Activating Lattice Oxygen by Electrochemical De-Lithiation for Efficient Benzyl Alcohol Oxidation.

Electrocatalytic benzyl alcohol oxidation reaction (EBOR) is a feasible way to produce high-value-added benzaldehyde and benzoic acid. However, the performance of catalyst usually suffers from the high energy barrier for the O─O bonding step resulting in sluggish process. Herein, lattice oxygen activation strategy is proposed by the electrochemical de-lithiation of LiNiO to catalyze the EBOR through direct O─O bonding to significantly enhance the EBOR performance.

Ferroptosis to Pyroptosis Regulation by Iron-Based Nanocatalysts for Enhanced Tumor Immunotherapy.

Immunogenic cell death serves as a pivotal mechanism in enhancing antitumor immunotherapy by engaging both innate and adaptive immune responses. However, a key unanswered question is which mode of cell death, particularly ferroptosis or pyroptosis, serves as the optimal pathway for activating the immune response. In this study, we introduce an innovative iron-based nanocatalytic medicine that strategically regulates ferroptosis to pyroptosis to augment antitumor immunotherapy.

Self-Reconstructed Amorphous CoO/NiCoB Heterostructure Catalysts for Enhanced HER Performance.

Amorphous electrocatalysts exhibit potentials as precursors for triggering the in situ reconstruction to generate the real catalytic active species toward electrochemical processes. In this work, a new kind of amorphous Ni-Co-B alloy pre-catalysts for hydrogen evolution reaction (HER) is reported, which is obtained via a facile electroless plating strategy on the nickel foam (NF). Interestingly, X-ray photoelectron spectroscopy, X-ray absorption spectroscopy and morphological characterizations identify the in situ reconstruction process during HER accompanied by the preferential leaching of surface B species and the formation of amorphous CoO nanosheet arrays as the real active sites.

Antioxidative Therapy of Alcoholic Liver Injury by Amorphous Two-Dimensional Cobalt Hydroxide Nanocatalyst.

The intake of excessive ethanol will activate an alternative ethanol metabolic pathway in the liver, resulting in the overproduction of reactive oxygen species (ROS), which further leads to alcoholic liver injury (ALI). Although several molecular antioxidants have been utilized in clinics for treating ALI, their efficacies are still less satisfactory. In this work, a nanocatalytic antioxidation therapeutic strategy is proposed for ALI treatment by constructing amorphous Co(OH) nanosheets with catalytic antioxidative property.

A natural killer cell mimic against intracellular pathogen infections.

In the competition between the pathogen infection and the host defense, infectious microorganisms may enter the host cells by evading host defense mechanisms and use the intracellular biomolecules as replication nutrient. Among them, intracellular relies on the host cells to protect itself from the attacks by antibiotics or immune system to achieve long-term colonization in the host, and the consequent clinical therapeutic failures and relapses after antibiotic treatment. Here, we demonstrate that intracellular surviving well even in the presence of vancomycin can be effectively eliminated using an emerging cell-mimicking therapeutic strategy.

Hybridized and engineered microbe for catalytic generation of peroxynitrite and cancer immunotherapy under sonopiezo initiation.

Living therapeutics is an emerging antitumor modality by living microorganisms capable of selective tropism and effective therapeutics. Nevertheless, primitive microbes could only present limited therapeutic functionalities against tumors. Hybridization of the microbes with multifunctional nanocatalysts is of great significance to achieve enhanced tumor catalytic therapy.

Oxygen Vacancy-Mediated Synthesis of Inter-Atomically Ordered Ultrafine Pt-Alloy Nanoparticles for Enhanced Fuel Cell Performance.

Pt-based intermetallics are expected to be the highly active catalysts for oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells but still face great challenges in controllable synthesis of interatomically ordered and ultrafine intermetallic nanoparticles. Here, we propose an oxygen vacancy-mediated atomic diffusion strategy by mechanical alloying to reduce the energy barrier of the transition from interatomic disordering to ordering, and to resist interparticulate sintering via strong M-O-C bonding. This synthesis results in a nanosized core/shell structure featuring an interatomically ordered PtM core and a Pt shell of two to three atomic layers in thickness and can be extended to the multicomponent PtM (M = Co, FeCo, FeCoNi, FeCoNiGa) systems.

