Ampere-level reduction of pure nitrate by electron-deficient Ru with K ions repelling effect.

Electrochemical nitrate reduction reaction offers a sustainable and efficient pathway for ammonia synthesis. Maintaining satisfactory Faradaic efficiency for long-term nitrate reduction under ampere-level current density remains challenging due to the inevitable hydrogen evolution, particularly in pure nitrate solutions. Herein, we present the application of electron deficiency of Ru metals to boost the repelling effect of counter K ions via the electric-field-dependent synergy of interfacial water and cations, and thus largely promote nitrate reduction reaction with a high yield and well-maintained Faradaic efficiency under ampere-level current density.

Towards High-Performance Li-Rich Cathode Materials: from Morphology Design to Electronic Structure Modulation.

Lithium-rich cathode materials (LRMs) have garnered significant interest owing to their high reversible discharge capacity (exceeding 250 mAh g⁻¹), which is attributed to the redox reactions of transition metal (TM) ions as well as the distinctive redox processes of oxygen anions. However, there are still many problems, such as their relatively poor rate performance and voltage fading and hysteresis, hindering their practical applications. Herein, the recent insights into the mechanisms and the latest advancements in the research of LRMs are discussed.

Incorporation of Fe/FeO Nanoparticles into Interlinked -Doped Porous Carbon Nanofiber Networks to Realizing Sequential Catalytic Conversion of Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries (LSBs) with energy density (2600 Wh/kg) much higher than typical Li-ion batteries (150-300 Wh/kg) have received considerable attention. However, the insulation nature of solid sulfur species and the high activation barrier of lithium polysulfides (LiPSs) lead to slow sulfur redox kinetics. By the introduction of catalytic materials, the effective adsorption of LiPSs, and significantly reduced conversion, energy barriers are expected to be achieved, thereby sharpening electrochemical reaction kinetics and fundamentally addressing these challenges.

Boosting Propane Dehydrogenation to Propylene via Electron Hole-Hydrogen Coupling on Cobalt Metal Surface.

Nonoxidative dehydrogenation of propane is useful for the high selectivity to propylene but is suffering from the heavy coke deposition on the catalyst surface. Herein, we present a proof-of-concept application of a hole-hydrogen (H) couple on a metallic cobalt surface to decrease the deactivation rate. The coupled H atoms on the Cobalt (Co) surface, partially resulting from propane dehydrogenation, enabled the desorption of propylene to avoid deep hydrogenolysis and coke deposition and realize selective and durable propylene production, while conventional Co metal-based catalysts do not generate propylene.

Boosting the Efficiency and Stability of Li-CO Batteries via a Ruthenium-Based Olefin-Metathesis Catalyst.

The practical application of Li-CO batteries is significantly hindered by high charge potential and short lifespan, mainly due to sluggish reaction kinetics and inadequate reaction reversibility. Homogeneous catalysts added to the electrolyte provide a promising strategy to address these issues. In this work, the third-generation Grubbs catalyst (G-III), which is efficient for olefin metathesis reactions, has been adopted as a homogeneous catalyst for Li-CO batteries.

Electrocatalytic Aromatic Alcohols Splitting to Aldehydes and H Gas.

Selective electrocatalytic transformation of alcohols to aldehydes offers an efficient and environmentally friendly platform for the simultaneous production of fine chemicals and pure hydrogen gas. However, traditional alcohol oxidation reactions (AORs) in aqueous electrolyte unavoidably face competitive reactions (e.g.

Organometallic Polymer Constructed by Active Fe-CN Centers for Boosting Sodium-Ion Storage.

Organic-metal coordination materials with rich structural diversity are considered as promising electrode materials for rechargeable sodium-ion batteries. However, the electrochemical performance can be constrained by the limited number of active sites and structural instability under the discharge/charge process. Herein, organometallic polymer microspheres (Fe-PDA-220) with a unique d-π conjugated structure was designed and successfully constructed through a simple synchronous polymerization and coordination reactions.

Electrocatalytic water-to-oxygenates conversion: redox-mediated direct oxygen transfer.

Electrocatalytic oxygenation of hydrocarbons with high selectivity has attracted much attention for its advantages in the sustainable and controllable production of oxygenated compounds with reduced greenhouse gas emissions. Especially when utilizing water as an oxygen source, by constructing a water-to-oxygenates conversion system at the anode, the environment and/or energy costs of producing oxygenated compounds and hydrogen energy can be significantly reduced. There is a broad consensus that the generation and transformation of oxygen species are among the decisive factors determining the overall efficiency of oxygenation reactions.

