Superatomic 1S orbital-mediated ethylene activation on Agn- clusters.

Single-cluster catalysts (SCCs) leverage superatomic properties via well-defined geometric/electronic configurations to enable novel reactions. The development of SCCs has facilitated atomic-level insights into catalyst design, thereby advancing our understanding of the fundamental nature of catalytic reactions. While orbital symmetry rules guide unimolecular catalyst design, the role of superatomic orbital symmetry in SCC reactivity remains elusive.

Carbonyl-rich organic cathodes for advanced aqueous batteries: progress and perspectives.

Aqueous batteries have garnered significant attention as compelling contenders for large-scale energy storage owing to their inherent safety, cost-effectiveness, and environmental sustainability. Significant endeavors have been dedicated to develop redox-active organic cathode materials, which is considered a crucial factor driving the development of aqueous batteries. Among various cathodes, carbonyl-rich organic compounds demonstrate exceptional potential in view of their strong electroactivity, ion-coupling sensitivity and structural versatility.

Photoinduced Amination of Endocyclic 1-Azaallyl Radicals.

A catalyst-free method has been discovered based on photoexcited electron donor-acceptor complexes to generate an iminyl radical and endocyclic 1-azaallyl radicals, elusive intermediates that have never been reported in synthesis. The two radicals then combine and, following reduction, ultimately provide unprotected 2-(hetero)aryl-3-aminopiperidines. This reaction expands the knowledge and synthetic application of endocyclic 1-azaallyl synthons with an intrinsic ring strain.

Enantioselective Radical-Radical Cross-Couplings of β-Hydroxy Amides and -Hydroxyphthalimide Esters via Ni/Photoredox Catalysis.

Enantioselective alkyl-alkyl cross-coupling is a powerful yet challenging strategy for constructing three-dimensional molecular architectures, which are essential in fields such as organic chemistry and pharmaceutical chemistry. While radical-radical cross-coupling offers a promising approach, achieving control over both cross- and enantioselectivity between two distinct alkyl radicals remains a formidable challenge due to their transient nature. In this article, we introduce a practical platform that combines photoredox and chiral nickel catalysis to tame transient primary and secondary alkyl radicals under mild conditions.

Hydrogen-Bonded Interfacial Super-Assembly of Spherical Carbon Superstructures for High-Performance Zinc Hybrid Capacitors.

Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors, but their tailor-made design to optimize the capacitive activity remains a confusing topic. Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures (SCSs) for Zn-ion storage with double-high capacitive activity and durability. Tetrachlorobenzoquinone (H-bond acceptor) and dimethylbenzidine (H-bond donator) can interact to form organic nanosheet modules, which are sequentially assembled, orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds (N-H···O).

Exciton Regulation and Fluorescence Switching via Redox-Responsive Heterojunction Interfaces.

Redox-responsive fluorescence regulation at heterointerfaces remains a critically underdeveloped yet strategically significant domain in advanced chemical sensing. Herein, we present an exciton modulation strategy enabled by heterojunction engineering between electron-rich CdSe quantum dots and an electron-deficient covalent triazine framework (CTF). This type-I CdSe@CTF heterostructure achieves nanoscale electronic decoupling and directional charge redistribution, unveiling a previously unreported fluorescence-switching mechanism governed by redox-triggered interfacial reconfiguration.

An Innovative Inter-Spectral Distance-Based Approach to Analyzing MALDI-TOF Mass Spectra of Closely Related Microbial Species.

Rationale: Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) is a highly efficient technique for microbial identification; however, the accuracy has always been a problem when identifying closely related microbial species. Improving spectral data identification algorithms is one of the key approaches to enhancing the discriminatory power and reliability of identification for the closely related species.

Methods: This study develops a dimensionality reduction method based on inter-spectral distance computation for the analysis of MALDI-TOF MS data.

Copper-Mediated C4-H Sulfonylation of Indoles via a Transient Directing Group Strategy.

The synthesis of C4-decorated indoles is of great significance in the construction of bioactive and functional molecules. Currently, the late-stage C4-H functionalization of indole scaffolds largely relies on toxic and expensive 4d/5d transition metal catalysts and preinstalled directing groups, which considerably limits their practical applications. In this work, we report a copper-mediated C4-H sulfonylation of indoles via a transient directing group strategy.

Unlocking the potential of a multi-electron p-type polyheterocycle cathode: when it meets a small-size and high-charge anion.

