Confinement Effect and Hydrogen Species Modulation toward Enhanced Electrochemical CO Reduction to Ethanol.

The protonation process of adsorbed *CO intermediates has been widely recognized as a critical determinant governing product selectivity in electrocatalytic carbon dioxide reduction reaction (eCORR). However, the active hydrogen species and mechanism of *CO protonation in acid eCORR remain ambiguous. Particularly, the involvement of H in *CO hydrogenation is still under debate.

3D Covalent Arsenic Polyoxomolybdate-Organic Polymer with Ultrahigh Photocatalytic Oxidative Ability for Aromatic C─H Activation.

The photocatalytic activation of inert aromatic C─H bonds under mild conditions remains a major challenge due to the inherent stability of sp C─H bonds and the lack of efficient, selective heterogeneous photocatalysts. Herein, by strategically balancing the solubility of aniline-functionalized arsenic polyoxomolybdate (AsPOM) with the organic linker of 1,4-bi(3-dimethylamino-1-oxoprop-2-enyl)benzene (BDOEB), a new 3D covalent AsPOM-organic polymer, termed POF-2, was successfully prepared. Its short- to medium-range ordered structure was resolved using the advanced total scattering atomic pair distribution function (PDF).

Metagenomic Next-Generation Sequencing Provides a Reliable Method for Early Diagnosis of Pneumocystis jirovecii Pneumonia After Kidney Transplant: A Single-Center Retrospective Cohort Study.

Objectives: Pneumocystis jirovecii pneumonia, a common pulmonary infection after kidney transplant, cannot be detected by conventional culture methods, and limitations have been shown with lung tissue biopsy, sputum collection, and sample smear staining. Early diagnosis is key as long-term survival is decreased in patients with Pneumocystis jirovecii pneumonia who are not treated in a timely and effective manner.

Materials And Methods: From January 2018 to January 2023, our study enrolled 110 patients with pulmonary infection seen at the First Affiliated Hospital of Xi'an Jiaotong University (China).

Regular Mesoporous Superparticles with a Tailored Opening Window and Tunable Surface Crisscrossed Grooves.

Regular hollow mesoporous superparticles with an opening window and controllable surface grooves can significantly improve the high-loading performance of aqueous zinc ion hybrid capacitors, but their synthesis remains a great challenge. Herein, an electrostatic force-assisted monomicelle confined assembly strategy is demonstrated for synthesizing such regular mesoporous hollow superparticles. The mesoporous superparticles feature a hollow (∼250 nm) in the center and a tailored transverse window (35-50 nm) to enable the superparticles to be totally connected from the inner to external surface, and a monolayer of spherical mesopores (∼15 nm) is arrayed in an orderly fashion on the hollow shell to form the unique crisscrossed grooves.

Predicting sorption of organic pollutants on soils with interpretable machine learning.

The sorption of organic pollutants (OPs) on soils plays a critical role in determining the environmental fate and transport of these compounds, which has been extensively studied. However, the complex nonlinear relationships between adsorption capacity and multiple influencing factors, as well as the relative contributions of these factors to adsorption behavior, remain inadequately understood. This study develops five machine learning (ML) models-support vector machine (SVM), deep neural networks (DNN), extreme gradient boosting (XGBT), random forest (RF), and gradient boosting decision tree (GBDT)-using a dataset of 352 data points from previous studies to predict OPs sorption on soils based on multiple factors.

Inwardly Directed Linker Propagation: Constructing 3D Covalent Organic Frameworks for Efficient HO Photosynthesis.

The limited design strategy of three-dimensional covalent organic frameworks (3D COFs) greatly restricts their structural diversification and potential applications. Herein, we propose an inwardly directed linker propagation strategy for the targeted assembly of 3D COFs (COF-IN-1 and COF-IN-2) and compare them with outwardly directed expanded COFs (COF-OUT-1 and COF-OUT-2). COF-OUTs exhibit planar heteroporous 2D frameworks with cpt topology, while COF-INs engineer controlled triple entanglements into networks, forming 3D frameworks with acs topology.

Recent Advances in Green Hydrogen Production by Electrolyzing Water with Anion-Exchange Membrane.

The development of clean and efficient renewable energy is of great strategic importance to realize green energy conversion and low-carbon growth. Hydrogen energy, as a renewable energy with "zero carbon emission", can be efficiently converted into hydrogen energy and electric energy by electrolysis of water to hydrogen technology. Anion-exchange membrane water electrolysis (AEMWE), substantially advanced by nonprecious metal electrocatalysts, is among the most cost-effective and promising water electrolysis technologies, combining the advantages of proton exchange membranes with the proven technology of traditional alkaline water electrolysis and potentially eliminating the disadvantages of both.

Polyoxometalated metal-organic framework superstructure for stable water oxidation.

