Design and Construction of a Porphyrin-Based Samarium(III)-Metal-Organic Framework for Antibiotic Detection.

Porphyrins bearing the unique 18π electron tetrapyrrolic macrocycles exhibit interesting photophysical and photochemical properties and have been considered as promising ligands for the construction of functionalized metal-organic frameworks (MOFs). The combination of porphyrin-type ligands with lanthanide metals featured with diverse coordination environments to realize the novel functions as well as the diversity of the MOF is thus attractive but challenging. Herein, an unprecedented porphyrin-based samarium MOF (Sm-BCPP) composed of a 5,10-bis(4-carboxyphenyl)-10,20-diphenyl porphyrin (HBCPP) ligand and samarium-formed one-dimensional clusters has been constructed via a solvothermal approach, and the synthesized Sm-BCPP has excellent chemical stabilities, exhibiting red luminescence.

Enhanced Cooperative Generalized Compressive Strain and Electronic Structure Engineering in W-NiN for Efficient Hydrazine Oxidation Facilitating H Production.

As promising bifunctional electrocatalysts, transition metal nitrides are expected to achieve an efficient hydrazine oxidation reaction (HzOR) by fine-tuning electronic structure via strain engineering, thereby facilitating hydrogen production. However, understanding the correlation between strain-induced atomic microenvironments and reactivity remains challenging. Herein, a generalized compressive strained W-NiN catalyst is developed to create a surface with enriched electronic states that optimize intermediate binding and activate both water and NH.

Insulator-donor electron wavefunction coupling in pseudo-bilayer organic solar cells achieving a certificated efficiency of 19.18.

The incorporation of polymeric insulators has led to notable achievements in the field of organic semiconductors. By altering the blending concentration, polymeric insulators exhibit extensive capabilities in regulating molecular configuration, film crystallinity, and mitigation of defect states. However, current research suggests that the improvement in such physical properties is primarily attributed to the enhancement of thin film morphology, an outcome that seems to be an inevitable consequence of incorporating insulators.

Competing Hexagonal and Square Lattices on a Spherical Surface.

The structural properties of packed soft-core particles provide a platform to understand the cross-pollinated physical concepts in solid-state and soft-matter physics. Confined on a spherical surface, the traditional differential geometry also dictates the overall defect properties in otherwise regular crystal lattices. Using molecular dynamics simulation of the Hertzian model as a tool, we report here the emergence of new types of disclination patterns: domain and counter-domain defects, when hexagonal and square patterns coexist.

Copper-Catalyzed Oxidative Arylation and Hydroxylation of Indolin-2-ones for Direct Construction of Tetrasubstituted Carbon Centers.

This study introduces a novel methodology for the direct construction of tetrasubstituted centers, utilizing secondary C(sp)-H and C(sp)-H substrates, specifically indolin-2-ones and indoles, through an innovative oxidative cross-coupling reaction. Facilitated by a straightforward copper salt catalyst, this reaction proceeds efficiently at a mild temperature of 40 °C under operationally streamlined conditions. Emphasizing sustainability, this method is notably enhanced by employing air (molecular oxygen) as an eco-friendly oxidant.

Atomically engineering interlayer symmetry operations of two-dimensional crystals.

Crystal symmetry, which governs the local atomic coordination and bonding environment, is one of the paramount constituents that intrinsically dictate materials' functionalities. However, engineering crystal symmetry is not straightforward due to the isotropically strong covalent/ionic bonds in crystals. Layered two-dimensional materials offer an ideal platform for crystal engineering because of the ease of interlayer symmetry operations.

Molecular Design of Positively Charged 3D Covalent-Organic Framework Membranes for Li/Mg Separation.

3D covalent-organic framework (3D COF) membranes have unique features such as smaller pore sizes and more interconnected networks compared with 2D COF counterparts. However, the complicated and unmanageable fabrication hinders their rapid development. Molecular simulation, which can efficiently explore the structure-performance relationship of membranes, holds great promise in accelerating the development of 3D COF membranes.

Solar-Driven Sulfide Oxidation Paired With CO Reduction Based on Vacancies Engineering of Copper Selenide.

Photovoltaic-driven electrochemical (PV-EC) carbon dioxide reduction (COR) coupled with sulfide oxidation (SOR) can efficiently convert the solar energy into chemical energy, expanding its applications. However, developing low-cost electrocatalysts that exhibit high selectivity and efficiency for both COR and SOR remains a challenge. Herein, a bifunctional copper selenide catalyst is developed with copper vacancies (v-CuSe) for the COR-SOR.