Ultrasound-triggered and glycosylation inhibition-enhanced tumor piezocatalytic immunotherapy.

Nanocatalytic immunotherapy holds excellent potential for future cancer therapy due to its rapid activation of the immune system to attack tumor cells. However, a high level of N-glycosylation can protect tumor cells, compromising the anticancer immunity of nanocatalytic immunotherapy. Here, we show a 2-deoxyglucose (2-DG) and bismuth ferrite co-loaded gel (DBG) scaffold for enhanced cancer piezocatalytic immunotherapy.

Nebulized Immunotherapy of Orthotopic Lung Cancer by Mild Magnetothermal-Based Innate Immunity Activations.

Advances in adaptive immunity have greatly contributed to the development of cancer immunotherapy. However, its over-low efficacy and insufficient invasion of immune cells in the tumor tissue, and safety problems caused by cytokine storm, have seriously impeded further clinical application for solid tumor immunotherapy. Notably, the immune microenvironment of the lungs is naturally enriched with alveolar macrophages (AMs).

Triple Regulations via Fe Redox Boosting Nitrate Reduction to Ammonia at Industrial Current Densities.

Electrochemical nitrate reduction reaction (NO RR) has promising prospects for green synthesis of ammonia and environmental remediation. However, the performance of catalysts at high current density usually suffers from the high energy barrier for the nitrate (NO ) to nitrite (NO ) and the competitive hydrogen evolution. Herein, we proposed a two-step relay mechanism through spontaneous redox reaction followed electrochemical reaction by introducing low-valence Fe species into NiP nanosheets to significantly enhance the NO RR performance at industrial current density.

A MOF@MOF S-scheme Heterojunction with Lewis Acid-Base Sites Synergistically Boosts Cocatalyst-Free CO Cycloaddition.

The photocatalytic cycloaddition reaction between CO and epoxide is one of the most promising green routes for CO utilization, for which high performance photocatalysts are intensely desired. Herein, we have constructed an S-scheme heterojunction of MIL-125@ZIF-67 modified by amino groups, which achieves a cyclic carbonate yield of as high as 99 % without employing any co-catalyst, outperforming the previously reported photocatalysts. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and in-situ electron paramagnetic resonance (EPR) spectroscopy reveal the important role of photogenerated electron migration from Lewis acid (Co) sites to the O atom of epoxide in triggering its ring-opening (the rate-determining step of CO cycloaddition reaction) under the assistance of photogenerated hole.

Magnetothermal-activated gene editing strategy for enhanced tumor cell apoptosis.

Precise and effective initiation of the apoptotic mechanism in tumor cells is one of the most promising approaches for the treatment of solid tumors. However, current techniques such as high-temperature ablation or gene editing suffer from the risk of damage to adjacent normal tissues. This study proposes a magnetothermal-induced CRISPR-Cas9 gene editing system for the targeted knockout of HSP70 and BCL2 genes, thereby enhancing tumor cell apoptosis.

Membrane-Free Electrocatalytic Co-Conversions of PBS Waste Plastics and Maleic Acid into High-Purity Succinic Acid Solid.

Plastic pollution, an increasingly serious global problem, can be addressed through the full lifecycle management of plastics, including plastics recycling as one of the most promising approaches. System design, catalyst development, and product separation are the keys in improving the economics of electrocatalytic plastics recycling. Here, a membrane-free co-production system was devised to produce succinic acid (SA) at both anode and cathode respectively by the co-electrolysis of polybutylene succinate (PBS) waste plastics and biomass-derived maleic acid (MA) for the first time.

Allicin‒Decorated FeOOH Nanocatalytic Medicine for Fe/Fe Cycling‒Promoted Efficient and Sustained Tumor Regression.

