Desulfurization of organosulfur substrates is highly important due to its relation with the industrial hydrodesulfurization (HDS) process of fossil fuels, which helps to eliminate the sulfur-containing impurities such as thiols, sulfide, thiophenes, etc. from crude oil for the production of easily processed and more cleanly combusted fuel with very low sulfur content. While the HDS process involves a hydrogenolysis reaction under a high pressure of hydrogen gas at high temperature, the hydrolysis of C-S bonds of organosulfur substrates at ambient conditions may very well be considered as a potential alternative for model desulfurization reactions. However, unlike the availability of an appreciable number of reports on base, acid, and metal ion mediated hydrolysis of thioesters in the literature, reports on the hydrolysis of more difficult substrates such as thiolates, sulfides, and other organosulfur substrates remained unavailable until 2017. The very recent discovery of a transition metal mediated hydrolysis reaction of C-S bonds at ambient conditions, however, has rapidly filled in this gap within the past few years. Development of this new stoichiometric reaction allowed the desulfurization of a large number of organosulfur substrates, including aliphatic and aromatic thiols, thiocarboxylic acids, sulfides, disulfides, thiophenes, and dibenzothiophene, at ambient conditions and was subsequently converted to a catalytic process for the hydrolysis of thiols. A brief overview of this new reaction strategy, a proposed reaction mechanism, a critical analysis of the efficiency, and future prospects are presented.
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http://dx.doi.org/10.1021/acsorginorgau.3c00038 | DOI Listing |
Biochem J
January 2025
School of Chemistry and Bio21 Molecular Science and Biotechnology Institute, University of Melbourne, Parkville, Victoria 3010, Australia.
The sulfosugar sulfoquinovose (SQ) is catabolized through the sulfoglycolytic Entner-Doudoroff pathway, beginning with the oxidation of SQ to sulfogluconolactone by SQ dehydrogenase. We present a comprehensive structural and kinetic characterization of Pseudomonas putida SQ dehydrogenase (PpSQDH). PpSQDH is a tetrameric enzyme belonging to the short-chain dehydrogenase/reductase (SDR) superfamily with a strong preference for NAD+ over NADP+.
View Article and Find Full Text PDFNat Commun
November 2024
Bioland Laboratory, Guangzhou, China.
α-Functionalized Si-, Ge-, B-, Se-, and S-amide moieties are present in many medicinally active molecules, but their synthesis remains challenging. Here, we demonstrate a high-throughput synthesis using amide-sulfoxonium ylides as carbene precursors in a Si-H, Ge-H, B-H, Se-H, and S-H insertion reactions to target a wide range of α-silyl, α-geryl, α-boryl, α-selenyl, and α-sulfur (hetero)amides. The process is featured as simple operation, mild conditions, broad substrate scope, high functional group compatibility, and excellent chemoselectivity.
View Article and Find Full Text PDFChembiochem
December 2024
College of Food Science and Engineering, Jiangxi Agricultural University, Nanchang, 330045, China.
Sulfide:Quinone Oxidoreductase (Sqr) Catalyzes The Initial Procedure On Sulfide Transformation, Alongside Sulfide (HS, S) Oxidization Coupled With Coenzyme Q (CoQ) Reducing And Reactive Sulfur Species (RSS) Production. Here, We Assessed The Reactivity Of Propanethiol (PT) As An Alternative Substrate For Sqr To Maintain Intracellular Homeostasis In Strain S-1 Capable Of Degrading Emerging Sulfur-Containing Pollutants. We Deleted A Gene Encoding Sqr, And Serial Transcriptional Difference Induced By RSS Dynamics Was Therefore Revealed.
View Article and Find Full Text PDFOrg Lett
September 2024
College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, P. R. China.
Stable and easy-to-handle sodium salts of sulfonyl oximes were first identified to proceed via visible-light-driven phophine-mediated successive deoxygenation to realize the -Markovnikov hydrothiolation of alkenes, which could serve as an odorless sulfur source. Mechanistic studies revealed that the key thiyl radical intermediate could be generated from the sulfonyl oxime anion via a phosphine-mediated fragmentation and a sequential deoxygenation process. Notably, a wide range of alkenes, including acrylamides, acrylates, vinyl ketones, vinyl sulfones, and acrylonitriles, are competent substrates for this protocol, which is highly beneficial for the construction of structurally diversified organosulfur compounds.
View Article and Find Full Text PDFChem Sci
September 2024
School of Chemistry, Bio21 Molecular Science and Biotechnology Institute, University of Melbourne Parkville Victoria 3010 Australia
2,3-Dihydroxypropanesulfonate (DHPS) and sulfolactate (SL) are environmentally important organosulfur compounds that play key roles as metabolic currencies in the sulfur cycle. Despite their prevalence, the pathways governing DHPS and SL production remain poorly understood. Here, we study DHPS-3-dehydrogenase from (HpsN), a bacterium capable of utilizing DHPS as a sole carbon source.
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