We report a non-biomimetic total synthesis of (+)-daphnepapytone A, an unprecedented member of the guaiane-derived sesquiterpenoids that displays moderate inhibitory activity against -glycosidase (IC50 = 159 ± 2.1 M) and possesses a highly strained bridging cyclobutane motif. Our de novo approach provided expedient access to the tetracyclic core of (+)-daphnepapytone A through an intramolecular allenyl

There were two mistakes in the chemical drawings in Table 2 in the published article. Compound 12o was mistakenly depicted as the 2-substituted pyridine derivative; however, the compound prepared was the 3-pyridine derivative. Furthermore, in compound 12z the methyl ester was mistakenly shown in the 6-position of the lactam, whereas it must be correctly depicted as the regioisomeric compound with the

In conventional studies, radicals and nonradicals were often considered independent mechanisms for organic pollutant oxidation, with their potential interaction between radicals and nonradicals largely overlooked in Fenton-like reactions. Herein, Cu-Co3O4 catalysts (x wt% Cu-Co3O4/OVs) featuring bifunctional bonding centers were fabricated, which enabled simultaneous co-capture of electron-rich contaminants

Intrinsically stretchable organic solar cells (IS-OSCs) are among the most promising technologies for wearable power applications. However, the development of electron acceptors that simultaneously meet the demands for high performance and mechanical stretchability remains a significant challenge. In this study, we creatively synthesized three oligomeric acceptors with flexible linkers (2YF-Br, 4YF-T

Ammonia (NH3) is an important feedstock for industry, an ideal energy carrier, and a perspective storage media for hydrogen. Recently, electrochemical NO3− reduction under acidic conditions has received considerable attention but it suffers from limited efficiency especially under low NO3− concentration. Here, we report an in-situ formed positively charged polyethyleneimine-modified Cu under acidic

Azobenzenes are versatile photoswitches that can be used to generate elaborate optical tools including photopharmaceuticals. However, the targeted application-guided design of new photoswitches with specific properties remains challenging. We have developed synthetic protocols for derivatives of the dfdc (di-ortho-fluoro-di-ortho-chloro) azobenzene scaffold with chemical alterations in the para-/ortho-positions

Accurately predicting the spin crossover (SCO) temperature (T1/2) in spin crossover compounds remains a significant challenge, due to their extreme sensitivity to minor variations in ligand and crystal structure. In this study, we uncover a critical link between the redox potential of ligands and SCO behavior within Hofmann-type clathrates {Fe(R-pbpy+)2[µ2-M(CN)4]2} (R = electron-donating or electron-withdrawing

Crosslinking strategies have emerged as an attractive technology for deciphering protein complexes and protein–protein interactions (PPIs). However, commonly used crosslinking strategies present significant challenges for the precise analysis of protein complexes and dynamic PPIs in native biological environments. Here, we report the development of the first visible-light-inducible lysine-specific

The inherent O2 sensitivity of Ni–Fe carbon monoxide dehydrogenases (CODHs), crucial for rapid CO to CO2 interconversion, presents substantial challenges for industrial application. Transforming CO/CO2, a prevalent anthropogenic air pollutant, into valuable carbon chemicals either directly or through intermediate steps via biocatalytic methods offers a promising pathway to achieve net-zero emissions

Understanding the hydrogenation behavior of *NO during electrochemical nitrate reduction reaction (NO3RR) is essential for designing catalysts with high selectivity toward ammonia (NH3) and valuable intermediates like hydroxylamine. Spinel cobalt oxides (Co3O4) are promising NO3RR electrocatalysts, yet the exact *NO hydrogenation mechanism remains unclear. Here, we integrate theoretical calculations

Antimicrobial resistance (AMR) is a severe threat to modern health care and must be addressed to prevent millions of deaths in the coming decades. Antimicrobial polymers (APs) do not provoke resistances and are promising alternatives to conventional antibiotics. Classic APs possess an amphiphilic structure (cationic and hydrophobic). Herein we question the necessity of amphiphilicity in APs and find

Luminescent emitters based on lanthanide ions are of ubiquitous importance in the biological sciences, but typically need sensitisation from a covalently attached adjacent chromophore – an “antenna” – to have suitable emission intensities. Here we show that the mechanical bond can be used to connect the antenna to the emitter, providing unique dynamic features and stimuli-responsiveness to the resulting

Recent advances in materials development for organic light-emitting diodes (OLEDs) have been driven by an emerging design concept known as multiple-resonance (MR), which provides the benefits of high efficiency and color purity required for commercial OLED displays. Borylation reaction constructing MR frameworks is a key step for developing new π-conjugated systems, while this reaction includes the

Chiral covalent organic frameworks (CCOFs) are promising candidates for chiral optoelectronics and sensing, but their weak solid-state fluorescence and chiroptical responses often limit practical utility. Here, we introduce a novel CCOF synthesized from achiral monomers, 2-hydroxy-1,3,5-benzenetricarbaldehyde and hydrazine, via imine condensation with chiral induction strategy, yielding salicylaldehyde

Achieving effective exciton dissociation and charge transport in linear polymer photocatalysts for H2O2 photosynthesis remains a formidable challenge. Herein, we fabricated three-motif cross-linked polymers by rationally introducing a third functional component into a two-motif linear polymer, which were employed for circulation-flow photocatalytic H2O2 production. By strategically modulating the third

