All-solid-state batteries (ASSBs) possess the advantage of ensuring safety while simultaneously maximizing energy density, making them suitable for next-generation battery models. In particular, sulfide solid electrolytes (SSEs) are viewed as promising candidates for ASSB electrolytes due to their excellent ionic conductivity. However, a limitation exists in the form of interfacial side reactions occurring between the SSEs and cathode active materials (CAMs), as well as the generation of sulfide-based gases within the SSE.
View Article and Find Full Text PDFNanoscale bubbles form inevitably during the transfer of two-dimensional (2D) materials on a target substrate due to their van der Waals interaction. Despite a large number of studies based on nanobubble structures with localized strain, the dielectric constant (κ) in nanobubbles of MoS is poorly understood. Here, we report κ measurements for nanobubbles on MoS by probing the polarization forces based on electrostatic force microscopy.
View Article and Find Full Text PDFThe catalytic redox activity of Cu(II) bound to the amino-terminal copper and nickel (ATCUN) binding motif (Xxx-Zzz-His, XZH) is stimulating the development of catalytic metallodrugs based on reactive oxygen species (ROS)-mediated biomolecule oxidation. However, low Cu(I) availability resulting from the strong Cu(II) binding affinity of the ATCUN motif is regarded as a limitation to efficient ROS generation. To address this, we replaced the imidazole moiety (p 7.
View Article and Find Full Text PDFPlatinum single-atom catalysts hold promise as a new frontier in heterogeneous electrocatalysis. However, the exact chemical nature of active Pt sites is highly elusive, arousing many hypotheses to compensate for the significant discrepancies between experiments and theories. Here, we identify the stabilization of low-coordinated Pt species on carbon-based Pt single-atom catalysts, which have rarely been found as reaction intermediates of homogeneous Pt catalysts but have often been proposed as catalytic sites for Pt single-atom catalysts from theory.
View Article and Find Full Text PDFSecuring the electrochemical durability of noble metal platinum is of central importance for the successful implementation of a proton exchange membrane fuel cell (PEMFC). Pt dissolution, a major cause of PEMFC degradation, is known to be a potential-dependent transient process, but its underlying mechanism is puzzling. Herein, we elucidate a chemical Pt dissolution process that can occur in various electrocatalytic conditions.
View Article and Find Full Text PDFWe report a local mapping photoresponse of WSe using a second-harmonic (2w) channel based on nondestructive electrostatic force microscopy (EFM). The 2w signals resulting from interaction between WSe and EFM tip are intrinsically related to the electrical conductivity of WSe. The photoresponse images and rise/decay time constants of WSe are obtained by local mapping 2w signals under illumination.
View Article and Find Full Text PDFSingle-atom catalysts (SACs) featuring atomically dispersed metal cations covalently embedded in a carbon matrix show significant potential to achieve high catalytic performance in various electrocatalytic reactions. Although considerable advances have been achieved in their syntheses and electrochemical applications, further development and fundamental understanding are limited by a lack of strategies that can allow the quantitative analyses of their intrinsic catalytic characteristics, that is, active site density (SD) and turnover frequency (TOF). Here we show an SD quantification method using a cyanide anion as a probe molecule.
View Article and Find Full Text PDFElectrocatalytic conversion of nitrogen oxides to value-added chemicals is a promising strategy for mitigating the human-caused unbalance of the global nitrogen-cycle, but controlling product selectivity remains a great challenge. Here we show iron-nitrogen-doped carbon as an efficient and durable electrocatalyst for selective nitric oxide reduction into hydroxylamine. Using in operando spectroscopic techniques, the catalytic site is identified as isolated ferrous moieties, at which the rate for hydroxylamine production increases in a super-Nernstian way upon pH decrease.
View Article and Find Full Text PDFElectrocatalytic conversion of CO into value-added products offers a new paradigm for a sustainable carbon economy. For active CO electrolysis, the single-atom Ni catalyst has been proposed as promising from experiments, but an idealized Ni-N site shows an unfavorable energetics from theory, leading to many debates on the chemical nature responsible for high activity. To resolve this conundrum, here we investigated CO electrolysis of Ni sites with well-defined coordination, tetraphenylporphyrin (N-TPP) and 21-oxatetraphenylporphyrin (NO-TPP).
View Article and Find Full Text PDFSingle-atom catalysts (SACs) have quickly emerged as a new class of catalytic materials. When confronted with classical carbon-supported nanoparticulated catalysts (Pt/C), SACs are often claimed to have superior electrocatalytic properties, e.g.
View Article and Find Full Text PDFFood Addit Contam Part A Chem Anal Control Expo Risk Assess
March 2020
Heterocyclic amines (HCAs) are potent mutagens generated by the high temperatures of the cooking process. The purpose of this study was to develop and validate analytical methods for HCAs determination using high-performance liquid chromatography-tandem mass spectrometry in seven food matrices: corn oil, milk, 20% ethanol, pork, flat fish, sea mustard (), and radish. Six isotopically labelled internal standards were used for quantitation, and Chem Elut and Oasis hydrphilic-liphophilic balance cartridges were applied for sample preparation to remove interferences.
View Article and Find Full Text PDFThe free energy of H adsorption () on a metallic catalyst has been taken as a descriptor to predict the hydrogen evolution reaction (HER) kinetics but has not been well applied in alkaline media. To assess this, we prepare Pd@Pt and PdH@Pt core-shell octahedra enclosed by Pt(111) facets as model catalysts for controlling the affected by the ligand, the strain, and their ensemble effects. The Pt shell thickness is adjusted from 1 to 5 atomic layers by varying the amount of Pt precursor added during synthesis.
View Article and Find Full Text PDFCarbon monoxide is widely known to poison Pt during heterogeneous catalysis owing to its strong donor-acceptor binding ability. Herein, we report a counterintuitive phenomenon of this general paradigm when the size of Pt decreases to an atomic level, namely, the CO-promoting Pt electrocatalysis toward hydrogen evolution reactions (HER). Compared to pristine atomic Pt catalyst, reduction current on a CO-modified catalyst increases significantly.
View Article and Find Full Text PDFObjective: The purpose of this study is to determine the optimal energy level of virtual monochromatic images from spectral CT compared with conventional polychromatic images for reducing beam-hardening artifacts caused by contrast media in the thorax.
Materials And Methods: A total of 101 consecutive patients who underwent chest CT with contrast enhancement were retrospectively included in this study. The same contrast media and injection protocols were applied to the whole study population.
Heterocyclic amines (HCAs) and acrylamide are unintended hazardous substances generated by heating or processing of foods and are known as carcinogenic and mutagenic agents by the animal experiments. A simple method was established for a rapid and accurate determination of 12 types of HCAs (IQ, MeIQ, Glu-P-1, Glu-P-2, MeIQx, Trp-P-1, Trp-P-2, PhIP, AαC, MeAαC, Harman and Norharman) and acrylamide in three food matrices (non-fat liquid, non-fat solid and fat solid) by isotope dilution liquid chromatography-tandem mass spectrometry (LC-MS/MS). In every sample, a mixture of internal standards including IQ-d3, MeIQx-d3, PhIP-d3, Trp-P-2-(13)C2-(15)N and MeAαC-d3 was spiked for quantification of HCAs and (13)C3-acrylamide was also spiked for the analysis of acrylamide.
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