Catalytic applications of organic-inorganic hybrid porous materials.

Organic-inorganic hybrid porous materials (OIHMs) inherit the unique properties from both organic and inorganic components, and the flexibility in the incorporation of functional groups renders the OIHMs an ideal platform for the construction of catalytic materials with multiple active sites. The preparation of OIHMs with precise locations of organic-inorganic components and tunable structures is one of the important topics for the catalytic application of OIHMs, but it is still very challenging. In this feature article, we describe our work related to the preparation of OIHMs confining active sites in the nanostructure and a layer-by-layer assembly method and their applications in acid-base catalysis, catalytic hydrogenation and photocatalysis with a focus on the elucidation of the synergistic effects of different active sites and the unique properties of OIHMs in catalysis.

Changes in metabolic parameters and serum YKL-40 levels in Chinese rheumatoid arthritis patients during tocilizumab therapy.

Objective: To investigate the metabolic changes during therapy of tocilizumab (TCZ) and methotrexate (MTX) in non-diabetic rheumatoid arthritis (RA) patients and for the first time explore the associations between metabolic parameters and serum YKL-40 (sYKL-40) levels.

Methods: We enrolled active non-diabetic RA patients who were refractory to MTX. Patients received intravenous TCZ (8 mg/kg) once every 4 weeks combined with MTX for 24 weeks.

InCl-Assisted Surface Defects Restoring to Enhance Lead-Free CsZrCl Nanocrystals for X-Ray Imaging and Blue LED Applications.

As one type of recent emerging lead-free perovskites, CsZrCl nanocrystals are widely concerned, benefiting from the eminent designability, high X-ray cutoff efficiency, and favorable stability. Improving the luminescence performance of CsZrCl nanocrystals has great importance to cater for practical applications. In view of the surface defects frequently formed by the liquid phase method, the particle morphology and surface quality of this material are expected to be regulated if certain intervention is made in the synthesis process.

Reactant enrichment in hollow void of Pt NPs@MnOx nanoreactors for boosting hydrogenation performance.

In confined mesoscopic spaces, the unraveling of a catalytic mechanism with complex mass transfer and adsorption processes such as reactant enrichment is a great challenge. In this study, a hollow nanoarchitecture of MnO-encapsulated Pt nanoparticles was designed as a nanoreactor to investigate the reactant enrichment in a mesoscopic hollow void. By employing advanced characterization techniques, we found that the reactant-enrichment behavior is derived from directional diffusion of the reactant driven through the local concentration gradient and this increased the amount of reactant.

Enzyme-Compatible Core-Shell Nanoreactor for in Situ H -Driven NAD(P)H Regeneration.

The regeneration of the reduced form cofactor NAD(P)H is essential for the extra-cellular application of bio-reduction, which necessitates not only the development of efficient artificial NAD(P)H regeneration catalytic system but also its well compatibility with the cascade enzymatic reduction system. In this work, we reported the preparation of a metal nanoparticle (NP) and metal complex integrated core-shell nanoreactor for H -driven NAD(P)H regeneration through the immobilization of a Rh complex on Ni/TiO surface via a bipyridine contained 3D porous organic polymer (POP). In comparison with the corresponding single component metal NPs and the immobilized Rh complex, the integrated catalyst presented simultaneously enhanced activity and selectivity in NAD(P)H regeneration thanks to the rapid spillover of activated H species from metal NPs to Rh complex.

Design of Hollow Nanoreactors for Size- and Shape-Selective Catalytic Semihydrogenation Driven by Molecular Recognition.

Mimicking the structures and functions of cells to create artificial organelles has spurred the development of efficient strategies for production of hollow nanoreactors with biomimetic catalytic functions. However, such structure are challenging to fabricate and are thus rarely reported. We report the design of hollow nanoreactors with hollow multishelled structure (HoMS) and spatially loaded metal nanoparticles.

Microenvironment engineering of supported metal nanoparticles for chemoselective hydrogenation.

Selective hydrogenation with supported metal catalysts widely used in the production of fine chemicals and pharmaceuticals often faces a trade-off between activity and selectivity, mainly due to the inability to adjust one factor of the active sites without affecting other factors. In order to solve this bottleneck problem, the modulation of the microenvironment of active sites has attracted more and more attention, inspired by the collaborative catalytic mode of enzymes. In this perspective, we aim to summarize recent advances in the regulation of the microenvironment surrounding supported metal nanoparticles (NPs) using porous materials enriched with organic functional groups.

