Abstracts

Owing to the function of manipulating light absorption distribution, tandem organic solar cells containing multiple sub-cells exhibit high power conversion efficiencies. However, there is substantial challenge in precisely controlling the inter-subcells carrier migration which determines the balance of charge transport across the entire device. The conductivity of “nanowires”-like conducting channel in interconnecting layer between sub-cells should be improved which calls for fine engineering on the morphology of polyelectrolyte in interconnecting layer. Here we develop a simple method to effectively manipulating the domains of conductive components in commercial available polyelectrolyte PEDOT:PSS. The using of poor solvent could effectively modify the configuration of polystyrene sulfonic acid and thus the space for conductive components. Based on our strategy, the insulated shells wrapping conductive domains are thinned and the efficiencies of tandem organic solar cells are improved. We believe our method might provide guidance for the manufacture of tandem organic solar cells.

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Comprehensive Summary

Carbon dioxide can be converted into functional heterocycles known as cyclic carbonates, whose recent reactivity has been expanded towards the formation of tailor-made engineering polymers. This minireview gives an overview of the most topical developments in this area with a special focus on the synthetic methods employed to prepare these CO₂ based synthons. In addition, their application potential in the area of polymer science using a variety of polymerization techniques is discussed that have in common the ring-opening of the carbonate monomers. Future perspectives are provided that provide impetus for the scientific communities aligning research to the use of sustainable processes for polymers from recyclable carbon sources such as CO₂.

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Comprehensive Summary

Rationally developing efficient and durable bifunctional catalysts toward oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is critical for rechargeable zinc-air batteries (ZABs). Herein, a bead-like CoSe₂@NC@NCNFs bifunctional catalyst was designed and fabricated by confining cubic CoSe₂ nanoparticles to three-dimensional (3D) porous MOFs-derived nitrogen-doped carbon (NC) and one-dimensional (1D) N-doped carbon nanofibers (NCNFs) through a facile encapsulate strategy. The 1D/3D continuous network structure contributes to the improvement of specific surface area and electronic conductivity, while the strong synergistic effect between CoSe₂ sites and Co-N_x-C sites can effectively enhance electron/mass transfer and reduce the diffusion resistance. The as-constructed CoSe₂@NC@NCNFs catalyst exhibit high catalytic activity and stability toward ORR/OER with a high half-wave potential of 0.80 V (vs. RHE) in ORR and a low overpotential of 280 mV at 10 mA cm⁻² in OER. More encouragingly, the rechargeable ZABs with CoSe₂@NC@NCNFs cathode deliver high peak power densities (126.8 mW cm⁻²), large specific capacities (763.1 mA h g⁻¹), and robust charge-discharge cycling stability over 240 cycles. This study provides a facile strategy for designing efficient bifunctional catalysts for rechargeable energy conversion applications.

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Comprehensive Summary

Cell-free expression systems have emerged as a versatile and powerful platform for metabolic engineering, biosynthesis and synthetic biology studies. Nevertheless, successful examples of the synthesis of complex natural products using this system are still limited. Bicyclomycin, a structurally unique and complex diketopiperazine alkaloid, is a clinically promising antibiotic that selectively inhibits the transcription termination factor Rho. Here, we established a modular cell-free expression system with cascade catalysis for the biosynthesis of bicyclomycin from a chemically synthesized cyclodipeptide. The six cell-free expressed biosynthetic enzymes, including five iron- and α-ketoglutarate-dependent dioxygenases and one cytochrome P450 monooxygenase, were active in converting their substrates to the corresponding products. The co-expressed enzymes in the cell-free module were able to complete the related partial pathway. In vitro biosynthesis of bicyclomycin was also achieved by reconstituting the entire biosynthetic pathways (i.e., six enzymes) using the modular cell-free expression system. This study demonstrates that the modular cell-free expression system can be used as a robust and promising platform for the biosynthesis of complex antibiotics.

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This review comprehensively summarizes the various structures of Fe-MOFs, along with recent research progress on their synthesis and multifunctional applications in gas storage and separation, catalysis, bioimaging, and magnetism.

Comprehensive Summary

Iron-based metal-organic frameworks (Fe-MOFs) have attracted extensive interest from researchers due to their tunability, favorable properties, and chemical versatility. Compared with conventional porous materials, Fe-MOFs exhibit better performance in a wide variety of applications. Herein, the structures of Fe-MOFs are summarized to explore potential structures based on isoreticular chemistry, as well as the recent research progress in their synthesis and multifunctional applications. The rapid development of Fe-MOFs has broadened the application range of Fe-MOFs, and a brief description of Fe-MOF applications in gas storage and separation, catalysis, bioimaging, and magnetism is outlined, with the aim to expand the prospects of Fe-MOFs in more practical applications.

Quinazolone and imidazole were introduced to both sides of ethenone to construct novel structural quinazolone-derived imidazolenones as unique multitargeting antibacterial agents. The medicinal identification revealed that quinazolone-derived imidazolenones were expected to be further developed into a novel class of multitargeting antimicrobial agents to cope with multi-drug resistant bacterial infections.

