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Despite the growing demand for hydrogen peroxide it is almost exclusively manufactured by the energy-intensive anthraquinone process. Alternatively, H 2 O 2 can be produced electrochemically via the two-electron oxygen reduction reaction, although the performance of the state-of-the-art electrocatalysts is insufficient to meet the demands for industrialization. Interestingly, guided by first-principles calculations, we found that the catalytic properties of the Co–N 4 moiety can be tailored by fine-tuning its surrounding atomic configuration to resemble the structure-dependent catalytic properties of metalloenzymes. Using this principle, we designed and synthesized a single-atom electrocatalyst that comprises an optimized Co–N 4 moiety incorporated in nitrogen-doped graphene for H 2 O 2 production and exhibits a kinetic current density of 2.8 mA cm −2 (at 0.65 V versus the reversible hydrogen electrode) and a mass activity of 155 A g −1 (at 0.65 V versus the reversible hydrogen electrode) with negligible activity loss over 110 hours. Producing H 2 O 2 electrochemically currently use electrocatalysts that are insufficient to meet the demands for industrialization. A single-atom electrocatalyst with an optimized Co–N4 moiety incorporated in nitrogen-doped graphene is shown to exhibit enhanced performance for H 2 O 2 production.

The direct conversion of gaseous methane to energy‐dense liquid derivatives such as methanol and ethanol is of profound importance for the more efficient utilization of natural gas. However, the thermo‐catalytic partial oxidation of this simple alkane has been a significant challenge due to the high C−H bond energy. Exploiting electrocatalysis for methane activation via active oxygen species generated on the catalyst surface through electrochemical water oxidation is generally considered as economically viable and environmentally benign compared to energy‐intensive thermo‐catalysis. Despite recent progress in electrochemical methane oxidation to alcohol, the competing oxygen evolution reaction (OER) still impedes achieving high faradaic efficiency and product selectivity. In this review, an overview of current progress in electrochemical methane oxidation, focusing on mechanistic insights on methane activation, catalyst design principles based on descriptors, and the effect of reaction conditions on catalytic performance are provided. Mechanistic requirements for high methanol selectivity, and limitations of using water as the oxidant are discussed, and present the perspective on how to overcome these limitations by employing carbonate ions as the oxidant.

This study investigates the immobilization of dinuclear iridium‐imidazole complexes onto indium tin oxides for the electrochemical oxygen evolution reaction (OER) in acidic media. The immobilized iridium complexes show exceptional catalytic activity and stability, which are attributed to the facile cleavage of the elongated μO bonds between the two iridium metal centers. This cleavage leads to the formation of dangling oxygen, which plays a crucial role in facilitating thermochemical water dissociation. O2 is released through a dangling oxygen–participated mechanism, accompanied by the regeneration of the μO bonds. This unique OER mechanism, possibly specific to immobilized (strained) molecular catalysts, resembles the lattice oxygen participation mechanism reported for unstable oxides, but with the advantage of high stability in acidic media. This study not only identifies a new mechanism but can also inform the design of immobilized molecular catalysts with enhanced performance. Dinuclear iridium complexes immobilized on ITO surfaces enable highly efficient and stable oxygen evolution in acidic media. Through a novel mechanism involving the reversible cleavage/regeneration of distorted μ‐oxo bridges, the catalysts facilitate the thermochemically assisted dangling oxygen participation mechanism. This study unveils a unique and durable pathway for oxygen evolution, offering insights for next‐generation molecular electrocatalyst design.

The aim of the present study was to investigate the dependence of the high cycle fatigue property on the microporosity variation of a low-pressure die-cast A356 alloy. Also, it aimed to describe quantitatively the relationship between the fatigue property and monotonic tensile strength using modified Basquin’s equation which takes into account the microporosity variation. The fatigue life of the A356 alloy can be described by an exponential dependence on the variation of the fractographic porosity, in terms of the modified Basquin’s equation which is composed of the defect susceptibility of fatigue life to microporosity variation and the maximum tensile strength achievable in the defect-free condition. Using a modified form of Basquin’s equation, the maximum values of the fatigue strength coefficient and exponent in the defect-free condition are 341.5 MPa and −0.076, respectively, even though the nominal values of fatigue strength coefficient and exponent without consideration of microporosity variation are 237.6MPa and −0.048, respectively. Also, the difference between the maximum tensile strength and the fatigue strength coefficient on modified Basquin’s equation is about 120MPa, and it arises from variation in the deformation behavior due to the difference of loading condition between the monotonic and cyclic test modes such as the strain rate, Bauschinger effect, cyclic work hardening and damage accumulation on loading condition.