Microglial Piezo1 senses Aβ fibril stiffness to restrict Alzheimer's disease.

The pathology of Alzheimer's disease (AD) is featured with extracellular amyloid-β (Aβ) plaques, whose impact on the mechanical properties of the surrounding brain tissues is unclear. Microglia sense and integrate biochemical cues of the microenvironment. However, whether the microglial mechanosensing pathways influence AD pathogenesis is unknown.

Synergy of metal nanoparticles and organometallic complex in NAD(P)H regeneration via relay hydrogenation.

Most, if not all, of the hydrogenation reactions are catalyzed by organometallic complexes (M) or heterogeneous metal catalysts, but to improve both the activity and selectivity simultaneously in one reaction via a rational combination of the two types of catalysts remains largely unexplored. In this work, we report a hydrogenation mode though H species relay from supported metal nanoparticles (NPs) to M, where the former is responsible for H dissociation, and M is for further hydride transferring to reactants. The synergy between metal NPs and M yields an efficient NAD(P)H regeneration system with >99% selectivity and a magnitude higher activity than the corresponding metal NPs and M.

Efficient Transfection of In vitro Transcribed mRNA in Cultured Cells Using Peptide-Poloxamine Nanoparticles.

In vitro transcribed messenger RNA (mRNA) vaccines have displayed enormous potential in fighting against the coronavirus disease 2019 (COVID-19) pandemic. Efficient and safe delivery systems must be included in the mRNA vaccines due to the fragile properties of mRNA. A self-assembled peptide-poloxamine nanoparticle (PP-sNp) gene delivery system is specifically designed for the pulmonary delivery of nucleic acids and displays promising capabilities in mediating successful mRNA transfection.

Covalent organic frameworks with high quantum efficiency in sacrificial photocatalytic hydrogen evolution.

Organic semiconductors offer a tunable platform for photocatalysis, yet the more difficult exciton dissociation, compared to that in inorganic semiconductors, lowers their photocatalytic activities. In this work, we report that the charge carrier lifetime is dramatically prolonged by incorporating a suitable donor-acceptor (β-ketene-cyano) pair into a covalent organic framework nanosheet. These nanosheets show an apparent quantum efficiency up to 82.

The promotion effect of π-π interactions in Pd NPs catalysed selective hydrogenation.

The utilization of weak interactions to improve the catalytic performance of supported metal catalysts is an important strategy for catalysts design, but still remains a big challenge. In this work, the weak interactions nearby the Pd nanoparticles (NPs) are finely tuned by using a series of imine-linked covalent organic frameworks (COFs) with different conjugation skeletons. The Pd NPs embedded in pyrene-COF are ca.

The Oligodendrocyte Transcription Factor 2 OLIG2 regulates transcriptional repression during myelinogenesis in rodents.

OLIG2 is a transcription factor that activates the expression of myelin-associated genes in the oligodendrocyte-lineage cells. However, the mechanisms of myelin gene inactivation are unclear. Here, we uncover a non-canonical function of OLIG2 in transcriptional repression to modulate myelinogenesis by functionally interacting with tri-methyltransferase SETDB1.

Anti-melanoma differentiation-associated 5 gene antibody-positive dermatomyositis exhibit three clinical phenotypes with different prognoses.

Objectives: We aimed to identify different subtypes of dermatomyositis (DM) patients positive with anti-melanoma differentiation-associated gene 5 antibody (DM-MDA5+) for customised treatments to improve the outcomes.

Methods: Among 96 DM-MDA5+ patients, subgroups with similar phenotypes were delineated using hierarchical clustering analysis of the clinico-biological characteristics. Classification and regression trees were used to build a classification model and survival analysis was used to evaluate the prognoses of subgroups.

The Fabrication of Pd Single Atoms/Clusters on COF Layers as Co-catalysts for Photocatalytic H Evolution.

The particle size of co-catalysts significantly affects the activity of semiconductors in photocatalysis. Herein, we report that the photocatalytic H evolution (PHE) activity of a visible light responsive covalent organic framework (COF) layer supported on SiO nanoparticles was greatly promoted from 47.7 to 85.