Comprehensive Summary

Alkaloids are one of the prominent members in the development of new antimicrobial agents. This work discovered a class of alkaloid quinazolone-derived imidazolenones as novel structural type of antibacterial agents with large potential to treat severe bacterial infections in the agricultural and food field. Preliminary bioactive assay displayed that some of the prepared compounds exhibited good inhibition against the tested strains, and cyclohexylimidazole-derived 7-fluoroquinazolone 22a (MIC = 0.002 mmol/L) exhibited a 12.5-fold stronger inhibition than norfloxacin against Escherichia coli ATCC 25922. Further studies revealed that compound 22a not only possessed the ability of rapid bactericidal property and low propensity to develop resistance but also showed low cytotoxic effects toward red blood cells. The preliminary mechanism exploration indicated that compound 22a could cause membrane damage by disrupting bacterial membrane as well as depolarizing the cell membrane. Moreover, compound 22a could insert into DNA, which might hinder the replication of DNA. Molecular docking suggested that compound 22a could bind to gyrase and topoisomerase, which might be due to the suppressed expression of related genes. Meanwhile, compound 22a could disorder the metabolism and stimulate the production of reactive oxygen species to affect bacterial growth. The series of investigations suggested the promise of alkaloid quinazolone-derived imidazolenones as novel multitargeting antibacterial candidates for treatment of bacterial infections.

Comprehensive Summary

With the tactful material design, skillful device engineering, and in-depth understanding of morphology optimization, organic solar cells (OSCs) have achieved considerable success. Therefore, OSCs have reached high power conversion efficiencies (PCEs) exceeding 19%. Especially, continuously emerging new materials have been considered as one of the key factors to improve the PCEs of OSCs. Among molecular design strategies, side-chain engineering is an easy and commonly-used means which can optimize the solubility, alter intermolecular stacking arrangement, fine-tune the open circuit voltage (V _OC), thus ultimately improve the performance. As hybrid side chains, silane and siloxane side chains have considerable effects, not only in increasing the carrier mobility and tuning the energy level, but also in affecting the crystallinity and molecular orientation. In this review, the latest developments in photovoltaic materials based on silane and siloxane side chains are presented to illustrate the structure-property relationships. The review comprehensively includes silane-side based polymer/small molecule donors; siloxane-side based polymer/small molecule donors, and polymer/small molecule acceptors. Then the similarities and differences between these two side chains are demonstrated. Finally, the possible applications and future prospects of silane and siloxane side chains are presented.

Photo-modulation of gene-editing enzymes CRISPR/Cas9 has been achieved by a bifunctional small-molecule ligands strategy.

Comprehensive Summary

The control of protein functions with light is valuable for spatiotemporal probing of biological systems. Current small-molecule photo- modulation methods include the light-induced uncaging of inhibitors and chromophore-assisted light inactivation with reactive oxygen species (ROS). However, the constant target protein expression results in inadequate photo-modulation efficiency, particularly for less potent inhibitors and chromophores. Herein, we report a novel bifunctional small-molecule ligands strategy to photo-modulate gene-editing enzymes CRISPR/Cas9. A coumarin-derived small-molecule ligand Bhc-BRD0539 is developed to uncage the active inhibitor upon light irradiation and to generate ROS in the Cas9 proximity for the dual inhibition of Cas9 activity. Our results highlight the synergistic photo-modulation with bifunctional small-molecule ligands, which offers a valuable addition to current CRISPR/Cas9 photo-modulation technologies and may extend to other protein classes.

Comprehensive Summary

Since the discovery of the hydroformylation (oxo-synthesis or Roelen reaction) and the Reppe-reaction, the transition metal-catalyzed carbonylation reactions, providing versatile, facile, and even atom-economic methods for the selective incorporation of C=O functionality to various skeletons, have gained tremendous importance in synthetic organic chemistry from laboratories to industrial applications. The carbonylation of carbon-carbon multiple bonds, aromatic halides, triflates etc. in the presence of various nucleophiles has led the way to produce aldehydes, carboxylic acids, esters, amides, etc. in the fine chemical industry. However, these protocols usually proceed in conventional, fossil-based, and usually toxic reaction environments. Thus, several attempts have been directed to develop efficient carbonylation methods in alternative, less harmful, non-fossil-based and even in renewable reaction media. In this review, we overview the recent applications of alternative solvents such as water, biomass-based alcohols, γ-valerolactone (GVL), 2-methyltetrahydrofuran (2Me-THF), ionic liquids (ILs), deep eutectic solvents (DES), and alkyl levulinates, limonene, α-pinene, and dimethyl carbonate as well as fluorous media to improve efficiency, safety and environmentally benign nature of carbonylation protocols.

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Comprehensive Summary

Multi-substituted cyclohexanes play a crucial role as scaffolds in bioactive compounds. While significant progress has been made in synthesising substituted cyclohexanes, methods for the stereoselective assembly of 1,3-disubstituted cyclohexanes remain scarce. This study presents a novel approach involving nickel catalysis to achieve stereoselective carboboration of 1,4-cyclohexadiene. This innovative process allows for the simultaneous introduction of a boron group and an aryl or an alkyl fragment into the 1,4-cyclohexadiene framework under mild conditions, with exclusive regioselectivity and excellent cis configuration. The resulting products feature a double carbon bond and the incorporation of the boron group, offering significant potential for subsequent transformations and downstream applications.

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