Electron Divergence of Cu and Pd in CuPd Alloy-Based Heterojunctions Boosts Concerted C≡C Bond Binding and the Volmer Step for Alkynol Semihydrogenation.

Electrocatalytic semihydrogenation of alkynols presents a sustainable alternative to conventional thermal methodologies for the high-value production of alkenols. The design of efficient catalysts with superior catalytic and energy efficiency for semihydrogenation poses a significant challenge. Here, we present the application of an electron-divergent CuPd alloy-based heterojunction in promoting the electrocatalytic semihydrogenation of alkynols to alkenols using water as the proton source.

Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis.

The tunability of reaction pathways is required for exploring efficient and low cost catalysts for ammonia synthesis. There is an obstacle by the limitations arising from scaling relation for this purpose. Here, we demonstrate that the alkali earth imides (AeNH) combined with transition metal (TM = Fe, Co and Ni) catalysts can overcome this difficulty by utilizing functionalities arising from concerted role of active defects on the support surface and loaded transition metals.

Tailoring the growth route of lithium peroxide through the rational design of a sodium-doped nickel phosphate catalyst for lithium-oxygen batteries.

Tailoring the morphology and structure of LiO, the discharge product of lithium-oxygen batteries (LOBs), through the rational design of cathode catalysts is an efficient strategy to promote the electrochemical performance of LOBs. In this work, sodium-doped nickel phosphate nanorods (Na-NiPO NRs) grown on Ni foam (NF) were prepared by the hydrothermal method and subsequent calcination. For the Na-NiPO NRs, the electronic structure could be optimized and abundant void space among the nanorods would provide abundant transport channels.

Poly(-phenylenediamine)-Coated Metal-Organic Frameworks for High-Performance Sodium-Ion Batteries: The Balance of Capacity and Stability.

Metal-organic frameworks (MOFs) with well-defined porous structures and highly active frameworks are considered as promising electrode materials for sodium-ion batteries (SIBs). However, the structure pulverization upon sodiation/desodiation impacts on their practical application in SIBs. To address this issue, poly(-phenylenediamine) (PPA) was uniformly coated onto the surface of MIL-88A, a typical Fe-based MOF through in situ polymerization initiated by the metal ions (Fe) of MIL-88A.

Tailoring the Growth and Morphology of Lithium Peroxide: Nickel Sulfide/Nickel Phosphate Nanotubes with Optimized Electronic Structure for Lithium-Oxygen Batteries.

Heterogeneous crystalline-amorphous structures, with tunable electronic structures and morphology, hold immense promise as catalysts for lithium-oxygen batteries (LOBs). Herein, a nanotube network constructed by crystalline nickel sulfide/amorphous nickel phosphate (NiS/NiPO) heterostructure is prepared on Ni foam through the sulfurization of the precursor generated hydrothermally. Used as cathodes, the NiS/NiPO nanotubes with optimized electronic structure can induce the deposition of the highly porous and interconnected structure of Li O with rich Li O -electrolyte interfaces.

Light-driven Oxidative Demethylation Reaction Catalyzed by a Rieske-type Non-heme Iron Enzyme Stc2.

Rieske-type non-heme iron oxygenases/oxidases catalyze a wide range of transformations. Their applications in bioremediation or biocatalysis face two key barriers: the need of expensive NAD(P)H as a reductant and a proper reductase to mediate the electron transfer from NAD(P)H to the oxygenases. To bypass the need of both the reductase and NAD(P)H, using Rieske-type oxygenase (Stc2) catalyzed oxidative demethylation as the model system, we report Stc2 photocatalysis using eosin Y/sulfite as the photosensitizer/sacrificial reagent pair.

High-Performance PEO-Based All-Solid-State Battery Achieved by Li-Conducting High Entropy Oxides.

A rock-salt-structured Li-conducting high entropy oxide was prepared and utilized as an active filler in a polyethylene oxide (PEO)-based solid-state composite electrolyte. X-ray diffraction and high-resolution transmission electron microscopy were adopted to analyze the crystal structure of the high entropy oxide containing 20% of Li ions (HL20). The HL20 was crystallized in the 3̅ space group with Li ions located at the center of the MO octahedra.

The mechanism of in vitro non-enzymatic glycosylation inhibition by Tartary buckwheat's rutin and quercetin.

Tartary buckwheat is rich in rutin, quercetin, and other flavonoids, which exert prominent effects by inhibiting non-enzymatic glycosylation. In this study, an in vitro non-enzymatic glycosylation model was established, and the inhibitory effects of rutin and quercetin on the early, middle, and late products of non-enzymatic glycosylation were determined. Furthermore, their effects on the formation of advanced glycation end products (AGEs) and on protein functional groups and secondary structure were analyzed.