High-voltage p-type organic cathodes are attracting broad attention for boosting zinc batteries, but are hindered by single-electron reactions and low utilization of redox sites due to high reaction energy barriers with incompatible anions. Here we design polyheterocycle organics (PHOs) grafting dual-site-active phenothiazine and piperazine motifs to form donor-acceptor-extended structures which show multi-electron p-type redox reactions for superior anion storage. With the decrease in anionic Stokes radius and the increase in charge density (TFSI → OTF → SO ), SO exhibits the strongest bipedal ion-pairing ability with PHOs during oxidation an ultralow activation energy (0.

Asymmetric Charge Distribution of Dual Active Sites in Nitroaromatics Toward High-Performance Zinc Organic Batteries.

Organic small molecules have emerged as promising cathode candidates for aqueous zinc-ion batteries owing to their structural tunability and high redox activity. However, their development is hindered by inherently low operating voltages and limited specific capacities. Herein, a bipolar organic molecule is reported featuring intramolecular asymmetric charge distribution.

Molecular Engineering of Intrinsic Chromophoric Polyimides: Chemically Amplified Color Photoresists for Advanced Optical Systems.

Color photoresists represent a cornerstone technology in advanced optical systems, enabling critical functionalities ranging from flexible display pixel manufacturing to direct lithography of antidust color coatings for space exploration equipment. While conventional dye-polymer composite photoresists dominate industrial applications, their intrinsic limitations in thermal stability, mechanical durability, electrical insulation, and long-term color stability fundamentally restrict their deployment in extreme environments. This study pioneers a molecular engineering strategy to overcome these challenges through the development of intrinsically colored photosensitive polyimides (PSPIs).

Multifunctional Molecular Agent for Tau-targeted Combinational Therapy of Alzheimer's Disease.

Tau aggregation inhibitors or neurotoxic-metal chelators have been extensively studied as potential treatment for Alzheimer's disease. However, it is a great challenge to improve their therapeutic effects while reducing neurotoxicity. Herein, we designed and synthesized two new compounds, (1,4,7,10-tetraazacyclododecane-1,4,7,10-tetrayl)tetrakis((3,4,5-trihydroxyphenyl)methanone) (4GA) and (4,10-dimethyl-1,4,7,10-tetraazacyclododecane-1,7-diyl)bis((3,4,5-trihydroxyphenyl)methanone) (2GA).

Decomposition of AunO- clusters into gold oxide and metallic components: Unraveling the impact of single-atom oxygen on the reactivity modulation.

Gold clusters serve as ideal models for probing chemical bonding theories and their reactions with O2 provide valuable insights into the O2 activation mechanisms on gold-based catalysts. While extensive research has been conducted on pristine gold clusters, investigations into the reactivity of nonmetal-doped gold clusters remain limited. Here, we explore the reactions of AunO- (n = 5-20) with O2 using cluster reaction experiments and density functional theory calculations, and our findings reveal that many AunO- exhibits a structure-activity relationship different from those of pure gold clusters and small gold oxide clusters.

Deep reinforcement learning as an interaction agent to steer fragment-based 3D molecular generation for protein pockets.

Designing high-affinity molecules for protein targets (especially novel protein families) is a crucial yet challenging task in drug discovery. Recently, there has been tremendous progress in structure-based 3D molecular generative models that incorporate structural information of protein pockets. However, the capacity for molecular representation learning and the generalization for capturing interaction patterns need substantial further developments.

Te-Modulated Fe Single Atom with Synergistic Bidirectional Catalysis for High-Rate and Long-Cycling Lithium-Sulfur Battery.

Single-atom catalysts (SACs) have garnered significant attention in lithium-sulfur (Li-S) batteries for their potential to mitigate the severe polysulfide shuttle effect and sluggish redox kinetics. However, the development of highly efficient SACs and a comprehensive understanding of their structure-activity relationships remain enormously challenging. Herein, a novel kind of Fe-based SAC featuring an asymmetric FeN-TeN coordination structure was precisely designed by introducing Te atom adjacent to the Fe active center to enhance the catalytic activity.

Boosting Self-Trapped Exciton Emission via Interlayer Pillaring in Layered Lead Halide Frameworks.

Corrugated layered hybrid lead halides have emerged as a promising class of intrinsic broadband self-trapped exciton (STE) emitters for single-component white-light emission. However, regulating the structure to improve photoluminescence performance while maintaining a high intrinsic stability remains challenging. In this study, we introduce an elongated and nonconjugated biscyclohexyl dicarboxylate ligand to pillar two new members of ultrastable layered lead halide frameworks.

Evolution of CoNi Alloy Electronic Structure Buffered by Carbon Nanolayer to Tune Selective Generation of Reactive Oxygen Species.

