Regulating the Thermodynamic Uniformity and Kinetic Diffusion of Zinc Anodes for Deep Cycling of Ah-Level Aqueous Zinc-Metal Batteries.

Zn metal anodes in mildly acidic electrolytes usually suffer from a series of problems, including parasitic dendrite growth and severe side reactions, significantly limiting the Zn utilization efficiency and cycling life. A deep understanding of the Zn stripping/plating process is essential to obtain high-efficiency and long-life Zn metal anodes. Here, the factors affecting the Zn stripping/plating process are revealed, suggesting that thermodynamic uniformity in bulk structures promotes an orderly Zn stripping process, and a fast kinetic diffusion rate on the Zn surface facilitates uniform Zn deposition.

QUEST#4X: An Extension of QUEST#4 for Benchmarking Multireference Wave Function Methods.

Given a number of data sets for evaluating the performance of single reference methods for the low-lying excited states of closed-shell molecules, a comprehensive data set for assessing the performance of multireference methods for the low-lying excited states of open-shell systems is still lacking. For this reason, we propose an extension (QUEST#4X) of the radical subset of QUEST#4 ( , , 3720) to cover 110 doublet and 39 quartet excited states. Near-exact results obtained by iterative configuration interaction with selection and second-order perturbation correction (iCIPT2) are taken as benchmark to calibrate static-dynamic-static configuration interaction (SDSCI) and static-dynamic-static second-order perturbation theory (SDSPT2), which are minimal MRCI and CI-like perturbation theory, respectively.

Cyclo-N : a Novel 5/6 Fused Polynitrogen Anion for High Energy Density Materials.

After cyclo-pentazolate anion, a 5/6 fused structure of N is constructed, and four novel nitrogen-rich ionic compounds are assembled on its basis. The results of the quantum calculations revealed an uneven distribution of electrons on cyclo-N , with significant charge density near the N5/N9 atoms and an ADCH charge of -0.425.

Molecularly imprinted electrochemical sensor to sensitively detect tetramethylpyrazine in Baijiu.

Tetramethylpyrazine (TMP) is a compound known for its natural health benefits, but current detection methods for TMP are overly expensive and time-consuming. In this study, we developed functional materials with TMP molecular recognition properties using molecularly imprinted technology. As TMP does not produce electrochemical signals in the detection potential range, hexacyanoferrate was selected as a redox probe, combined with the highly conductive polymer PEDOT:PSS to enhance electrode conductivity.

Aerolysin Nanopore Electrochemistry.

ConspectusIons are the crucial signaling components for living organisms. In cells, their transportation across pore-forming membrane proteins is vital for regulating physiological functions, such as generating ionic current signals in response to target molecule recognition. This ion transport is affected by confined interactions and local environments within the protein pore.

The divergent reactivity of β-diketiminato aluminium hydrides with organophosphoryl compounds.

The reactions of LAlH (L = HC(CMeNAr), Ar = 2,6-PrCH) (1) with diphenylphosphane oxide [PhP(O)H], diphenylphosphinamide [PhP(O)NH], and diaryl/alkyl phosphane [(RO)P(O)H (R = Ph, or Pr)] afford their corresponding compounds with compositions LAl(H)OP(Ph) (2), LAl[OP(Ph)] (3), LAl{[N(H)P(O)(Ph)][OP(Ph)]} (4), LAl(OPr) (5), and LAl(OPh) (6), respectively. These reactions probably undergo a process of dehydrogenation coupling, deaminating dehydrogenation coupling, or chain-breaking coupling. It is noteworthy to mention that the reaction of compound 1 with 2 equiv.

Manipulating the interfacial integration mode of a bio-templated porous ZSM-5 platform with an Au/CuZnO catalyst for enhanced efficiency and recycling stability in glycerol conversion to 1,3-dihydroxyacetone.

Despite the potential to significantly enhance the economic viability of biomass-based platforms through the selective conversion of glycerol to 1,3-dihydroxyacetone (DHA), a formidable challenge persists in simultaneously achieving high catalytic activity and stability along this reaction pathway. Herein, we have devised a strategic approach to manipulate the interfacial integration within composite catalysts to address the performance trade-off. Through the modulation of the composite process involving a bio-templated porous ZSM-5 zeolite platform (bZ) and an Au/CuZnO catalyst, three distinct interfacial bonding modes were achieved: physical milling, encapsulation by zeolite, and growth on zeolite.

Symmetry Breaking: Case Studies with Organic Cage-Racemates.

ConspectusSymmetry is a pervasive phenomenon spanning diverse fields, from art and architecture to mathematics and science. In the scientific realms, symmetry reveals fundamental laws, while symmetry breaking─the collapse of certain symmetry─is the underlying cause of phenomena. Research on symmetry and symmetry breaking consistently provides valuable insights across disciplines, from parity violation in physics to the origin of homochirality in biology.

NIR-II absorption and photothermal conversion in a photochromic metal-organic framework based on -2,2'-biquinoline-4,4'-dicarboxylate.