Design of the Synergistic Rectifying Interfaces in Mott-Schottky Catalysts.

The functions of interfacial synergy in heterojunction catalysts are diverse and powerful, providing a route to solve many difficulties in energy conversion and organic synthesis. Among heterojunction-based catalysts, the Mott-Schottky catalysts composed of a metal-semiconductor heterojunction with predictable and designable interfacial synergy are rising stars of next-generation catalysts. We review the concept of Mott-Schottky catalysts and discuss their applications in various realms of catalysis.

Young children with autism show atypical prefrontal cortical responses to humanoid robots: An fNIRS study.

Background: Previous behavioral studies have found that children with autism spectrum disorder (ASD) show greater interest in humanoid robots than in humans. However, the neural mechanism underlying this is not clear. This study compared brain activation patterns between children with ASD and neurotypical children while they watched videos with robots and humans.

Direct Oxygen Transfer from H O to Cyclooctene over Electron-Rich RuO Nanocrystals for Epoxidation and Hydrogen Evolution.

Production of more than 20 million tons of epoxides per year from olefins suffers from low atom economy due to the use of oxidants and complex catalysts with unsatisfactory selectivity, leading to huge environmental and economic costs. We present a proof-of-concept application of electron-rich RuO nanocrystals to boost the highly selective epoxidation of cyclooctene via direct oxygen transfer from water as the sole oxygen source under mild conditions. The enhanced electron enrichment of RuO nanocrystals via the Schottky effect with nitrogen-doped carbons largely promotes the capture and activation of cyclooctene to give a high turnover frequency (260 h ) of cyclooctene oxide, far surpassing the reported values (<20 h ) of benchmarked catalysts at room temperature with oxidants.

Novel design of cryptosystems for video/audio streaming via dynamic synchronized chaos-based random keys.

In this paper, a novel chaos-based cryptosystem is proposed to ensure the communication security of video/audio streaming in the network environment. Firstly, by the proposed synchronization controller for the master and slave chaotic systems, respectively, embedded in the transmitter and receiver, the cryptosystem can generate the synchronized and dynamic chaotic random numbers at the transmitter and receiver simultaneously. Then integrating the chaotic random numbers with SHA3-256 (Secure hash algorithm 3), the design of synchronized dynamic key generators (SDKGs) is completed.

Highly Reversible Zinc Anode Enabled by a Cation-Exchange Coating with Zn-Ion Selective Channels.

Rechargeable aqueous zinc-ion batteries (ZIBs) have attracted extensive attention due to their low cost and high safety. However, the critical issues of dendrite growth and side reactions on the Zn metal anode hinder the commercialization of ZIBs. Herein, we demonstrated that the formation of ZnSO(OH)·5HO byproducts is closely relevant to the direct contact between the Zn electrode and SO/HO.

Facilitating Hot Electron Injection from Graphene to Semiconductor by Rectifying Contact for Vis-NIR-Driven H O Production.

Solar-driven production of hydrogen peroxide (H O ), as an important industrial chemical oxidant with an extensive range of applications, from oxygen reduction is a sustainable alternative to mainstream anthraquinone oxidation and direct hydrogenation of dioxygen methods. The efficiency of solar to hydrogen peroxide over semiconductor-based photocatalysts is still largely limited by the narrow light absorption to visible light. Here, the authors proposed and demonstrate the proof-of-concept application of light-generated hot electrons in a graphene/semiconductor (exemplified with widely used TiO ) dyad to largely extend visible light spectra up to 800 nm for efficient H O production.

Boosting Mass Exchange between Pd/NC and MoC/NC Dual Junctions via Electron Exchange for Cascade CO Fixation.

Merging existing catalysts together as a cascade catalyst may achieve "one-pot" synthesis of complex but functional molecules by simplifying multistep reactions, which is the blueprint of sustainable chemistry with low pollutant emission and consumption of energy and materials only when the smooth mass exchange between different catalysts is ensured. Effective strategies to facilitate the mass exchange between different active centers, which may dominate the final activity of various cascade catalysts, have not been reached until now, even though charged interfaces due to work function driven electron exchange have been widely observed. Here, we successfully constructed mass (reactants and intermediates) exchange paths between Pd/N-doped carbon and MoC/N-doped carbon induced by interfacial electron exchange to trigger the mild and cascade methylation of amines using CO and H.