Cr-MOF composited with facet-engineered bimetallic alloys for inducing photocatalytic conversion of CO to CH.

The design of efficient photocatalysts is crucial for photocatalytic CO reduction. This study developed photocatalysts based on MIL-101(Cr) composited with a facet-engineered Pt/Pd nanoalloy (PPNA). Photocatalytic performance evaluations show that MIL-101(Cr) loaded with PPNA exposing {111} facets, namely M-A(111), exhibits a CO to CH conversion rate of 9.

A high entropy metallic-high entropy nonmetallic community as a high performance electrocatalyst for the oxygen evolution reaction and oxygen reduction reaction.

The multi-element synergism in high-entropy materials (HEMs) provides great opportunities as multi-functional catalysts or for the promotion of tandem reactions. Herein, a strategy that utilizes a high entropy precursor is proposed to realize the formation of a unique high entropy metallic-high entropy non-metallic community (HEM-HENMC). Aminotriazole acts as a "bonding agent" for the high entropy precursor, and not only binds the five metals Cr, Mn, Fe, Co and Ni together, but also introduces nitrogen and carbon .

A Versatile Method for Preparation of BrCOFs Aerogels and Efficient Functionalization via Suzuki-Miyaura Reaction.

Covalent organic frameworks (COFs) aerogels solve the restrictions on processability and application caused by the insolubility and non-fusibility of powders while avoiding the inaccessibility of pore structures by dense stacking. At the current start-up stage where COFs aerogels are scarce and difficult to synthesize, design of generalized synthetic methods play an indispensable role in guiding and developing COFs aerogels. Moreover, evolving the functionality of COF aerogels is equal vital, which achieves higher performance and broader practical applications.

Platinum/Platinum Sulfide on Sulfur-Doped Carbon Nanosheets with Multiple Interfaces toward High Hydrogen Evolution Activity.

Platinum (Pt)-based materials are among the most competitive electrocatalysts for the hydrogen evolution reaction (HER) due to suitable hydrogen adsorption energy. Due to the rarity of Pt, it is desirable to develop cost-effective Pt-based electrocatalysts with low Pt loading. Herein, Pt/PtS electrocatalysts on S-doped carbon nanofilms (PPS/C) have been successfully fabricated through a precursor reduction route with a complex of Pt and 1-dodecanethiol (1-DDT) as the precursor.

Metal Center-Tuned Photocatalytic Carbon Dioxide Reduction for Frameworks with the Tetraphenylethene-Imidazole Ligand.

As heterogeneous photocatalysts that can effectively transform CO to CO, two MOFs with different metal centers, namely, [M(tipe)(HO)](ClO)·solvent (M = Ni named as and M = Co referred to as ), were synthesized by reactions of 1,1,2,2-tetrakis(4-(imidazole-1-yl)phenyl)ethene (tipe) with the corresponding metal perchlorate. Both and have 3D structures, in which the metal centers have the same coordination environment with the NO donor set. Driven by visible light, the CO production catalyzed by is 6734.

Rh(III)-Catalyzed C(sp)-H Thiolation of 8-Methylquinolines Promoted by Benzoic Anhydride.

Herein, we developed a ligand-promoted Rh(III)-catalyzed C(sp)-H thiolation of 8-methylquinolines. The effect of ligands on improving the activity of the catalytic centers has been studied in detail and proven to be significant. Various substituents are well tolerated under this reaction condition to provide potential precursors for organic synthesis.

Template-Assisted Epitaxial Growth of Ordered SnO Nanorods Arrays with Different Hollow Structures for High-Performance Sodium Storage.

Anode materials for sodium ion batteries (SIBs) are confronted with severe volume expansion and poor electrical conductivity. Construction of assembled structures featuring hollow interior and carbon material modification is considered as an efficient strategy to address the issues. Herein, a novel template-assisted epitaxial growth method, ingeniously exploiting lattice matching nature, is developed to fabricate hollow ordered architectures assembled by SnO nanorods.

Preparation of sp carbon-bonded π-conjugated COF aerogels by ultrasound-assisted mild solvothermal reaction for multi-functional applications.

Molding COFs into aerogels from monomers can establish interpenetrating spatial network structures on the centimeter scale that increase the accessibility of dominant pore channels and the convenience of real application, which radically gets rid of the difficult reprocessing problems of insoluble and non-fusible powder COFs. However, the construction of bulk COF structures and achieving crystallinity are often incompatible, especially with sp carbon-based COFs, whose powder synthesis has been quite demanding. Herein, for the first time, we report an efficient method to prepare sp carbon-linked π-conjugated DFB-TMTA-COF (DT-COF) aerogels by an ultrasound-assisted mild solvothermal technique and freeze-drying.