A BCA -coordinated MOF (1) was initially discovered to exhibit electron transfer photochromism. Remarkably, the photogenerated radicals (1P) showed a maximum absorption enhancement peak at 1158 nm, resulting from the synergistic effects of planar π-conjugation induced by -coordination and π-π interactions among [BCA]˙˙ radicals, thereby promoting the NIR-II photothermal effect.

Constructing fecal-derived electrocatalysts for CO upcycling: simultaneously tackling waste and carbon emissions.

The escalating global fecal waste and rising CO levels present dual significant environmental challenges, further intensified by urbanization. Traditional fecal waste management methods are insufficient, particularly in addressing the related health risks and environmental threats. This study explores the synthesis of biochar from pig manure as a carbon substrate to disperse and stabilize Cu nanoparticles, resulting in the formation of an efficient Cu-NB-2000 electrocatalyst for electrocatalytic CO reduction (ECR).

Spontaneously Photocatalytic Nanoplatform for Sensitive Diagnosis and Penetrated Therapy of Cancer.

In this study, a sensitive diagnosis and spontaneously photocatalytic therapy of cancer based on chemiluminescence (CL) and nanozyme was studied. Briefly, carbon nitride-supported copper nanoparticles (CuCNs) loaded with luminol (CuCN-L) were utilized to develop a microneedle patch (CuCN-L/MN). The CuCN-L probe could target overexpressed HO in the TME and actively emit CL to achieve cancer cell imaging for diagnosis.

Bromide-promoted cascade annulation of isocyanobiaryls with aldehydes through photoredox catalysis.

Herein, we report a cascade annulation of readily available isocyanobiaryls with simple aldehydes photoredox catalysis, providing a straightforward approach towards valuable 6-hydroxyalkylated phenanthridines. Mechanistic studies indicated the generation of a key acyl radical from aldehydes by hydrogen atom abstraction with a bromine radical. This protocol exhibits exceptional chemoselectivity, excellent tolerance of various functional groups and mild reaction conditions.

Solvent-Free Artificial Light-Harvesting System in a Fluid Donor with Highly Efficient Förster Resonance Energy Transfer.

Multi-step Förster resonance energy transfer (FRET) plays a vital role in photosynthesis. While the energy transfer efficiency (Φ) of a naturally occurring system can reach 95%, that of most artificial light-harvesting systems (ALHSs) is still limited. Herein, we propose a strategy to construct highly efficient ALHSs using a blue-emitting, supercooled ionic compound of naphthalimide (NPI) as the donor, a green-emitting BODIPY derivate as a relay acceptor, and a commercially available, red-emitting dye [rhodamine B (RhB)] as the final acceptor.

Sabatier Principle Inspired Bifunctional Alloy Interface for Stable and High-Depth Discharging Zinc Metal Anodes.

Achieving stable Zn anodes is essential for advancing high-performance Zn metal batteries. Here, we propose a Sabatier principle inspired bifunctional transition-metal (TM) interface to enable homogeneous Zn dissolution during discharging and dendrite-free Zn deposition during charging. Among various TM-coated Zn (TM@Zn) electrodes, Cu@Zn exhibits the highest reversibility and structural stability, attributed to the optimal interaction between Cu and Zn.

Glycan-Matchmade Multivalent Decoration of Enzyme Labels for Amplified Electrochemical Detection of Glycoproteins.

Glycoproteins are of significant value to liquid biopsy of human diseases. Herein, we present a universal electrochemical platform for the amplified detection of glycoproteins, taking advantage of the glycan-matchmade multivalent decoration of enzyme labels for the enzymatic signal amplification. Briefly, the glycan-matchmade multivalent decoration involves two steps, i.

Phytic acid-based nanomedicine against mTOR represses lipogenesis and immune response for metabolic dysfunction-associated steatohepatitis therapy.

Metabolic dysfunction-associated steatohepatitis (MASH) is one of the most common chronic liver diseases and is mainly caused by metabolic disorders and systemic inflammatory responses. Recent studies have indicated that the activation of the mammalian (or mechanistic) target of rapamycin (mTOR) signaling participates in MASH progression by facilitating lipogenesis and regulating the immune microenvironment. Although several molecular medicines have been demonstrated to inhibit the phosphorylation or activation of mTOR, their poor specificity and side effects limit their clinical application in MASH treatment.

4D live tracing reveals distinct movement trajectories of meiotic chromosomes.

Proper chromosome alignment at the spindle equator is a prerequisite for accurate chromosome segregation during cell division. However, the chromosome movement trajectories prior to alignment remain elusive. Here, we established a 4D imaging analysis framework to visualize chromosome dynamics and develop a deep-learning model for chromosome movement trajectory classification.

Divergent Synthesis of Polysubstituted 1,2-Dihydropyridines and Pyridines through Manganese-Mediated Radical Cascade Cyclization of Tertiary Enamides.