Design and Synthesis of Novel Dual-Functional Protic Ionic Liquids with a Superior High CO Absorption Efficiency.

As a predictive tool, quantum chemical calculations can be used to design protic ionic liquids (PILs) and predict the result. By adding anionic negative potential sites, two dual-functional PILs diethylenetriamine-barbituric acid [CHN][CHNO] and diethylenetriamine-ethylenolactonium [CHN][CHNO] were designed. The simulation results indicated that multisite absorption of anions and cations resulted in an expected absorption ratio exceeding 3:1 (mol CO:mol ILs).

A Review on MXene/Nanocellulose Composites: Toward Wearable Multifunctional Electromagnetic Interference Shielding Application.

With the rapid development of mobile communication technology and wearable electronic devices, the electromagnetic radiation generated by high-frequency information exchange inevitably threatens human health, so high-performance wearable electromagnetic interference (EMI) shielding materials are urgently needed. The 2D nanomaterial MXene exhibits superior EMI shielding performance owing to its high conductivity, however, its mechanical properties are limited due to the high porosity between MXene nanosheets. In recent years, it has been reported that by introducing natural nanocellulose as an organic framework, the EMI shielding and mechanical properties of MXene/nanocellulose composites can be synergically improved, which are expected to be widely used in wearable multifunctional shielding devices.

Groupy: An Open-Source Toolkit for Molecular Simulation and Property Calculation.

In this work, an open-source, versatile, and flexible code named Groupy is present for calculating various molecular properties and preparing input files of molecular simulation software such as Gaussian. This code requires only SMILES as input, but can output many new useful data and files in multiple formats. The output information is clear and easy to read.

"One-Pot" Synthesized Phosphorus Corrole-Based Metal-Organic Frameworks for Synergistic Phototherapy and Chemodynamic Therapy.

As a distinctive class of porphyrin derivatives, corroles offer exceptional potential in phototherapy applications owing to their unique electronic structures. However, developing metal-organic frameworks (MOFs) that incorporate photosensitive corroles as functional ligands for synergistic phototherapy remains a formidable challenge. Herein, for the first time, the unique phosphorus corrole-based MOFs Cor(P)-Hf with (3,18)-connected gea topology are reported, which are constructed by Cs-symmetric dicarboxylate 3-connected linkers, 10-pentafluorophenyl-5,15-di(p-benzoate)phosphorus corrole (Cor(P)), and the peculiar D-symmetric 18-connected Hf-oxo clusters.

A FRET Autophagy Imaging Platform by Macrocyclic Amphiphile.

Autophagy is a ubiquitous process of organelle interaction in eukaryotic cells, in which various organelles or proteins are recycled and operated through the autophagy pathway to ensure nutrient and energy homeostasis. Although numerous fluorescent probes have been developed to image autophagy, these environment-responsive probes suffer from inherent deficiencies such as inaccuracy and limited versatility. Here, we present a modular macrocyclic amphiphile Förster Resonance Energy Transfer (FRET) platform (SC6A12C/NCM, SN), constructed through the amphiphilic assembly of sulfonatocalix[6]arene (SC6A12C) with N-cetylmorpholine (NCM) for lysosome targeting.

A Hydrolytically Stable Metal-Organic Framework for Simultaneous Desulfurization and Dehydration of Wet Flue Gas.

Metal-organic frameworks (MOFs) have great prospects as adsorbents for industrial gas purification, but often suffer from issues of water stability and competitive water adsorption. Herein, we present a hydrolytically stable MOF that could selectively capture and recover trace SO from flue gas, and exhibits remarkable recyclability in the breakthrough experiments under wet flue-gas conditions, due to its excellent resistance to the corrosion of SO and the water-derived capillary forces. More strikingly, its SO capture efficiency is barely influenced by the increasing humidity, even if the pore filling with water is reached.

Application of β-Keto Acylpyrazoles as 2C Synthons in Asymmetric Cyclizations of -Hydroxychalcones: Stereoselective Construction of -3,4-Dihydrocoumarins.

An asymmetric tandem esterification/Michael addition reaction of β-keto acylpyrazoles with -hydroxychalcones has been established under the catalysis of a bifunctional squaramide-tertiary amine. A wide variety of biorelevant 3,4-dihydrocoumarin derivatives were generally obtained in high yields (up to 93%) with excellent diastereo- and enantioselectivities (>19:1 dr, up to 93% ee) under mild reaction conditions. This reaction represents the successful application of β-keto acylpyrazoles as 2C building blocks in catalytic asymmetric cyclizations.