Sodium metal batteries (SMBs) with gel polymer electrolytes (GPEs) are considered promising candidates for high energy-density batteries due to their high theoretical capacity and cost effectiveness. However, the intrinsic flammability of GPE poses challenges for their widespread application. Inspired by the concept of the capsules, a triethyl phosphate (TEP)-based GPE with co-sustained-release effect

Bioconjugation chemistry has been a powerful avenue in expanding the repertoire of druggable proteome, as well as in identifying new E3 ligases to support targeted protein degradation (TPD). However, a large fraction of proteome remains inaccessible with existing covalent probes. Herein, we incorporated various electron-withdrawing groups into styrene derivatives and identified β-nitrostyrene as a

Nonradiative (NR) processes are pivotal in engineering materials with tailored properties for energy utilization. However, their intrinsic rapidity and competitiveness pose huge challenges in on-demand manipulation. Herein, radical-assisted multiple NR processes were achieved to couple photothermy and photosensitization based on a unique near-infrared-absorbing diradical-featured croconium (CR) dendrimer

We synthesize and evaluate a diverse range of Mn/TiO2 catalysts with varying physical and redox properties for the methane-to-methyl-ester reaction using molecular oxygen in a diluted acid medium (10 wt% trifluoroacetic acid). Despite initial differences in manganese distributions, nearly all catalysts are active under the reaction conditions, and the degree of activity is partially correlated to catalyst

We report the synthesis and characterization of thio-tetracosulene 3, a highly twisted chiral macrocycle constructed via sulfur fluorine annulative substitution from a cyclometaphenylene derivative. It is the first macrocyclic aromatic compound with a plectonemic configuration, and the structure is unambiguously confirmed by single crystal X-ray diffraction study. The two enantiomers of 3 can be resolved

The fullerene family is known for its unique properties, facilitating the formation of large, lubricated nano-onions and the fragmentation into small carbon clusters through various processes. In this study, we explore the thermal evolution of C60 islands in Pt(111), focusing on the segregation of C60 islands, the formation of fullerene dimers, and the subsequent development of large graphene sheets

In this work, we introduce a modified dip-and-pull electrochemical X-ray photoelectron spectroscopy (ECXPS) approach that offers new mechanistic insight into the alkaline carbon monoxide reduction reaction (CORR) over a Cu(111) single crystal surface. We tackle two major unresolved questions in the CORR mechanism that persist in the literature. Firstly, we address the mechanism for methane formation

Supramolecular stereocomplexation is an important tool to advance sustainable polymers, and oxygen-containing polymers represent the most widely studied materials for stereocomplexation. However, the sulfur-containing analogues, a newly emerged class of sustainable polymers, remain essentially unexplored because of a significant challenge encountered in the synthesis of stereoregular polymers and relatively

In optimizing the trade-off between power density and phosphoric acid retention in PA-doped polybenzimidazole (PA-PBI) membrane for improving performance of high temperature proton exchange membrane fuel cells (HT-PEMFCs), the self-reinforcing network of interfacial interactions of the HT-PEMs has to be deeply investigated. Herein, a breakthrough strategy employing a quaternary ammonium (QA)-functionalized

The assembly of metal clusters with organic building units by covalent bonds to form crystalline metal cluster-based covalent-organic frameworks (MCCOFs) material is a novel strategy in the field of reticular synthesis. However, only 2, 3, and 6 connectivity (valency) of metal cluster-based MCCOFs have been achieved in reported structures. Developing a higher connectivity remains a great challenge

In various types of intelligent devices, such as bionic robots, flexible polymeric elastomeric materials are essential for their operation, alongside the rigid skeleton. Conventional polymeric elastomeric materials, however, encounter a compromise between intelligence and mechanical robustness. Here we construct ionic gel-based elastomers that harmoniously merge high intelligence with superior mechanical

A series of novel samarium complexes bearing cyclopentadienyl–amide chelate ligands were synthesized and characterized by X-ray analysis. The complexes function as effective proton-coupled electron transfer (PCET) catalysts, facilitating molybdenum-catalyzed ammonia formation from dinitrogen under ambient conditions. In this reaction system, the Sm complexes could be recycled over 300 times, and they

The development of high-energy-density batteries operable over a wide temperature range is critical for sustainable energy storage. Sodium-chlorine (Na-Cl2) batteries show promising high theoretical energy densities but face significant safety challenges due to gaseous chlorine, particularly at high temperatures. Replacing Cl2 with liquid Br2 to construct a new Na-Br2 battery mitigates gas risks but

Silylamides are important ligands in coordination chemistry for their ability to stabilize low-coordination numbers and provide soluble, and even volatile, metal complexes. Such compounds provide valuable insights into the fundamental bonding and reactivity of their respective metals. Despite the wealth of homo- and heteroleptic hexamethyldisilazide complexes of divalent 3d ions (Sc-Ni, Zn), attempts

Using a combination of metal-promoted reactivity, in-situ covalent bond modification, and hydrogen bonding-promoted fluorine labilization, a unified approach was developed to self-assemble a library of customizable ligand architectures directly at the nickel center via selective cleavage of C‒F or C‒O bonds and the formation of C‒C or C‒N bonds. As a result, a structurally diverse set of nickelacarbatrane