A Mn(III)-mediated radical cascade cyclization of -propargyl enamides with sodium sulfinates was developed. Mechanistic studies indicated that this cascade process is mainly composed of the chemoselective addition of sulfonyl radical to C≡C bond and the regioselective intramolecular 6--trig cyclization. This protocol provided a powerful method for the divergent synthesis of diverse polysubstituted -sulfonylpyridines or 1,2-dihydropyridines just by varying solvent and temperature featuring good functional group compatibility and simple operation.

Manipulating Dynamic Light-Driven Solid-Liquid Transition and Static Reversible Photochromism via Organic Cocrystal Strategy.

Developing of molecular crystalline materials with light-induced multiple dynamic deformation in space dimension and photochromism on time scales has attracted much attention for its potential applications in actuators, sensoring and information storage. Nevertheless, organic crystals capable of both photoinduced dynamic effects and static color change are rare, particularly for multi-component cocrystals system. In this study, we first report the construction of charge transfer co-crystals allows their light-induced solid-to-liquid transition and photochromic behaviors to be controlled by trans-stilbene (TSB) as an electron donor and 3,4,5,6-Tetrafluorophthalonitrile (TFP) as an electron acceptor.

Ce1-xMnxVO4 with Improved Activity for Low-Temperature Catalytic Reduction of NO with NH3.

Novel Ce1-xMnxVO4 catalysts prepared via modified hydrothermal synthesis were used in selective catalytic reduction of NO using NH3 (NH3-SCR). The Ce1-xMnxVO4 catalysts displayed optimum NO removal efficiency at 250 oC. Physicochemical properties including crystal type, morphology, particle size, elemental composition, BET surface area, chemical bond, and valence state were studied by XRD, TEM, EDS, N2 adsorption-desorption, Raman spectroscopy, and XPS.

Ocean wave-driven covalent organic framework/ZnO heterostructure composites for piezocatalytic uranium extraction from seawater.

Piezoelectric catalysis possesses the potential to convert ocean wave energy into and holds broad prospects for extracting uranium from seawater. Herein, the Z-type ZnO@COF heterostructure composite with excellent piezoelectric properties was synthesized through in situ growth of covalent organic frameworks (COFs) on the surface of ZnO and used for efficient uranium extraction. The designed COFs shell enables ZnO with stability, abundant active sites and high-speed electron transport channels.

Tailorable biosensors for real-time monitoring of stress distribution in soft biomaterials and living tissues.

Visualizing mechanical stress distribution in soft and live biomaterials is essential for understanding biological processes and improving material design. However, it remains challenging due to their complexity, dynamic nature, and sensitivity requirements, necessitating innovative techniques. Since polysaccharides are common in various biomaterials, a biosensor integrating a Förster resonance energy transfer (FRET)-based tension sensor module and carbohydrate-binding modules (FTSM-CBM) has been designed for real-time monitoring of the stress distribution of these biomaterials.

Structural Isomerism of {Ag14}10+ Nanocluster Encapsulated by Bowl-like Polyoxometalates.

The structural isomerism of atomically precise nanoclusters provides a preeminent theoretical model to investigate the structure-property relationships. Herein, we synthesized three bowl-like polyoxometalate (POM)-encapsulated Ag nanoclusters (denoted as {Ag14(Sb3W30)2}-1, {Ag14(Sb3W30)2}-1a, and {Ag14(Sb3W30)2}-2) via a facile one-pot solvothermal approach. Among them, for the first time, an unprecedented isomeric {Ag14}10+ nanoclusters are obtained in polyoxoanions {Ag14(Sb3W30)2}-1 and {Ag14(Sb3W30)2}-2, which should be probably induced by the different distribution of coordinating O atoms in two isomeric bowl-like {Sb3W30} ligands.

In situ synthesis of HKUST-1 on copper-ammonia fiber for preparation of quaternary-ammonium chitosan based active packaging with sustained-release cinnamaldehyde.

Cinnamaldehyde (CIN) is gaining interest as a highly effective natural antimicrobial agent to extend the shelf life of fruits. However, its inherent instability limits further applications. In this work, a new strategy for the synthesis of HKUST-1 to encapsulate CINs by in situ growth method using copper-ammonia fiber as precursors is proposed.

Nanoization of Technical Pesticides: Facile and Smart Pesticide Nanocapsules Directly Encapsulated through "On Site" Metal-Polyphenol Coordination Assembly for Improved Efficacy and Biosafety.

Facile pesticide nanocapsules were successfully prepared by directly encapsulating the antisolvent precipitation of pesticides through instantaneous "on site" coordination assembly of tannic acid and Fe, avoiding tedious preparation, time consumption, and large amounts of organic solvents. The pesticide nanocapsules showed excellent resistance to ultraviolet photolysis and rainwater washing owing to the nanocapsule walls. The smart pesticide nanocapsules exhibited the controlled release of pesticides under multidimensional stimuli, such as acidic/alkaline pH, glutathione, HO, phytic acid, laccase, tannase, and sunlight, which were related to the physiological and natural environments of crops, pests, and pathogens.