The frequent occurrence of oil spills not only results in the waste of petroleum resources, but also poses a serious threat to the marine ecological environment. Considering the large amount of crude oils with high viscosity, it is urgent to develop an adsorbent capable of efficiently reducing the viscosity for the cleanup of oil spills. Inspired by the “lotus effect” and “poikilotherm which utilize the solar energy for thermoregulation”, the low surface energy material polydimethylsiloxane (PDMS) and polypyrrole (PPy) were loaded over the island nonwoven fabric to fabricate a novel crude oil adsorbent material. Wherein, the fluorine-free PDMS was used to hydrophobically modify the nonwoven fabric, endowing it with excellent oil-water separation performance, with a separation efficiency of up to 95%. After 10 cycles, the separation efficiency of PPy/PDMS modified nonwoven fabric (PPy/PDMS@NF) was still above 90%, demonstrating superior recyclability. In addition, the PPy/PDMS@NF possessed the self-cleaning capabilities. Under one sun illumination (1.0 kW/m2), the surface temperature of the PPy/PDMS@NF reached to 60.7 ℃, and its adsorption capacity for high-viscosity crude oil reached to 7 gcrude oil/gsorbent. Thanks to its environmental friendliness and excellent adsorption capacity, this work provides a new option for dealing with the high-viscosity marine oil spill.

A design strategy towards stable fluorenyl radicals (FRs) is established by introducing donor-π-radical (D-π-R) conjugation between amine N atoms and FR centers through phenyl or 9-anthryl moieties. Four FRs with or without N atom containing protecting groups were designed and synthesized for comparison. X-ray crystallographic analysis displayed planar fluorenyl skeletons of CDP-FR and MA-FR, which form large dihedral angles with protecting groups. Even though, the increased bond-order of C-C and C-N bond be-tween radical center and N atoms by Wiberg bond analysis of all FRs confirmed the D-π-R conjugation. Time-dependent DFT calcula-tions based on frontier molecular orbital analysis further revealed the contribution of D-π-R structures as donor-acceptor effect on the lowest energy absorptions of carbazole and diphenylamine substituted CDP-FR and DPAA-FR. Therefore, beneficial from D-π-R conjugations, CDP-FR and DPAA-FR showed better photo-stability than TP-FR and MA-FR. Our study here provides a new strategy to design and synthesize persistent stable monoradicals.

3,3-disubstituted oxindoles, forming the core of extensive bioactive natural products and drugs, attract tremendous efforts to develop efficient methods for their preparation. Here, a substrate-photosensitive strategy for the selective synthesis of 3-substituted 3-aminooxindoles from N-Boc isatin ketimines irradiated by visible light was reported with high yields and broad functional group compatibility.

Natural products with high oxidation states and complex chemical skeletons exhibit diverse bioactivities due to their unique interactions with biological targets. The high oxidation state is characterized by the presence of multiple oxygen-containing functional groups such as hydroxyl groups, carbonyl groups, and epoxides that are usually tough to construct selectively. In recent years, thanks to the development of efficient strategies and sophisticated methodologies, significant advancements have been made in the total syntheses of highly oxidized natural products (HONPs), which are reviewed herein.

Imbalance in the levels of ascorbic acid (AA) can pose a risk to human health. Therefore, it’s essential to establish an accurate method for the detection of AA. In this work, a novel N-doped carbon composite (MnOx@NC) with dual enzyme-like activities to detect AA was prepared by calcination of Mn-MOF containing H3TTPCA ligand. Interestingly, the •O2− that leads to its oxidase-like activity was not formed by dissolved oxygen, but came from the synergistic effect of lattice oxygen generated by calcination and the transformation of MnⅡ/MnⅢ/MnⅣ, and the presence of H2O2 provided much •OH, which cause its peroxidase-like activity. Meanwhile, the residual N element came from H3TTPCA ligand assisted the catalytic process. Accordingly, a dual-signal sensing platform and smartphone-assisted recognition for detection of AA was developed and a colorimetric sensor array was established to distinguish three antioxidants. This work also demonstrates considerable promise for the detection of AA in authentic pharmaceuticals.

The morphology of the active layer plays a crucial role in the performance of organic photovoltaics. Although volatile additives are commonly used to manipulate the morphology, their mechanism of action remain poorly understood. In this study, we conducted a systematic exploration of the mechanism of the traditional volatile additive 1-CN in film formation kinetics of typical PM6:Y6 system. We found that 1-CN induces a secondary aggregation effect, improving film morphology and promoting face-on crystalline orientation. Through elucidating its impact on exciton dynamics, we established a link between morphology optimization and increased exciton diffusion length and accelerated charge separation. Our findings unveil the unique mechanism of action of volatile additive, providing a new perspective for improving the morphology and enhancing the performance of organic photovoltaic devices.

An efficient, additive- and catalyst -free, visible-light-driven radical C-H methylation of heteroarenes (including quinoxalinones, pyra-zinones, quinolinones and coumarins) utilizing readily available methylamines as the methyl source has been developed. The trans-formation possesses the advantages of operational simplicity, mild reaction conditions and broad substrate scope. Mechanistic studies disclosed that a photoactive electron donor-acceptor (EDA) complex between methylamines and heteroarenes is crucial to this trans-formation.

