Mechanistic Study on Oxygen Reduction Reaction in High-Concentrated Electrolytes for Aprotic Lithium-Oxygen Batteries.

Highly concentrated electrolytes (HCEs) have energized the development of high-energy-density lithium metal batteries by facilitating the formation of robust inorganic-derived solid electrolyte interfaces on the lithium anode. However, the oxygen reduction reaction (ORR) occurring on the cathode side remains ambiguous in HCE-based lithium-oxygen (Li-O) batteries. Herein, we investigate the ORR mechanism in a highly concentrated LiTFSI-CHCN electrolyte using ultra-microelectrode voltammetry coupled with in situ spectroscopies.

Heterogeneous Carbonylation of Alcohols on Charge-Density-Distinct Mo-Ni Dual Sites Localized at Edge Sulfur Vacancies.

Alcohols carbonylation is of great importance in industry but remains a challenge to abandon the usage of the halide additives and noble metals. Here we report the realization of direct alcohols heterogeneous carbonylation to carbonyl-containing chemicals, especially in methanol carbonylation, with a remarkable space-time-yield (STY) of 4.74 mol/kg/h and a durable stability as long as 100 h on Ni@MoS catalyst.

Loss of USP10 promotes hepatocellular carcinoma proliferation by regulating the serine synthesis pathway through inhibition of LKB1 activity.

Metabolic dysregulation is emerging as a critical factor in tumorigenesis, and reprogramming of serine metabolism has been identified as an essential factor in the progression of hepatocellular carcinoma (HCC). Studies have shown that LKB1 deficiency can activate mTOR to upregulate the serine synthesis pathway (SSP) and promote tumor progression. Our team discovered that ubiquitin-specific protease 10 (USP10) can inhibit HCC proliferation through mTOR, but its relationship with SSP needs further investigation.

Cooperative Diarylborinic Acid/Chloride-Catalyzed Formal Si Reaction of -4-Hydroxymethyl-1,2-Cyclopentene Oxides.

A catalytic formal Si reaction was designed to achieve stereoretentive products for -4-hydroxymethyl-1,2-cyclopentene oxides by using diarylborinic acid as a dual role catalyst and chloride as a catalytic transient nucleophile through a double-displacement mechanism. This reaction offers the advantages of a low catalyst loading of 0.1 mol % and wide substrate scope, even including -substituents.

An Artificial Leaf with Patterned Photocatalysts for Sunlight-Driven Water Splitting.

Plant leaves can turn entirely absorbed light into chemical energy due to their spatially separated photosystems I and II in the thylakoid membrane that enables unidirectional Z-scheme type charge transfer between them. In artificial systems that mimic leaves, a lack of spatial and interfacial control of active units (i.e.

Calculations of Dissociation Dynamics of CHOH on a Global Potential Energy Surface Reveal the Mechanism for the Formation of HCOH; Roaming Plays a Role.

The experimental observation of hydroxymethylene, HCOH, following excitation of methanol at 193 nm, was reported recently (Hockey, E. K.; McLane, N.

Highly active manganese nitride-europium nitride catalyst for ammonia synthesis.

The development of efficient catalysts for ammonia synthesis under mild conditions is critical for establishing a carbon-neutral society powered by renewable ammonia. While significant effort has been focused on Fe and Ru-based catalysts, there have been very limited studies on manganese-based catalysts for ammonia synthesis because of their low intrinsic catalytic activity. Herein, we report that the synergy between manganese nitride (MnN) and europium nitride (EuN) yields an ammonia synthesis rate that is 41 and 25 times higher than that of neat MnN and EuN, respectively.

Over 21% Efficient Cesium Lead Triiodide Solar Cell Enabled by Molten Salt Accelerating the Crystallization Processes.

High-quality CsPbI with low defect density is indispensable for acquiring excellent photoelectric performance. Meticulous regulation of the CsPbI crystal growth processes is both feasible and efficacious in enhancing the quality of perovskite films. In this study, the cesium formate (CsFo) is introduced.

