Latest ArticlesThe biosecurity hazards caused by pathogenic fungus have been widely concerned. Given the long-term coexistence of eukaryotic pathogens and quorum sensing bacteria in different habitats in environments, we hypothesized that they have social interactions via signal molecules. In this work, we firstly discovered the well-known bacterial signal molecules play an adverse role in the cell morphology and metabolism in a model pathogen Trichosporon asahii. N-Tetradecanoyl-L-homoserine lactone (C14-HSL) was discovered to increase pathogen hazards of T. asahii, which limited mycelium by 52%, but enhanced cell aggregation by 93%. Higher fluorescence intensity of tryptophan (59%) and aromatic protein (2-fold) contents after the treatment of C14-HSL, indicating that aromatic proteins helped aggregate Trichosporon and showed hydrophobicity. Transcriptome analysis revealed that C14-HSL upregulated the shikimate pathway (above 1-fold) located in downstream of tricarboxylic acid cycle, which contributed to the synthesis of more aromatic proteins and the formation of larger flocs. The limited mycelial growth of T. asahii attributed to the up-regulated expressions of cell cycle process. The fungal transboundary response to bacterial C14-HSL was controlled by signal transduction pathways. This study provides new insights into the co-evolution of bacterial and pathogenic fungi in microecosystems.
Glycosyl radicals, produced under mild photoredox conditions, show unique utility in the preparation of C-linked glycoconjugates. We herein report the construction of C-glycosidic bonds on α,β-dehydroalanine (DHA) of peptides with easily available glycosyl bromides as glycosyl radical precursors under highly anomeric control, leading to C-glycosylation modifications of peptides. This method not only has outstanding functional group compatibility, but also is feasible in near-physiological conditions (pH ~ 7 and temperature T ≤ 37 ℃ in aqueous media).
Detection and observation of reactive intermediates is an essential step in investigation of reaction pathways. However, most reactive intermediates are unstable and present at low concentrations; their short lifetimes make them difficult to detect and characterize. Supramolecular containers offer opportunities for the stabilization and characterization of those labile species, through isolation from the media and protection inside the cavity of the host. In this review, we summarize the examples of labile reaction intermediates that are stabilized and characterized with the help of supramolecular containers. The container compounds include carcerands, deep cavitands and amide naphthotubes. We focus on unstable guest species – cyclobutadiene, benzocyclopropenone, o-benzyne, 1,2,4,6-cycloheptatetraene, anti-Bredt's olefin, fluorophenoxycarbene, O-acylisoamide, and hemiaminal – that act as intermediates in certain organic reactions
Closed pores formed in hard carbons play an essential role in sodium storage at plateau region. However, the effect of different structural features on the diffusion of sodium ions into closed pores remains unclear. Herein, a precursor reconstruction strategy is conducted to regulate carbon microstructures including interlayer spacing, defect concentration, and closed pore volume by changing the ratio of aromatic and polysaccharide components. Aromatic structure parts tend to develop disordered carbons with fewer defects, larger interlayer spacing, and smaller closed pore volume, while polysaccharide components prefer to form disordered carbons with more defects, smaller interlayer spacing, and larger closed pore volume. Through the correlation analysis of microstructure features and the sodium storage capacity below 0.1 V. It finds that the intercalation capacity is proportional to the ratio of pseudo-graphitic domains, whereas the pore filling capacity appeared at lower potential gradually decreases with the increasing defect concentration due to homo-ionic repulsion effect, without linear correlation with short-range microcrystalline and closed pore volume. The optimized sample with suitable interlayer spacing and defect concentration exhibits a high plateau capacity of 241.7 mAh/g. This work provides insights into the exploitation of closed pore sodium storage performance.
In some industrial wastewater, heavy metals combine with organic complexing agents to form heavy metal complexes (HMCs). These HMCs can be difficult to decompose and remove through conventional techniques due to their higher stability than free heavy metal ions. In recent years, persulfate based advanced oxidation processes (PS-based AOPs) have been recognized as a viable technique for HMCs degradation. Nevertheless, a comprehensive and in-depth understanding of the relevant HMCs decomplexation mechanisms in PS-based AOPs is still lacking. This review delineates the current progress of HMCs decomplexation in PS-based AOPs. We discuss the distinctions between the two widely used oxidant types in PS-based AOPs techniques. Moreover, we summarize and highlight the decomplexation mechanisms based on electron and energy transfer, and degradation pathways of HMCs. We also emphasize the effects of environmental water constituents, namely pH, inorganic ions, and natural organic matter (NOM), on HMCs decomplexation. Ultimately, we identify the existing challenges and perspectives that will steer the direction of advancing PS-based AOPs to remove HMCs.
An amphiphilic derivative with a large Stokes shift by introducing flexible hydrophilic long chains into a rigid ethylene-pyrene compound have been successfully synthesized. The alkylated compound exhibited a notable change in charge distribution, facilitating cation-π interactions. Through the process of amphiphilic self-assembly, the formation of highly ordered aggregates enabled effective photo-dimerization under 449 nm LED irradiation. Notably, this photo-responsive technology not only exhibited advanced multi-color emission effects, including white light emission but also exhibited environmentally friendly behavior in the aqueous phase.
