Copper radical alcohol oxidases (CRO-AlcOx), which have been recently discovered among fungal phytopathogens, are attractive for the production of fragrant fatty aldehydes. With the initial objective to investigate the secretion of CRO-AlcOx by natural fungal strains, we undertook time course analyses of the secretomes of three Colletotrichum species (C. graminicola, C. tabacum, and C. destructivum) using proteomics. The addition of a copper-manganese-ethanol mixture in the absence of any plant-biomass mimicking compounds to Colletotrichum cultures unexpectedly induced the secretion of up to 400 proteins, 29 to 52% of which were carbohydrate-active enzymes (CAZymes), including a wide diversity of copper-containing oxidoreductases from the auxiliary activities (AA) class (AA1, AA3, AA5, AA7, AA9, AA11, AA12, AA13, and AA16). Under these specific conditions, while a CRO-glyoxal oxidase from the AA5_1 subfamily was among the most abundantly secreted proteins, the targeted AA5_2 CRO-AlcOx were secreted at lower levels, suggesting heterologous expression as a more promising strategy for CRO-AlcOx production and utilization. C. tabacum and C. destructivum CRO-AlcOx were thus expressed in Pichia pastoris, and their preference toward both aromatic and aliphatic primary alcohols was assessed. The CRO-AlcOx from C. destructivum was further investigated in applied settings, revealing a full conversion of C and C alcohols into their corresponding fragrant aldehydes. In the context of the industrial shift toward greener processes, the biocatalytic production of aldehydes is of utmost interest owing to their importance for their use as flavor and fragrance ingredients. Copper radical alcohol oxidases (CRO-AlcOx) have the potential to become platform enzymes for the oxidation of alcohols to aldehydes. However, the secretion of CRO-AlcOx by natural fungal strains has never been explored, while the use of crude fungal secretomes is an appealing approach for industrial applications to alleviate various costs pertaining to biocatalyst production. While investigating this primary objective, the secretomics studies revealed unexpected results showing that under the oxidative stress conditions we probed, Colletotrichum species can secrete a broad diversity of copper-containing enzymes (laccases, sugar oxidoreductases, and lytic polysaccharide monooxygenases [LPMOs]) usually assigned to "plant cell wall degradation," despite the absence of any plant-biomass mimicking compound. However, in these conditions, only small amounts of CRO-AlcOx were secreted, pointing out recombinant expression as the most promising path for their biocatalytic application.
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http://dx.doi.org/10.1128/AEM.01526-21 | DOI Listing |
Nanoscale
December 2024
School of Medical Technology and Engineering, Henan University of Science and Technology, Luoyang 71000, China.
Infectious bacteria pose an increasing threat to public health, and hospital-acquired bacterial infections remain a significant challenge for wound healing. In this study, we developed an advanced nanoplatform utilizing copper doped magnetic vortex nanoring coated with polydopamine (Cu-MVNp) based nanotherapeutics for bacterial infection tri-therapy. This multifunctional nanoplatform exhibits remarkable dual-stimulus thermogenic capabilities and Fenton-like peroxidase activity.
View Article and Find Full Text PDFEnviron Res
December 2024
School of Nuclear Science and Technology, University of South China, 421000, China.
The copper-based materials were considered as promising catalysts for the activation of peroxydisulfate (PDS), but the study on the CuS-activated PDS under LED illumination and alkaline condition was little reported. In this work, CuS, a simple and readily available heterogeneous catalyst, was employed to enhance the activation of PDS under alkaline condition through LED illumination. The results indicated that under LED illumination, the degradation rate of tetracycline (TC) during the first 15 min was 3.
View Article and Find Full Text PDFJ Am Chem Soc
December 2024
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
Adiponitrile (ADN) has wide applications, especially in the polymer industry. With the substantial and increasing global demand for ADN, effective production of ADN using safe and abundant starting materials is highly desirable but very challenging. Herein, we discovered that CuBr, combined with 1,10-phenanthroline (phen), could effectively promote the ammoxidation reaction of cyclohexanone to ADN with a yield of >99% using aqueous ammonia as the nitrogen source and O as the terminal oxidant under mild reaction conditions (80 °C, 5 atm O).
View Article and Find Full Text PDFBioact Mater
March 2025
Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.
Chemo-dynamic therapy (CDT) has a great potential in tumor extirpation. It entails producing hypertoxic reactive oxygen species (ROS) that damage the DNA of tumor cells and other biomacromolecules. However, the efficiency of CDT is severely hampered by the massive presence of glutathione (GSH) in tumor cells and the interference of ROS defense systems, such as Mutt homolog 1 (MTH1) protein sanitizes ROS-oxidized nucleotide pools.
View Article and Find Full Text PDFOrg Lett
December 2024
Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712, United States.
We disclose a broad platform for copper-catalyzed atom transfer radical addition (ATRA) of electron-deficient olefins. Catalytic Cu(dtbbpy)(OTf) enables radical addition of electron-deficient alkyl halides to acrylates, acrylamides, and vinyl sulfones in fair to excellent yields. The resultant ATRA products can be used in a variety of telescoped reactions, including substitution with basic amine nucleophiles to afford α-amino esters.
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