The development of new efficient strategies for the construction of the C-S bond has attracted considerable interest due to its presence in various crucial biological systems and pharmaceutical compounds. Alkene hydrothiolation is one of the simplest and most atom-economic methods for organosulfur synthesis. This review focuses on transition-metal-catalyzed C-S bond formation via alkene hydrothiolation with thiols and is divided into three sections covering 3d, 4d, and 5d transition-metal-catalyzed hydrothiolation re-ported from 2013 to the present. Synthetic methods, substrate scope, and reaction mechanisms are discussed. We aim to provide a concise overview of recent advances in the hydrothiolation of alkenes and hopefully encourage further exploration to fill the gaps. The current landscape suggests considerable potential for future innovation and discovery in this field.

A practical molecular editing strategy has been established for the direct and consecutive C-3 diazenylation and C-2 arylation of indoles with aryltriazenes under metal-free and ambient conditions. A sequence of tandem reactions has been developed via the sustained release of aryldiazonium species from aryltriazenes to achieve the controlled multiple bonds sequential cleavage and formation. This strategy enables the regio- and chemo-controlled consecutive C−H functionalization of indole at two adjacent reactive sites (C-2 versus C-3) without pre-functionalization of the reactive sites and even without the assistance of the directing group, metal catalyst or ligand. Detailed mechanistic experiments and DFT calculations along with supported a sequence of tandem reaction mechanisms. The synthetic importance of this methodology is evident from the simple operation, good functional group tolerance, gram-scale synthesis, late-stage modification of pharmaceuticals and in vitro cytotoxicity evaluation.

Here, we present a 6-step gram-scale synthesis of (±)-gregatin A, a fungal polyketide characterized by an alkylated furanone core origi-nally isolated from Cephalosporium gregatum. The synthetic route features an intermolecular 1,3-dipolar cycloaddition, a Mo-mediated disconnection of isoxazole skeleton, and an acid-mediated desilylation/enamine hydrolysis and hemiketalization cascade. Notably, this synthetic approach establishes a versatile platform applicable to the synthesis of diverse gregatin congeners, allowing for the introduc-tion of varied side chains. Our method not only facilitates the scalable production of (±)-gregatin A but also opens avenues for the ex-ploration of structural analogs with unique biological activities.

Carbon, with its excellent conductivity and structural stability, plays a crucial role in energy storage and conversion technologies and is considered an ideal choice in electrochemical energy storage for electrode materials. To address these needs and safeguard the environment, scientists have been investigating novel approaches to synthesis. In this field, molten salts or salt melts have emerged as a powerful and environmentally friendly alternative for synthesizing porous carbon materials with tunable chemical and structural properties. These salt systems can serve not only as solvents and reaction media but also as templates. Similar to traditional templating strategies, porous carbon materials synthesized using salt templates do not sacrifice carbon yield, but what sets them apart from traditional methods is that template removal can be achieved through deionized water washing. This article introduces a self-activation method that is applied to the preparation of carbon nanomaterials with high porosity and enormous specific surface area. The working principle, process steps, preparation characteristics, and research progress of this process are summarized, and its potential applications in next-generation electrochemical energy storage devices are discussed and envisioned.

Bicyclo [3.2.1] octane-type intermediate (BOI) is a crucial intermediate that can react with water to undergo decarboxylation and produce theaflavins. Given this reactivity, it is logical to assume that BOI can also react with other polar solvents, such as alcohols, to yield the corresponding analogues. In this study, pyrogallol (PG) was used as the substrate and Ag2O as the oxidant to synthesize BOIPPG in an acetone system. Subsequently, our hypothesis was confirmed by the successful synthesis of e-substituted purpurogallin formic acid ester derivatives. Finally, we established a novel detailed mechanism for the generation of benzotropolone derivatives with the aid of a mechanical quantum.

Inverted (p-i-n) perovskite solar cells (PSCs) are favored by researchers owing to their superior compatibility with flexible substrates and tandem device fabrication. Additionally, the hole transport layer (HTL) serves as a template for perovskite growth, which is critical for enhancing the device performance. However, the current research on how the HTL promotes perovskite crystallization is insufficient. Here, 4PADCB, a self-assembled monolayer (SAM) hole transport material, was optimized as a superior template for perovskite growth through comparative analysis; accordingly, compact perovskite film with vertical growth was prepared. The better matched energy level alignment between 4PADCB and perovskite suppressed nonradiative recombination at the interface and enabled rapid hole extraction. Moreover, high-quality perovskite film growth on 4PADCB exhibited lower Young’s modulus and less residual stress. By integrating 4PADCB into p-i-n PSCs, the optimal device achieved a power conversion efficiency of 24.80%, with an open-circuit voltage of 1.156 V, thus achieving the best rank among devices without perovskite post-treatment, additives, dopants, or intermediate layers. Furthermore, the unencapsulated device demonstrated exceptional thermostability and photostability under maximum power point tracking. Thus, this work provides a new understanding for the development of novel SAMs and perovskite growth, and it is expected to further improve device performance.