Intravenous immunoglobulin for interstitial lung diseases of anti-melanoma differentiation-associated gene 5-positive dermatomyositis.

Objective: Rapidly progressive interstitial lung disease (RP-ILD) in DM patients positive for anti-melanoma differentiation-associated gene 5 (anti-MDA5) autoantibody (MDA5-DM) often have a poor prognosis, frequently fatal. As there is a scarcity of data regarding the effect of intravenous immunoglobulin (IVIG) on RP-ILD in MDA5-DM patients (MDA5-RPILD), we conducted this study to determine the efficacy of a IVIG add-on initial treatment.

Methods: Patients with newly-onset MDA5-RPILD from September 2018 to June 2020 were retrospectively reviewed for 6 months in the First Affiliated Hospital of Zhengzhou University.

Synthesis of Bifunctional Porphyrin Polymers for Catalytic Conversion of Dilute CO to Cyclic Carbonates.

Development of efficient solid catalysts for catalytic conversion of dilute CO is of extreme importance for carbon capture and utilization. We report the synthesis of bifunctional polymers co-incorporated with porphyrin-Zn as Lewis acid sites and Br as nucleophiles for the cycloaddition of dilute CO with epoxides in this work. It was found that the Br/Zn ratio has a volcano relation with the activity of bifunctional polymers in a cycloaddition reaction, indicating the synergy effect between Lewis acid sites and nucleophiles.

Diagnostic Performance of PI-RADS v2, Proposed Adjusted PI-RADS v2 and Biparametric Magnetic Resonance Imaging for Prostate Cancer Detection: A Preliminary Study.

Purpose: To evaluate the diagnostic performance of PI-RADS v2, proposed adjustments to PI-RADS v2 (PA PI-RADS v2) and biparametric magnetic resonance imaging (MRI) for prostate cancer detection.

Methods: A retrospective cohort of 224 patients with suspected prostate cancer was included from January 2016 to November 2018. All the patients underwent a multi-parametric MR scan before biopsy.

Synthesis of Sulfonated Porous Organic Polymers with a Hydrophobic Core for Efficient Acidic Catalysis in Organic Transformations.

Synthesis of sulfonated porous polymers with improved hydrophobicity and stability is of extreme importance in both academic research and industrial applications. However, there is often a trade-off between acidity and surface hydrophobicity of sulfonated polymers. In this study, we report a strategy for the synthesis of sulfonated porous organic polymers (S-PT) with improved hydrophobicity via free radical polymerization method by using a rigid and large multidentate monomer, 1,3,5-tri(4-vinylphenyl)-benzene, having a hydrophobic core.

Hydrogenation of benzoic acid derivatives over Pt/TiO under mild conditions.

Hydrogenation of benzoic acid (BA) to cyclohexanecarboxylic acid (CCA) has important industrial and academic significance, however, the electron deficient aromatic ring and catalyst poisoning by carboxyl groups make BA hydrogenation a challenging transformation. Herein, we report that Pt/TiO is very effective for BA hydrogenation with, to our knowledge, a record TOF of 4490 h at 80 °C and 50 bar H, one order higher than previously reported results. Pt/TiO catalysts with electron-deficient and electron-enriched Pt sites are obtained by modifying the electron transfer direction between Pt and TiO.

Quantification of pancreatic iron overload and fat infiltration and their correlation with glucose disturbance in pediatric thalassemia major patients.

Background: Diabetes mellitus affects more than a quarter of patients with thalassemia major (TM) worldwide, and increases the risk for cardiac complications, contributing to significant morbidity. Pancreatic iron overload (IO) and fat infiltration have been correlated with this endocrinal complication in adult TM patients. It has been shown that in adult TM patients, iron accumulation and fat infiltration are found to be heterogeneous in the pancreatic head, body, and tail region.

Initial predictors for short-term prognosis in anti-melanoma differentiation-associated protein-5 positive patients.

Background: Anti-melanoma differentiation-associated protein-5 (anti-MDA5) positive patients are characterized by the high mortality rate caused by interstitial lung disease (ILD). We conducted a retrospective study to summarize the clinical features and identify the initial predictors for death in anti-MDA5 positive patients.

Methods: We designed a retrospective cohort of anti-MDA5 positive patients.