagent characteristics on the efficiency of analyte capture on the surface of microbeads. This model accounts for different bead movements inside the microchannel, with the goal of simulating an actual active binding environment. The model is further validated experimentally where different microfluidic channels are tested to capture the target analytes. Our experimental results are shown to meet theoretical predictions. While the model is demonstrated here for the analysis of IgG capture in simple and herringbone-structured microchannels, it can be readily adapted to a broad range of target molecules and different device designs.Photoelectrochemical (PEC) sensors are usually based on a single output signal, that is, the photocurrent change caused by the (photoelectro)chemical reaction between target analytes and photoelectrodes. However, the photocurrent may be influenced by redox species other than the target analyte; therefore, modifying the surface of photoelectrodes with probes that selectively bind to the analyte is essential. Moreover, even though various surface modification methods have been developed, distinguishing molecularly similar chemicals using PEC sensing systems remains a significant challenge. To address these selectivity issues, we proposed a photoanode-based PEC sensor that utilizes a cathodic transient current as a second output signal in addition to the photocurrent, which arises from the back reduction of photo-oxidized species. Factors influencing the back reduction were investigated by observing the transient photocurrent of hematite photoanodes in the presence of model redox probes. The chemical environment around the electrode-electrolyte interface was manipulated by altering the electrolyte composition or modifying the electrode surface. The favorable interaction between the electrode surface and redox species led to an increase in the extent of back reduction and the cathodic transient current. VH298 inhibitor In addition, the extent of back reduction also depends on the chemical identity of the redox species, such as the kinetics of subsequent chemical reactions. Therefore, the synergistic combination of the photocurrent and the cathodic transient current enabled the differentiated detection of various catecholamine neurotransmitters with a single pristine photoelectrode, which has never been achieved using traditional PEC methods. Revisiting the transient photocurrent can complement conventional PEC applications and offers possibilities for more effective semiconductor-based applications.Although plenty of superhydrophobic surfaces have been developed owing to their tremendous potential applications, it is still a great challenge for the superhydrophobic surfaces to possess environmental friendliness, biocompatibility, and mechanical durability simultaneously. Herein, a non-fluorinated flexible superhydrophobic surface was designed by constructing a film-substrate system with labyrinth-like wrinkles combining an intrinsically hydrophobic Zn film and a polydimethylsiloxane (PDMS) substrate. Excellent superhydrophobicity with a contact angle up to 168.5° and a slide angle as low as 0° has been achieved on the Zn/PDMS surface, which is attributed to the micro-/nano-textured structures of the labyrinth-like wrinkles, providing sufficient air pockets to form a stable Cassie-Baxter state. Furthermore, the Zn/PDMS surface retains excellent superhydrophobicity under stretching, bending, and twisting mechanical deformation up to 500 cycles due to the stability of the micro-/nano-textured structures of the labyrinth-like wrinkles protected by the fantastic self-healing ability of the micro-cracks. Additionally, the Zn/PDMS superhydrophobic surface possesses an outstanding self-cleaning performance for various contaminants. The present work provides a valuable routine to design non-fluorinated flexible superhydrophobic surfaces with superb mechanical durability and self-cleaning property as promising functional layers for flexible electronics, wearable devices, biomedical engineering, and so forth.The recent commercial success of flexible and foldable displays has resulted in growing interest in stretchable electronics which are considered to be the next generation of the optoelectronic technology. Stretchable display technologies are being intensively studied for versatile applications including wearable, attachable, and shape changeable electronics. In this paper, we present high fill factor, stretchable inorganic light-emitting diode (LED) displays fabricated by connecting mini-LEDs and stretchable interconnects in a double-layer modular design. The double-layer modular design enables an increased areal coverage of LEDs and stretchable interconnectors with both electrical and mechanical stability. The main features of the double-layer modular design, fabrication processes, and device characteristics for the high fill factor, stretchable inorganic LED display are discussed, with experimental and computational results. Demonstrations of a passive matrix LED display confirm the potential value of the multi-layer structured, stretchable electronics in a wide range of applications that need high fill factor with high stretchability.Carbon nanoarchitectures derived from biobased building blocks are potential sustainable alternatives to electrode materials generated with petroleum-derived resources. We aim at developing a fundamental understanding on the connection between the structure and electrochemical performance of porous carbon nanofiber (PCNF) architectures from the polysaccharide chitosan as a biobased building block. We fabricated a range of PCNF architectures from the chitosan carbon precursor and tailored their structure by varying the amount and molecular weight of the sacrificial pore-forming polymer poly(ethylene oxide). The morphology (high-resolution scanning electron microscopy), carbon structure (X-ray diffraction, transmission electron microscopy), pore network (N2 gas adsorption, small-angle X-ray scattering), and surface/bulk composition (X-ray photoelectron spectroscopy, energy-dispersive X-ray spectroscopy) were studied in detail together with a comprehensive electrochemical analysis on the fabricated electrodes. In supercapacitor devices, the best-performing freestanding electrode had (1) a high accessible surface area (as,BET ≈ 700 m2 g-1) and hierarchical pore network (micro- and mesopores) providing a fast ion diffusion process, high specific capacitance, and rate capability, (2) surface chemistry allowing a high Coulombic efficiency by avoiding parasitic Faradaic side reactions, and (3) a unique turbostratic carbon nanostructure leading to low charge transfer resistance while keeping good electrical conductivity.