Facile mass transport channel and accessible active sites is crucial for binder-free air electrode catalysts in rechargeable flexible zinc-air battery (ZAB). Herein, a ZnS/NH3 dual-assisted pyrolysis strategy is proposed to prepare N/S-doped hierarchical porous bamboo carbon cloth (HP-NS-BCC) as binder-free air electrode catalyst for ZAB. BCC fabric with abundant micropores is firstly used as flexible carbon support to facilitate the heteroatom-doping and construct the hierarchical porous structure. ZnS nanospheres and NH3 activization together facilitate the electronic modulation of carbon matrix by N/S-doping and optimize the macro/meso/micropores structure of carbon fibers. Benefiting from the highly-exposed N/S-induced sites with enhanced intrinsic activity, the optimized mass transport of biocarbon fibers, as well as the ultra-large specific surface area of 2436.1 m2 g-1, the resultant HP-NS-BCC catalyst exhibits improved kinetics for oxygen reduction/evolution reaction. When applied to rechargeable aqueous ZABs, it achieves a high open-circuit voltage of 1.516 V and a significant peak power density of 249.1 mW cm−2. As binder-free air electrode catalyst, the flexible ZAB also displays stable cycling over 500 cycles with a minimal voltage gap of 0.42 V, showcasing promising applications in flexible electronic devices.

A highly enantioselective palladium-catalyzed intramolecular Heck reaction of unactivated alkenes is developed, which provides a powerful route to access a broad range of chiral 3,3-disubstituted-2,3-dihydrobenzofurans bearing all-carbon quaternary stereocenter of interest in pharmaceutical research. Its salient features include high yield, excellent chemo- and enantioselectivity, mild condi-tions, a broad substrate scope as well as versatile transformations of the product.

A visible-light-induced photoredox-catalyzed regioselective and stereoselective C(sp2)-H amination of enamides with bench-stable and easily accessible N-aminopyridium salts is developed, affording synthetically and biologically prominent vicinal 1,2-diamine scaffolds in broad substrate scope and excellent functional group compatibility. The transformation proceeded through a radical pathway involving the Giese addition of the relatively electrophilic N-centered amidyl radical species to nucleophilic β-olefinic position of enamides followed by the ensuing single electron oxidation and β-H elimination, delivering geometrically-defined Z-configured β-amino enamides. The operational simplicity, environmentally friendliness and cost efficiency of this methodology has paved a new avenue to enrich the arsenal of synthetically crucial functionalized enamides and their derivatives.

Room-temperature sodium-sulfur (RT-Na/S) batteries display attractive potential in large-scale energy-storage, but their practical application was still restricted by the serious dissolution of polysulfides. Herein, supported by the constructing of interface engineering, the metal sulfide-carbon nanocomposite can be prepared with considerable electrochemical properties. Utilizing the double-helix structure of carrageenan-metal hydrogels as precursors, in-situ metal sulfide (MxSy) nanostructure/3D carbon aerogels (3D CAs) can be successfully constructed. Importantly, with the assistance of the vulcanization process, 3D carbon architecture was maintained in the composites and act as a skeleton to optimize their structural stability. As the anode of RT-Na/S batteries, ZnS/S@C and NiS2/S@C delivered an excellent cycling stability and rate performance (179.8mAhg−1 at 20Ag−1 after 10000 cycling for ZnS/S@C, 220.3 mAhg−1 at 10Ag−1 after 3000 cycling for NiS2/S@C). The detailed investigation of mechanism revealed that the powerful adsorption for Na2S4 was originated from 3D metal sulfide-carbon structure. The well-designed architecture of sulfide-carbon composites servers as an electrocatalyst to alleviate the shuttle effect of polysulfides, resulting in the long-term electrochemical stability. Given this, the work is expected to provide promising insights for designing advanced anode materials for RT-Na/S batteries.

Ten novel isocoumarins, including four pairs of enantiomers, were isolated from Artemisia dubia var. subdigitata (Asteraceae). Com-pounds 1, 2 and 3a/3b possessed a unique 6/6/6-tricyclic system comprising an unusual 1-(2-methylcyclohexyl) propan-1-one moiety fused with isocoumarin core skeleton. Compounds 4a/4b were characterized as an unexpected 2,5-dimethylcyclohexan-1-one scaffold, and compounds 5a/5b and 6a/6b were rare 1,2-seco-isocoumarin. Their structures and absolute configurations were elucidated through spectroscopic data, X-ray crystallography, ECD and NMR calculations with DP4+ analyses. Plausible biosynthetic pathways were proposed from the naturally occurring isocoumarin. Network pharmacological analysis suggested that the targets of compound 1 were significantly enriched in the cell cycle and PI3K-Akt signaling pathway. The molecular docking revealed that compound 1 had high binding affinity with CDK2 (total score: 6.8717). Furthermore, compounds 1 and 2 exhibited inhibitory activity on three human hepa-toma cell lines, with inhibitory ratios of 85.1% and 84.5% (HepG2), 88.2% and 87.3% (Huh7), and 69.2% and 69.1% (SK-Hep-1) at 200 μM, respectively.