In the tumor treatment by Fenton reaction‒based nanocatalytic medicines, the gradual consumption of Fe(II) ions greatly reduces the production of hydroxyl radicals, one of the most active reactive oxygen species (ROS), leading to much deteriorated therapeutic efficacy. Meanwhile, the ROS consumption caused by the highly expressed reduced glutathione (GSH) in the tumor microenvironment further prevents tumor apoptosis. Therefore, using the highly expressed GSH in tumor tissue to promote the Fe(III) reduction to Fe(II) can not only weaken the resistance of tumor to ROS attack, but also generate enough Fe(II) to accelerate the Fenton reaction.

Construction of an electron-transfer channel Cu-O-Ni to inhibit the overoxidation of Ni for durable methanol oxidation at industrial current density.

The electrocatalytic methanol oxidation reaction (MOR) is a viable approach for realizing high value-added formate transformation from biomass byproducts. However, usually it is restricted by the excess adsorption of intermediates (CO) and overoxidation of catalysts, which results in low product selectivity and inactivation of the active sites. Herein, a novel Cu-O-Ni electron-transfer channel was constructed by loading NiCuO on nickel foam (NF) to inhibit the overoxidation of Ni and enhance the formate selectivity of the MOR.

Anode-Electrolyte Interfacial Acidity Regulation Enhances Electrocatalytic Performances of Alcohol Oxidations.

The local acidity at the anode surface during electrolysis is apparently stronger than that in bulk electrolyte due to the deprotonation from the reactant, which leads to the deteriorated electrocatalytic performances and product distributions. Here, an anode-electrolyte interfacial acidity regulation strategy has been proposed to inhibit local acidification at the surface of anode and enhance the electrocatalytic activity and selectivity of anodic reactions. As a proof of the concept, CeO Lewis acid component has been employed as a supporter to load Au nanoparticles to accelerate the diffusion and enrichment of OH toward the anode surface, so as to accelerate the electrocatalytic alcohol oxidation reaction.

Biomimetic-Structured Cobalt Nanocatalyst Suppresses Aortic Dissection Progression by Catalytic Antioxidation.

As one of the most lethal cardiovascular diseases, aortic dissection (AD) is initiated by overexpression of reactive oxygen species (ROS) in the aorta that damages the vascular structure and finally leads to massive hemorrhage and sudden death. Current drugs used in clinics for AD treatment fail to efficiently scavenge ROS to a large extent, presenting undesirable therapeutic effect. In this work, a nanocatalytic antioxidation concept has been proposed to elevate the therapeutic efficacy of AD by constructing a cobalt nanocatalyst with a biomimetic structure that can scavenge pathological ROS in an efficient and sustainable manner.

Electrocatalytic ORR-coupled ammoximation for efficient oxime synthesis.

State-of-the-art technology for cyclohexanone oxime production typically demands elevated temperature and pressure, along with the utilization of expensive hydroxylamine sulfate or oxidants. Here, we propose an electrochemistry-assisted cascade strategy for the efficient cyclohexanone ammoximation under ambient conditions by using in situ cathode-generated green oxidants of reactive oxygen species (ROS) such as OOH* and HO. This electrochemical reaction can take place at the cathode, achieving over 95% yield, 99% selectivity of cyclohexanone oxime, and an electron-to-oxime (ETO) efficiency of 96%.

Electrocatalytic functional group conversion-based carbon resource upgrading.

The conversions of carbon resources, such as alcohols, aldehydes/ketones, and ethers, have been being one of the hottest topics most recently for the goal of carbon neutralization. The emerging electrocatalytic upgrading has been regarded as a promising strategy aiming to convert carbon resources into value-added chemicals. Although exciting progress has been made and reviewed recently in this area by mostly focusing on the explorations of valuable anodic oxidation or cathodic reduction reactions individually, however, the reaction rules of these reactions are still missing, and how to purposely find or rationally design novel but efficient reactions in batches is still challenging.

An explainable long short-term memory network for surgical site infection identification.

Background: Currently, surgical site infection surveillance relies on labor-intensive manual chart review. Recently suggested solutions involve machine learning to identify surgical site infections directly from the medical record. Deep learning is a form of machine learning that has historically performed better than traditional methods while being harder to interpret.