Rational design of organic ligands for metal-organic frameworks as electrocatalysts for CO reduction.

Electrocatalytic carbon dioxide (CO) reduction to valuable chemical compounds is a sustainable technology with enormous potential to facilitate carbon neutrality by transforming intermittent energy sources into stable fuels. Among various electrocatalysts, metal-organic frameworks (MOFs) have garnered increasing attention for the electrochemical CO reduction reaction (CORR) owing to their structural diversity, large surface area, high porosity and tunable chemical properties. Ligands play a vital role in MOFs, which can regulate the electronic structure and chemical environment of metal centers of MOFs, thereby influencing the activity and selectivity of products.

Multi-layered heterogeneous interfaces created in CoSe@NiS/NF to enhance supercapacitor performances by multi-step alternating electrodeposition.

Heterogeneous interface construction is of far-reaching significance to optimize the electrochemical performance of electrodes. Herein, a multi-step alternating electrochemical deposition (MAED) method is proposed to alternately deposit CoSe and NiS nanosheets on a nickel foam (NF), forming a special alternate layer-by-layer structure with multi-layered heterogeneous interfaces. The creation of the multi-layered heterogeneous interfaces provides a large interfacial area for redox reactions with optimum interstitials facilitating ion diffusion, thus greatly improving the electrochemical energy storage efficiency.

Design of High-Performance Formyl-Functionalized COF Aerogels as Quasi-Solid Lithium Battery Electrolyte by a Solvent Substitution Strategy.

Covalent organic framework (COF) aerogels with functional groups offer exceptional processability and functionality for various applications. These hierarchical porous materials combine the advantages of COFs with the benefits of aerogels, overcoming the limitations of conventional insoluble and nonfusible COF powders. However, achieving both high crystallinity and shape retention remains a challenge for functionalized COF aerogels.

Self-Sustained-Release Strategy Realizes Colloid Oriented Assembly to Fabricate Prussian Blue with Hierarchical Structure.

The controlled self-assembly of nanomaterials has been a great challenge in nanosynthesis, especially for hierarchical architectures with high complexity. Particularly, the structural design of Prussian blue (PB) series materials with robustness and fast nucleation is even more difficult. Herein, a self-sustained-release strategy based on the slow release of metal ions from coordination ions is proposed to guide the assembly of PB crystals.

Cerebrospinal fluid efflux through dynamic paracellular pores on venules as a missing piece of the brain drainage system.

The glymphatic system plays a key role in the clearance of waste from the parenchyma, and its dysfunction has been associated with the pathogenesis of Alzheimer's disease (AD). However, questions remain regarding its complete mechanisms. Here, we report that efflux of cerebrospinal fluid (CSF)/interstitial fluid (ISF) solutes occurs through a triphasic process that cannot be explained by the current model, but rather hints at the possibility of other, previously undiscovered routes from paravenous spaces to the blood.

Rh-Catalyzed Direct Heteroarylation of Unactivated C(sp)-H with -Heteroaryl Boronates.

Disclosed herein is a rhodium(III)-catalyzed direct heteroarylation reaction between unactivated aliphatic C(sp)-H bonds in 2-alkylpyridines and heteroaryl organoboron reagents. This catalytic protocol is compatible with various heterocyclic boronates containing - and -pyridine, pyrazoles, furan, and quinoline with strong coordination capability. The achievement of this methodology provides an efficient route to build new C(sp)-heteroaryl bonds.

Rational design of CT-coupled J-aggregation platform based on Aza-BODIPY for highly efficient phototherapy.

Supramolecular engineering is exceptionally appealing in the design of functional materials, and J-aggregates resulting from noncovalent interactions offer intriguing features. However, building J-aggregation platforms remains a significant challenge. Herein, we report 3,5-dithienyl Aza-BODIPYs with a donor-acceptor-donor (D-A-D) architecture as the first charge transfer (CT)-coupled J-aggregation BODIPY-type platform.

MOF-Based Membranes for Remediated Application of Water Pollution.