Density functional theory calculations are used to investigate thermal water decomposition over the close-packed (111), stepped (211), and open (100) facets of transition metal surfaces. A descriptor-based approach is used to determine that the (211) facet leads to the highest possible rates. A range of 96 binary alloys were screened for their potential activity and a rate control analysis was performed to assess how the overall rate could be improved. Graphical Abstract

A universal descriptor for the prediction of C–H bond activation barriers has been established, and combined with a thermodynamic analysis of methane activation, to provide design rules for various types of heterogeneous catalysts. While the search for catalysts capable of directly converting methane to higher value commodity chemicals and liquid fuels has been active for over a century, a viable industrial process for selective methane activation has yet to be developed 1 . Electronic structure calculations are playing an increasingly relevant role in this search, but large-scale materials screening efforts are hindered by computationally expensive transition state barrier calculations. The purpose of the present letter is twofold. First, we show that, for the wide range of catalysts that proceed via a radical intermediate, a unifying framework for predicting C–H activation barriers using a single universal descriptor can be established. Second, we combine this scaling approach with a thermodynamic analysis of active site formation to provide a map of methane activation rates. Our model successfully rationalizes the available empirical data and lays the foundation for future catalyst design strategies that transcend different catalyst classes.

Despite the growing demand for hydrogen peroxide it is almost exclusively manufactured by the energy-intensive anthraquinone process. Alternatively, H O can be produced electrochemically via the two-electron oxygen reduction reaction, although the performance of the state-of-the-art electrocatalysts is insufficient to meet the demands for industrialization. Interestingly, guided by first-principles calculations, we found that the catalytic properties of the Co-N moiety can be tailored by fine-tuning its surrounding atomic configuration to resemble the structure-dependent catalytic properties of metalloenzymes. Using this principle, we designed and synthesized a single-atom electrocatalyst that comprises an optimized Co-N moiety incorporated in nitrogen-doped graphene for H O production and exhibits a kinetic current density of 2.8 mA cm (at 0.65 V versus the reversible hydrogen electrode) and a mass activity of 155 A g (at 0.65 V versus the reversible hydrogen electrode) with negligible activity loss over 110 hours.

Reactive oxygen species (ROS) contribute to the development of non-alcoholic fatty liver disease. ROS generation by infiltrating macrophages involves multiple mechanisms, including Toll-like receptor 4 (TLR4)-mediated NADPH oxidase (NOX) activation. Here, we show that palmitate-stimulated CD11b + F4/80 low hepatic infiltrating macrophages, but not CD11b + F4/80 high Kupffer cells, generate ROS via dynamin-mediated endocytosis of TLR4 and NOX2, independently from MyD88 and TRIF. We demonstrate that differently from LPS-mediated dimerization of the TLR4–MD2 complex, palmitate binds a monomeric TLR4–MD2 complex that triggers endocytosis, ROS generation and increases pro-interleukin-1β expression in macrophages. Palmitate-induced ROS generation in human CD68 low CD14 high macrophages is strongly suppressed by inhibition of dynamin. Furthermore, Nox2 -deficient mice are protected against high-fat diet-induced hepatic steatosis and insulin resistance. Therefore, endocytosis of TLR4 and NOX2 into macrophages might be a novel therapeutic target for non-alcoholic fatty liver disease. Reactive species of oxygen promote the development of hepatic steatosis. Here, Kim et al. demonstrate that palmitate stimulates macrophage infiltration and increases oxidative stress during steatosis by binding to the TLR4–MD2 complex, which results in the activation of NOX2.

Epitranscriptomic features, such as single-base RNA editing, are sources of transcript diversity in cancer, but little is understood in terms of their spatial context in the tumour microenvironment. Here, we introduce spatial-histopathological examination-linked epitranscriptomics converged to transcriptomics with sequencing (Select-seq), which isolates regions of interest from immunofluorescence-stained tissue and obtains transcriptomic and epitranscriptomic data. With Select-seq, we analyse the cancer stem cell-like microniches in relation to the tumour microenvironment of triple-negative breast cancer patients. We identify alternative splice variants, perform complementarity-determining region analysis of infiltrating T cells and B cells, and assess adenosine-to-inosine base editing in tumour tissue sections. Especially, in triple-negative breast cancer microniches, adenosine-to-inosine editome specific to different microniche groups is identified. The spatial context of epitranscriptomic features in the tumour microenvironment remains poorly understood. Here, a method for transcriptomic and epitranscriptomic analysis of immunofluorescence-stained tissue, Select-seq, is applied to stem cell-like microniches in triple negative breast cancer.