Effects of isoprene on the ozonolysis of Δ-carene and β-caryophyllene: Mechanisms of secondary organic aerosol formation and cross-dimerization.

Elucidating the mutual effects between the different volatile organic compounds (VOCs) is crucial for comprehending the formation mechanism of atmospheric secondary organic aerosols (SOA). Here, the mixed VOCs experiments of isoprene and Δ-carene/β-caryophyllene were carried out in the presence of O using an indoor smog chamber. The suppression effect of isoprene was recognized by the scanning mobility particle sizer spectrometer, online vacuum ultraviolet free electron laser (VUV-FEL) photoionization aerosol mass spectrometry, and quantum chemical calculations.

Peroxymonosulfate promoted dioxygen activation with Mn(II)-nitrilotriacetic acid complexes for sulfadiazine degradation.

In the field of peroxymonosulfate (PMS) activation technology, there is a pressing need to reduce PMS consumption and enhance its utilization rate. The present study demonstrates that the introduction of dissolved oxygen (DO) into the Mn(II)-nitrilotriacetic acid (NTA)-activated PMS system significantly enhances the degradation efficiency of sulfadiazine and increases the PMS utilization rate from approximately 15.0 to 41.

Preparation of Stainless Steel Superhydrophobic Surface and Analysis of Hydrophobic Mechanism.

By analyzing the application conditions of hydrothermal oxidation equipment, we found that the corrosion resistance of stainless steel is crucial. It is necessary to prepare superhydrophobic surface to improve the corrosion resistance and find a cost-effective and environmentally friendly preparation method. Therefore, this paper proposes a method combining nanosecond laser and post-treatment, which uses nanosecond laser to etch microstructure and reduces the surface energy through diverse post-treatment methods to achieve hydrophobicity.

Facet-Engineered BiVO Photocatalysts for Water Oxidation: Lifetime Gain Versus Energetic Loss.

A limiting factor to the efficiency of water Oxygen Evolution Reaction (OER) in metal oxide nanoparticle photocatalysts is the rapid recombination of holes and electrons. Facet-engineering can effectively improve charge separation and, consequently, OER efficiency. However, the kinetics behind this improvement remain poorly understood.

Preparation of High Vibrational States in the Entire Molecular Beam.

Preparing highly excited molecules is of great interest in chemistry, but it has long been a challenge due to the high laser power required within the narrow line width to excite a weak transition. We present a cavity-enhanced infrared excitation scheme using a milliwatt laser. As a demonstration, about 35% of CO molecules in a ground-state rotational level were excited to the highly excited = 3 state in the entire pulsed supersonic beam, as confirmed by the depletion of molecules in the ground state.

Submicroscopic magnetite may be ubiquitous in the lunar regolith of the high-Ti region.

Magnetite is rare on the Moon. The ubiquitous presence of magnetite in lunar soil has been hypothesized in previous Apollo Mössbauer spectroscopy and electron spin resonance studies, but there is currently no mineralogical evidence to prove it. Here, we report a large number of submicroscopic magnetite particles embedded within iron-sulfide on the surface of Chang'e-5 glass, with a close positive correlation between magnetite content and the TiO content of the surrounding glass.

Insights into dioxygen binding on metal centers: an multireference electronic structure analysis.