Intramolecular Hydrogen Bonds Weaken Interaction Between Solvents and Small Organic Molecules Towards Superior Lithium-Organic Batteries.

The strong interaction between organic electrode materials (OEMs) and electrolyte components induces a high solubility tendency of OEMs, thus hindering the practical application of lithium-organic batteries. Herein, we propose an efficient strategy for intramolecular hydrogen bonds (HBs) to redistribute the charge of OEMs to weaken the interaction with electrolyte components, thereby suppressing their dissolution. For the designed 2,2',2''-(2,4,6-trihydroxybenzene-1,3,5-triyl) tris (1H-naphtho[2,3-d]imidazole-4,9-dione) (TPNQ) molecule, the intramolecular HBs (O-H⋅⋅⋅N and N-H⋅⋅⋅O) reduce the charge density of active sites and alter the charge distribution on the molecular skeleton.

pH-Responsive Persistent Luminescent Nanosystem with Sensitized NIR Imaging and Ratiometric Imaging Modes for Tumor Surgery Navigation.

Owing to autofluorescence-free feature, persistent luminescent (PersL) nanoparticles (PLNPs) become potential materials for tumor surgical navigation. However, it is still challenging to enhance PersL intensity, contrast ratio, and imaging stability so as to meet clinical demand and avoid missed detection of microlesions. Herein, integrating a tumor microenvironment (TME)-responsive strategy, sensitization enhancement, and internal-standard ratiometric method, a dual-mode PersL imaging strategy is proposed: After loading pH-responsive fluorescent molecule Rh-ADM on PLNPs ZnGaO:Cr,Mn (ZGCM-Rh8), the fluorescence resonance energy transfer (FRET) pathways between Cr and Rh-ADM, as well as Mn and Rh-ADM, could sensitize the NIR PersL emitted by Cr and quench the green PersL from Mn at acidic TME, respectively.

Surface-Assisted Passivation Growth of 2D Ultrathin β-BiO Crystals for High-Performance Polarization-Sensitive Photodetectors.

2D nonlayered materials (NLMs) have garnered considerable attention due to unique surface structure and bright application prospect. However, owing to the strong interatomic forces caused by intrinsic isotropic chemical bonds in all directions, the direct synthesis of ultrathin and large area 2D NLMs remains a tremendous challenge. Here, the surface-assisted passivation growth strategy is designed to synthesize ultrathin and large size β-BiO crystals with the thickness down to 0.

In Situ Welding Ionic Conductive Breakpoints for Highly Reversible All-Solid-State Lithium-Sulfur Batteries.

Poly(ethylene oxide) (PEO)-based solid-state lithium-sulfur batteries (SSLSBs) have garnered considerable interest owing to their impressive energy density and high safety. However, the dissolved lithium polysulfide (LiPS) together with sluggish reaction kinetics disrupts the electrolyte network, bringing about ionic conductive breakpoints and severely limiting battery performance. To cure this, we propose an in situ welding strategy by introducing phosphorus pentasulfide (PS) as the welding filler into PEO-based solid cathodes.

Space-Confined Vertical Growth of Large-Size Organic Semiconductor Single Crystals.

Organic semiconductor single crystals (OSSCs) have garnered considerable attention because of their high charge mobility and atomic-scale smooth surface. However, their large-size high-quality preparation remains challenging due to the inevitable defects and limited growth speed brought by traditional epitaxial growth. Here, we demonstrate a space-confined strategy, named out-of-plane microspacing in-air sublimation (OPMAS), for growing vertically millimeter-sized OSSCs in several minutes by revolutionizing the heterogeneous epitaxial growth mode severely depending on substrates into a spontaneous homogeneous growth mode free from substrates.

Organotropic Engineering of Luminescent Gold Nanoclusters for In Vivo Imaging of Lung Orthotopic Tumors.

Gold nanoclusters (AuNCs) are emerging as promising functional probes for bioapplications. However, because of rapid renal clearance, it is a challenge to tailor their biofate and improve their disease-targeting ability in vivo. Herein, we report an efficient strategy to tailor their organotropic actions by rationally designing AuNC assemblies.

Leveraging independent component analysis to unravel transcriptional regulatory networks: A critical review and future directions.

Transcriptional regulatory networks (TRNs) play a crucial role in exploring microbial life activities and complex regulatory mechanisms. The comprehensive reconstruction of TRNs requires the integration of large-scale experimental data, which poses significant challenges due to the complexity of regulatory relationships. The application of machine learning tools, such as clustering analysis, has been employed to investigate TRNs, but these methods have limitations in capturing both global and local co-expression effects.