To promote the practices of perovskite photovoltaics, it requires to develop efficient perovskite solar cells (PVSCs) standing long-time operation under the adverse environments. Herein, we demonstrate that the tailor-made conjugated polymers as conductive adhesives stabilized the originally redox-reactive heterointerface between perovskite and metal oxide, facilitating the access of efficient and stable inverted PVSCs. It was revealed that bithiophene and phenyl alternating conjugated polymers with partial glycol chains atop of the metal oxide layer has resulted in effective organic-inorganic hybrid hole transporting bilayers, which allow maintaining efficient hole extraction and transport, meanwhile preventing halide migration to directly contact with the nickel oxide (NiOx) layer. As a result, the corresponding inverted PVSCs with the organic-inorganic hole transporting bilayers have achieved an excellent power conversion efficiency of 23.22%, outperforming 20.65% of bare NiOx-based devices. Moreover, the encapsulated PVSCs with organic-inorganic bilayers exhibited the excellent photostability with 91% of the initial efficiency after 1000-h one-sun equivalent illumination in ambient conditions. Overall, this work provides new insights into stabilizing the vulnerable heterointerface for perovskite solar cells.
Development of hydrothermally stable, low-temperature catalysts for controlling nitrogen oxides emissions from mobile sources remains an urgent challenge. We have prepared a metal oxide-zeolite composite catalyst by depositing Mn active species on a mixture support of CeO2/Al2O3 and ZSM-5. This composite catalyst is hydrothermally stable and shows improved low-temperature SCR activity and significantly reduced N2O formation than the corresponding metal oxide catalyst. Comparing with a Cu-CHA catalyst, the composite catalyst has a faster response to NH3 injection and less NH3 slip. Our characterization results reveal that such an oxide-zeolite composite catalyst contains more acidic sites and Mn3+ species as a result of oxide-zeolite interaction, and this interaction leads to the generation of more NH4+ species bound to the Brønsted acid sites and more reactive NOx species absorbed on the Mn sites. Herein, we report our mechanistic understanding of the oxide-zeolite composite catalyst and its molecular pathway for improving the low-temperature activity and N2 selectivity for NH3-SCR reaction. Practically, this work may provide an alternative methodology for low-temperature NOx control from diesel vehicles.
Single-chain nanoparticles represent an emerging class of nanomaterials designed to mimic protein's folding paradigm. Intrachain covalent crosslinking toward the formation of single-chain nanoparticles encounters complex energy landscapes, leading to the potential occurrence of misfolding issues. While non-covalent crosslinking can circumvent this issue, the resulting single-chain nanoparticles exhibit lower structural stability compared to their covalently crosslinked counterparts. In this study, we present a novel approach for the synthesis of single-chain nanoparticles, achieved through the combination of non-covalent and covalent intramolecular crosslinking. Cyanostilbenes grafted onto the linear polymer form intrachain non-covalent stacks aided by hydrogen bonds, leading to the formation of non-covalently crosslinked single-chain nanoparticles. These nanoparticles undergo conversion to covalently crosslinked nanostructures through subsequent photo-irradiation using [2 + 2] photocycloaddition, a process facilitated by the supramolecular confinement effect. Consequently, the resulting single-chain nanoparticles demonstrate both intrachain folding efficiency and substantial stability, offering significant potential for advancing applications across diverse fields.
Electrochemical sensing provides a powerful technological means for the therapeutic drug monitoring of drug-resistant tuberculosis but requires a functionalized electrode to capture the analytes and catalyze their redox reactions. Herein, we construct a nickel–tannic acid supramolecular network (Ni–TA) on the surface of electrospun-derived C–CeO2 nanofiber for the sensitive and simultaneous detection of isoniazid (INZ) and hydrazine (HYD). Mechanistic investigations demonstrate that Ni–TA is electronegative and hydrophilic, thus facilitating an efficient mass and electron transfer. Ni–TA/C–CeO2 has higher adsorption rate constants (0.091 g mg–1 h–1 for INZ, and 0.062 g mg–1 h–1 for HYD) than native C–CeO2 (0.075 g mg–1 h–1 for INZ, and 0.047 g mg–1 h–1 for HYD). Moreover, Ni–TA/C–CeO2 (56 Ω) has lower charge transfer resistances than C–CeO2 (417 Ω). Ni–TA/C–CeO2 performs low detection limits and wide linearity ranges for INZ (0.012 µmol/L and 0.1–400 µmol/L, respectively) and HYD (0.008 µmol/L and 0.015–1420 µmol/L, respectively), coupled with high selectivity, cycle stability and reproducibility. This research demonstrated the promising applications of Ni–TA/C–CeO2 by analyzing human-collected plasma and urine samples.
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