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Promiscuity Guided Evolution of Decarboxylative Aldolases for Synthesis of Tertiary γ-Hydroxy Amino Acids.
Angew Chem Int Ed Engl
January 2025
University of Wisconsin Madison, Chemistry, 1101 University Ave, 53706, Madison, UNITED STATES OF AMERICA.
Many applications of enzymes benefit from activity on structurally diverse substrates. Here, we sought to engineer the decarboxylative aldolase UstD to perform a challenging C-C bond forming reaction with ketone electrophiles. The parent enzyme had only low levels of activity, portending multiple rounds of directed evolution and a possibility that mutations may inadvertently increase the specificity of the enzyme for a single model screening substrate.
View Article and Find Full Text PDFZn(TFSI)-Mediated Ring-Opening Polymerization for Electrolyte Engineering Toward Stable Aqueous Zinc Metal Batteries.
Nanomicro Lett
January 2025
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Fudan University, Shanghai, 200433, People's Republic of China.
Practical Zn metal batteries have been hindered by several challenges, including Zn dendrite growth, undesirable side reactions, and unstable electrode/electrolyte interface. These issues are particularly more serious in low-concentration electrolytes. Herein, we design a Zn salt-mediated electrolyte with in situ ring-opening polymerization of the small molecule organic solvent.
View Article and Find Full Text PDFKinetic and structural investigation of the 4-allyl syringol oxidase from Streptomyces cavernae.
Arch Biochem Biophys
January 2025
Microbial Biotechnology, Faculty of Biology and Biotechnology, Ruhr University Bochum, Universitaetsstrasse 150, 44780 Bochum, Germany.
4-Phenol oxidases are proposed to be involved in the utilization of lignin-derived aromatic compounds. While enzymes with selectivity towards 4-hydroxyphenyl and guaiacyl motifs are well described, we identified the first syringyl-specific oxidase from Streptomyces cavernae (Sc4ASO) only very recently. Here, in-depth studies were conducted to unravel the molecular origins of the outstanding selectivity of Sc4ASO.
View Article and Find Full Text PDFGold(I)-Catalyzed 2-Deoxy-β-glycosylation via 1,2-Alkyl/Arylthio Migration: Synthesis of Velutinoside A Pentasaccharide.
J Am Chem Soc
January 2025
Molecular Synthesis Center, Key Laboratory of Marine Drugs of Ministry of Education, Shandong Key Laboratory of Glycoscience and Glycotherapeutics, School of Medicine and Pharmacy, Ocean University of China, Qingdao 266003, China.
2-Deoxy-β-glycosides are essential components of natural products and pharmaceuticals; however, the corresponding 2-deoxy-β-glycosidic bonds are challenging to chemically construct. Herein, we describe an efficient catalytic protocol for synthesizing 2-deoxy-β-glycosides via either IPrAuNTf-catalyzed activation of a unique 1,2--positioned C2--propargyl xanthate (OSPX) leaving group or (PhO)PAuNTf-catalyzed activation of a 1,2--C2--alkynylbenzoate (OABz) substituent of the corresponding thioglycosides. These activation processes trigger 1,2-alkyl/arylthio-migration glycosylation, enabling the synthesis of structurally diverse 2-deoxy-β-glycosides under mild reaction conditions.
View Article and Find Full Text PDFChemical upcycling of polybutadiene into size controlled α,ω-dienes and diesters sequential hydrogenation and cross-metathesis.
Chem Sci
January 2025
Centre for Membrane Separations, Adsorption, Catalysis and Spectroscopy for Sustainable Solutions (cMACS), KU Leuven Celestijnenlaan 200F, Post Box 2454 3001 Leuven Belgium
Plastic waste conversion into valuable chemicals is a promising alternative to landfill or incineration. In particular, the chemical upcycling of polybutadiene rubber (PBR) could provide a renewable route towards highly desirable α,ω-dienes with varying chain lengths, which can find ample industrial application. While previous research has shown that the treatment of polybutadiene with a consecutive hydrogenation and ethenolysis reaction can afford long-chain α,ω-dienes, achieving precise control over the product chain length remains an important bottleneck.
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