Stable, nonprecious catalysts are vital for large-scale alkaline water electrolysis. Here, we report a grafted superstructure, MOF@POM, formed by self-assembling a metal-organic framework (MOF) with polyoxometalate (POM). In situ electrochemical transformation converts MOF into active metal (oxy)hydroxides to produce a catalyst with a low overpotential of 178 millivolts at 10 milliamperes per square centimeter in alkaline electrolyte.

In Situ Electrochemical Reconstruction of Cation-Vacancy-Enriched Ni@NiP Particles in Hollow N-Doped Carbon Nanofibers for Efficient Nitrate Reduction.

Electrochemical nitrate (NO ) reduction to ammonia (NH) under ambient conditions is promising to promote the artificial nitrogen cycling. Despite the development of transition metal-based catalysts, their incident in situ electrochemical reconstruction always leads to the ambiguity of veritable active sites and reaction mechanisms. In this work, we report an approach to encapsulate Ni@NiP particles with cationic Ni vacancies in hollow N-doped carbon nanofibers (designated Ni@Ni P@N-CNFs) for electrocatalytic NO reduction to NH and have investigated their surface reconstruction and reaction mechanisms using various in situ electrochemical characterizations and theoretical calculations.

Crystal-Facet Engineering of Mesoporous CuS Cascade Nanoreactors Enhances Photocatalytic C-C Coupling of CO-to-CH.

Crystal-facet heterojunction engineering of mesoporous nanoreactors with highly redox-active represents an efficacious strategy for the transformation of CO into valuable C products (e.g., CH).

Exploring the efficacy of acupuncture for tension-type headache: a literature review and insights from traditional Chinese medicine.

Tension-type headache (TTH) is a common primary headache disorder, and recent research has focused on various treatment options. However, studies evaluating acupuncture for TTH from the perspective of Traditional Chinese Medicine (TCM) and its mechanisms are limited. This literature review synthesizes findings from twelve clinical studies that investigated acupuncture for TTH treatment.

Covalent Organic Frameworks with Regulated Water Adsorption Sites for Efficient Cooling of Electronics.

The excessive heat accumulation has been the greatest danger for chips to maintain the computing power. In this paper, a passive thermal management strategy for electronics cooling was developed based on the water vapor desorption process of the covalent organic frameworks (COFs). The precise regulation for the number of carbonyl group and the ratio of hydrophilicity and hydrophobicity within pore channels was achieved by water adsorption sites engineering.

Bioinspired catalytic pocket promotes CO-to-ethanol photoconversion on colloidal quantum wells.

Sluggish surface reaction is a critical factor that strongly governs the efficiency of photocatalytic solar fuel production, particularly in CO-to-ethanol photoconversion. Here, inspired by the principles underlying enzyme catalytic proficiency and specificity, we report a biomimetic photocatalyst that affords superior CO-to-ethanol photoreduction efficiency (5.5 millimoles gram hour in average with 98.

Strategy of constructing D-A structure and accurate active sites over graphitic carbon nitride nanowires for high efficient photocatalytic nitrogen fixation.

Constructing photocatalysts for the stable and efficient production of NH is of excellent research significance and challenging. In this paper, the electron acceptor 5-amino-1,10-phenanthroline (AP) is introduced into the electron-donor graphitic carbon nitride (CN) framework by a simple heated copolymerization method to construct a donor-acceptor (D-A) structure. Subsequently, the phenanthroline unit is coordinated with transition metal Fe ions to obtain the photocatalyst Fe(III)-0.

One-Dimensional Single-Crystal Mesoporous TiO Supported CuWO Clusters as Photocatalytic Cascade Nanoreactor for Boosting Reduction of CO to CH.

Constructing nanoreactors with multiple active sites in well-defined crystalline mesoporous frameworks is an effective strategy for tailoring photocatalysts to address the challenging of CO reduction. Herein, one-dimensional (1-D) mesoporous single-crystal TiO nanorod (MS-TiO-NRs, ≈110 nm in length, high surface area of 117 m g, and uniform mesopores of ≈7.0 nm) based nanoreactors are prepared via a droplet interface directed-assembly strategy under mild condition.

Three-Dimensional Covalent Organic Frameworks Based on Linear and Trigonal Linkers for High-Performance HO Photosynthesis.

The design of three-dimensional covalent organic frameworks (3D COFs) using linear and trigonal linkers remains challenging due to the difficulty in achieving a specific non-planar spatial arrangement with low-connectivity building units. Here, we report the novel 3D COFs with linear and trigonal linkers, termed TMB-COFs, exhibiting srs topology. The steric hindrance provides an additional force to alter the torsion angles of peripheral triangular units, guiding the linear unit to connect with the trigonal unit into 3D srs frameworks, rather than the more commonly observed two-dimensional (2D) hcb structures.