Why does binding of dioxygen (O) to metal centers, the initial step of O storage, transportation, and activation, almost inevitably induce metal-to-O single-electron transfer and generate superoxo (O˙) species, instead of genuine O02 adducts? To address this question, this study describes highly correlated wavefunction-based calculations using CASSCF/NEVPT2 (CASSCF = complete active space self-consistent field, and NEVPT2 = -electron valence state second-order perturbation theory) approaches to explore the electronic-structure evolution of O association on Fe(II)(BDPP) (HBDPP = 2,6-bis((2-()-diphenylhydroxylmethyl-1-pyrrolidinyl)methyl)pyridine) and Co(II)(BDPP) to produce = 3 Fe(III)(BDPP)(O˙) (1) and Co(III)(BDPP)(O˙) (2). CASSCF/NEVPT2 calculations suggest that the processes furnishing 1 and 2 feature an avoided crossing resulting from interactions of two diabatic curves, of which one is characterized as Co(II) and Fe(II) centers interacting with a triplet O ligand and the other as Co(III) and Fe(III) centers bound to a superoxo ligand. In both cases, the avoided crossing induces a one-electron transfer from the divalent metal center to the incoming O ligand and leads to formation of trivalent metal-O˙ complexes.

Polyoxometalate-incorporated NiFe-based oxyhydroxides for enhanced oxygen evolution reaction in alkaline media.

NiFe-based oxyhydroxides are promising electrocatalysts for the oxygen evolution reaction (OER) in alkaline media, but further enhancing their OER performance remains a significant challenge. Herein, we incorporated polyoxometalates into NiFe oxyhydroxides to form a homogeneous/heterogeneous hybrid material, which induces the electronic interaction between Ni, Fe and Mo sites, as revealed by a variety of characterization experiments and theoretical calculations. The resulting hybrid electrocatalyst delivers a low overpotential of 203 mV at 10 mA cm and a TOF of 2.

Electron Sponge Effect by Dynamic-Regulated Electron Self-Flow toward Coupled Electrochemical Ammonia Synthesis.

A dynamic-regulated Pd-Fe-N electrocatalyst was effectively constructed with electron-donating and back-donating effects, which serves as an efficient engineering strategy to optimize the electrocatalytic activity. The designed PdFe/FeN features a comprehensive electrocatalytic performance toward the nitrogen reduction reaction (NRR, yield rate of 29.94 μg h mg and FE of 38.

Assessment of nanotoxicity in a human placenta-on-a-chip from trophoblast stem cells.

Maternal exposure to nanoparticles during gestation poses potential risks to fetal development. The placenta, serving as a vital interface for maternal-fetal interaction, plays a pivotal role in shielding the fetus from direct nanoparticle exposure. However, the impact of nanoparticles on placental function is still poorly understood, primarily due to the absence of proper human placental models.

Design and fabrication of acorn-like Janus molecularly imprinted materials for highly specific separation and enrichment of oxytetracycline from restaurant oily wastewater.

Molecularly imprinted polymer (MIP) is dedicated to the adsorption of target substances in the aqueous phase, but ignores the adsorption in a more complex environment (oily wastewater). In order to explore the application field of existing MIPs, acorn-like Janus particles were fabricated by photo-initiated seed swelling polymerization. A novel amphiphilic Janus-MIP was prepared with the acorn-like Janus particles as matrix, methacrylic acid, ethylene dimethacrylate and oxytetracycline (OTC) as functional monomers, crosslinking agents and template molecules via surface initiated-atom transfer radical polymerization (SI-ATRP).

Identification of AS1842856 as a novel small-molecule GSK3α/β inhibitor against Tauopathy by accelerating GSK3α/β exocytosis.

Glycogen synthase kinase-3α/β (GSK3α/β) is a critical kinase for Tau hyperphosphorylation which contributes to neurodegeneration. Despite the termination of clinical trials for GSK3α/β inhibitors in Alzheimer's disease (AD) treatment, there is a pressing need for novel therapeutic strategies targeting GSK3α/β. Here, we identified the compound AS1842856 (AS), a specific forkhead box protein O1 (FOXO1) inhibitor, reduced intracellular GSK3α/β content in a FOXO1-independent manner.

Breaking the Conversion-Selectivity Trade-Off in Methanol Synthesis from CO Using Dual Intimate Oxide/Metal Interfaces.

The selective hydrogenation of carbon dioxide (CO) to value-added chemicals, e.g., methanol, using green hydrogen retrieved from renewable resources is a promising approach for CO emission reduction and carbon resource utilization.