Membrane separation plays a crucial role in the current increasingly complex energy environment. Membranes prepared by metal-organic framework (MOF) materials usually possess unique advantages in common, such as uniform pore size, ultra-high porosity, enhanced selectivity and throughput, and excellent adsorption property, which have been contributed to the separation fields. In this comprehensive review, we summarize various designs and synthesized strategies of free-standing MOF and composite MOF-based membranes for water treatment.

Simultaneous single-cell analysis of 5mC and 5hmC with SIMPLE-seq.

Dynamic 5-methylcytosine (5mC) and 5-hydroxymethylcytosine (5hmC) modifications to DNA regulate gene expression in a cell-type-specific manner and are associated with various biological processes, but the two modalities have not yet been measured simultaneously from the same genome at the single-cell level. Here we present SIMPLE-seq, a scalable, base resolution method for joint analysis of 5mC and 5hmC from thousands of single cells. Based on orthogonal labeling and recording of 'C-to-T' mutational signals from 5mC and 5hmC sites, SIMPLE-seq detects these two modifications from the same molecules in single cells and enables unbiased DNA methylation dynamics analysis of heterogeneous biological samples.

A homologous series of macrocyclic Ni clusters: synthesis, structures, and catalytic properties.

Due to their intriguing ring structures and promising applications, nickel-thiolate clusters, such as [Ni(SR)] ( = 4-6), have attracted tremendous interest. However, investigation of the synthesis, structures, and properties of macrocyclic Ni clusters ( > 8) has been seriously impeded. In this work, a homologous series of macrocyclic nickel clusters, Ni(4MPT) ( = 9-12), was fabricated by using 4-methylphenthiophenol (4MPT) as the ligand.

Supramolecular assemblies of Cu(II) with a tetraphenylethene-imidazole ligand for tuning photocatalytic CO reduction.

Cu(II) supramolecular assemblies [Cu(tipe)(HO)](NO)·2.5HO (CuN4) and [CuCl(tipe)(CHCN)]·HO (CuN2Cl2) (tipe = 1,1,2,2-tetrakis(4-(imidazole-1-yl)phenyl)ethene) were synthesized and utilized for photocatalytic CO reduction. CuN4 exhibits CO production of up to 891 μmol g with a selectivity of 79.

Silver frameworks based on a tetraphenylethylene-imidazole ligand for electrocatalytic reduction of CO to CO.

Metal-organic frameworks (MOFs) can be used as electrocatalysts for the CO reduction reaction (CORR) because of their well-dispersed metal centers. Silver is a common electrocatalyst for reduction of CO to CO. In this study, two Ag-MOFs with different structures of [AgO(TIPE)](NO) (Ag-MOF1) and [Ag(TIPE)CFSO] (Ag-MOF2) [TIPE = 1,1,2,2-tetrakis(4-(imidazol-1-yl)phenyl)ethene] were synthesized and used for CO electroreduction.

Enhanced Photodynamic Therapy Synergizing with Inhibition of Tumor Neutrophil Ferroptosis Boosts Anti-PD-1 Therapy of Gastric Cancer.

For tumor treatment, the ultimate goal in tumor therapy is to eliminate the primary tumor, manage potential metastases, and trigger an antitumor immune response, resulting in the complete clearance of all malignant cells. Tumor microenvironment (TME) refers to the local biological environment of solid tumors and has increasingly become an attractive target for cancer therapy. Neutrophils within TME of gastric cancer (GC) spontaneously undergo ferroptosis, and this process releases oxidized lipids that limit T cell activity.

Co(III)-Catalyzed C6-Selective C-H Activation/Pyridine Migration of 2-Pyridones with Propiolates.

A versatile Co(III)-catalyzed C6-selective C-H activation/pyridine migration of 2-pyridones with available propiolates as coupling partners was demonstrated. This method features high atom economy, excellent regioselectivity, and good functional group tolerance by employing an inexpensive Co(III) catalyst under mild reaction conditions. Moreover, gram-scale synthesis and late-stage modifications of pharmaceuticals were performed to prove the effectiveness of these synthetic approaches.

Self-Assembly of Lanthanide-Aluminum Cluster-Organic Frameworks with Magnetocaloric Effect and Luminescence.

The self-assembly of the lanthanide metal-organic frameworks presents a formidable challenge but profound significance. Compared with the metal-organic frameworks based on 4f-3d ions, the chemistry of 4f-3p metal-organic frameworks has not been fully explored so far. In this study, two lanthanide-aluminum-based clusters [LnAl(IN)(μ-OH)(μ-O)(HO)]·HO ( = 2, Ln = Gd, abbreviated as ; = 2.