Highly Efficient Nitrogen Reduction to Ammonia through the Cooperation of Plasma and Porous Metal-Organic Framework Reactors with Confined Water.

While the ambient N reduction to ammonia (NH) using HO as hydrogen source (2N+6HO=4NH+3O) is known as a promising alternative to the Haber-Bosch process, the high bond energy of N≡N bond leads to the extremely low NH yield. Herein, we report a highly efficient catalytic system for ammonia synthesis using the low-temperature dielectric barrier discharge plasma to activate inert N molecules into the excited nitrogen species, which can efficiently react with the confined and concentrated HO molecules in porous metal-organic framework (MOF) reactors with V, Cr, Mn, Fe, Co, Ni and Cu ions. Specially, the Fe-based catalyst MIL-100(Fe) causes a superhigh NH yield of 22.

Efficient reduction of CO and inhibition of hydrogen precipitation by polyoxometalate photocatalyst modified with the metal Mn.

Photocatalytic reduction of CO to chemical fuels is attractive for solving both the greenhouse effect and the energy crisis, but the key challenge is to design and synthesize photocatalysts with remarkable performance under visible light irradiation. Efficient catalytic carbon dioxide reduction (CORR) with light is considered a promising sustainable and clean approach to solve environmental problems. Herein, we found a new photocatalyst ([Mn(en)][VBO(OH)]) (abbreviated as MnV) based on the modifiability of polyoxometalates, in which Mn acts as a modifying unit to efficiently reduce CO to CO and effectively inhibit the hydrogen precipitation reaction.

Enhanced effect of limb remote ischemic postconditioning combined with paeoniflorin on alleviating cerebral ischemic injury via neutrophil NADPH pathway.

Background: Limb remote ischemic postconditioning (LRIP) and paeoniflorin (PF) both can ameliorate cerebral ischemia reperfusion (I/R) injury. At present, whether LRIP combined with PF can achieve better therapeutic effect is unknown.

Purpose: This study explored the alleviating effect and mechanism of LRIP in combination with PF on cerebral I/R injury in rats.

Stretchable Tb-Tb Distance Regulates the Piezofluorochromic Behavior of Chiral Tb(III)-MOF upon Compression.

Luminescent chiral microcrystals with the Tb(COO) subunit indicated strong green mechano-luminescence under compression. Furthermore, piezofluorochromic behavior in the diamond anvil cell was observed, with the intensity tendency of decreasing-increasing-decreasing and a shortened lifetime upon compression, due to the reversible stretchable Tb-Tb interactions. The Tb-Tb distance upon compression was refined through situ high-pressure X-ray absorption spectra, which was consistent with the tendency of the piezofluorochromic intensity.

Plasma-Driven Efficient Conversion of CO and HO into Pure Syngas with Controllable Wide H/CO Ratios over Metal-Organic Frameworks Featuring In Situ Evolved Ligand Defects.

While the mild production of syngas (a mixture of H and CO) from CO and HO is a promising alternative to the coal-based chemical engineering technologies, the inert nature of CO molecules, unfavorable splitting pathways of HO and unsatisfactory catalysts lead to the challenge in the difficult integration of high CO conversion efficiency with produced syngas with controllable H/CO ratios in a wide range. Herein, we report an efficient plasma-driven catalytic system for mild production of pure syngas over porous metal-organic framework (MOF) catalysts with rich confined HO molecules, where their syngas production capacity is regulated by the in situ evolved ligand defects and the plasma-activated intermediate species of CO molecules. Specially, the Cu-based catalyst system achieves 61.

Regulated Dual Defects of Bridging Organic and Terminal Inorganic Ligands in Iron-based Metal-Organic Framework Nodes for Efficient Photocatalytic Ammonia Synthesis.

Engineering advantageous defects to construct well-defined active sites in catalysts is promising but challenging to achieve efficient photocatalytic NH synthesis from N and HO due to the chemical inertness of N molecule. Here, we report defective Fe-based metal-organic framework (MOF) photocatalysts via a non-thermal plasma-assisted synthesis strategy, where their NH production capability is synergistically regulated by two types of defects, namely, bridging organic ligands and terminal inorganic ligands (OH and HO). Specially, the optimized MIL-100(Fe) catalysts, where there are only terminal inorganic ligand defects and coexistence of dual defects, exhibit the respective 1.

Melt-quenched glass formation of a family of metal-carboxylate frameworks.

Metal-organic framework (MOF) glasses are an emerging class of glasses which complement traditional inorganic, organic and metallic counterparts due to their hybrid nature. Although a few zeolitic imidazolate frameworks have been made into glasses, how to melt and quench the largest subclass of MOFs, metal carboxylate frameworks, into glasses remains challenging. Here, we develop a strategy by grafting the zwitterions on the carboxylate ligands and incorporating organic acids in the framework channels to enable the glass formation.