Generation of non-radical reactive oxygen species (ROS) via peroxymonosulfate (PMS) activation is desired to drive selective Fenton-like reactions and strongly affected by the electronic structure of catalyst. While the static structure-activity relationship of catalysts is well explored, how the evolution of electronic structure dynamically affects the ROS generation remains poorly understood. This study fabricated carbon nanolayer-supported CoNi alloys (CoNi@CNT) with preset atomic Ni/Co ratio (x/y = 1:3, 2:2, 3:1) to probe the dynamic evolution of electronic structure and its subsequent role for the generation of non-radical ROS.

Tetrahedron DNA Nanostructures as microRNA Inhibitors to Alleviate Acute Pancreatitis.

Acute pancreatitis (AP) is an inflammatory pancreatic disorder characterized by tissue damage and necrosis. It not only affects the pancreas but also triggers systemic inflammatory responses, leading to multiorgan failure and potentially death. In recent years, microRNA (miRNA) sponges have demonstrated promise to enhance AP treatment outcomes by inhibiting specific miRNAs.

Local Acidic Microenvironment Construction via Alternating Current Electro-Fenton Process for Green Efficient Water Purification under Neutral Conditions.

The direct current electro-Fenton (DCE-Fenton) process is limited by finite Fe species cycling, low HO utilization rate, and stringent acidic pH requirements. In this study, a heterogeneous alternating current electro-Fenton (ACE-Fenton) process is proposed for the first time to achieve efficient pollutant removal under neutral conditions, leveraging enhanced Fe species cycling and the creation of a local acidic microenvironment to improve the HO utilization efficiency and •OH generation efficiency. For different pollutants, the ACE-Fenton process operates efficiently at pH = 7 with a pseudo-first-order kinetics constant that is 5.

Tumor Cell Membrane-Coated Oxygen-Evolving Carbon Nitride Nanozymes Combined with Curcumenol Delivery for Lung Cancer Therapy via 'Open-Source Throttling' Strategy.

Although nanozyme-mediated catalytic therapy presents promising prospects for cancer therapy, insufficient tumor targeting, a hypoxic tumor environment and high glutathione (GSH) levels limit its efficacy. Herein, a novel biomimetic Ce-doped carbon nitride nanozyme (MCeCN) with multiclass enzyme catalytic activity, oxygen generation, and targeted delivery of curcumenol (Cur) is developed for the combined treatment of non-small-cell lung cancer (NSCLC). Owing to the wrapping of the A549 cell membrane, these biomimetic nanoparticles demonstrate effective active targeting of NSCLC.

Molecular-Level Design of Polymeric Semiconductor Nanomotors with Multichannel Sensitive 3D Motion for Microorganism Inactivation.

The advancement of high-performance photocatalysts is crucial for the iteration of light-driven micro/nanomotors. However, most existing light-driven micro/nanomotors, which are typically fabricated from inorganic semiconductors, suffer from limited visible-light absorption and inadequate control over 3D motion. Polymeric semiconductors, as emerging photocatalytic materials, feature narrow bandgaps, tunable band structures, and the potential for rational molecular design to optimize activity.

Epichlorohydrin cross-linked chitosan for adsorption of reactive red 2 dye: Optimization and adsorption mechanism.

The direct discharge of wastewater containing chemical dyes seriously affects human health. Here, we prepared novel adsorbent cross-linked chitosan beads for adsorption of chemically synthesized dyes. The prepared chitosan beads were tested for a series of characterization and adsorption properties.

Fluorescence from pentacyanopropenide in melamine.

Aggregation-induced optical phenomena are at the forefront of modern materials science. In this work, tetracyanoethylene (TCNE) is reacted and encapsulated within melamine. Crystallization from aqueous tetrahydrofuran solutions containing melamine and TCNE at varying concentrations yields colorful crystals exhibiting multi-wavelength fluorescence emission.

Interfacial Engineered Perylene Diimide Sensitized Photocathode for Enhanced Photoelectrocatalytic Energy-Demanding Reduction Reactions.

Dye-sensitized photoelectrochemical cells (DSPECs) are emerging inexpensive devices for solar fuels production and chemical upgrading, yet their efficiency remains limited by poor photocurrent density especially in energy-demanding reactions. Here, we introduce a molecularly engineered photocathode that integrates perylene diimides (PDI)-capable of consecutive photoinduced electron transfer (ConPET) to generate an excited state (PDI) with potent reducing power-on a transparent conductive indium tin oxide nanoparticle (nanoITO) thin film substrate. By introducing an AlO atomic layer via atomic layer deposition (ALD) onto the interface of PDI and nanoITO, the nonproductive back-electron transfer (BET) was significantly suppressed by over 95%, as quantified by transient absorption spectroscopy, while preserving the exceptional photoredox activity of PDI.