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Integrating hydrogen production with anodic selective oxidation of sulfides over a CoFe layered double hydroxide electrode.

ABSTRACT: Replacing the sluggish oxygen evolution reaction (OER) with oxidation reactions for the synthesis of complex pharmaceutical molecules coupled with enhanced hydrogen evolution reaction (HER) is highly attractive, but it is rarely explored. Here, we report an electrochemical protocol for selective oxidation of sulfides to sulfoxides over a CoFe layered double hydroxide (CoFe-LDH) anode in an aqueous-MeCN electrolyte, coupled with 2-fold promoted cathodic H₂ productivity. This protocol displays high activity (85-96% yields), catalyst stability (10 cycles), and generality (12 examples) in selective sulfide oxidation. We demonstrate its applicability in the synthesis of four important pharmaceutical related sulfoxide compounds with scalability (up to 1.79 g). X-ray spectroscopy investigations reveal that the CoFe-LDH material evolved into amorphous CoFe-oxyhydroxide under catalytic conditions. This work may pave the way towards sustainable organic synthesis of valuable pharmaceuticals coupled with H₂ production.

SUBMITTER: Ma L

PROVIDER: S-EPMC8179046 | biostudies-literature | 2020 Nov

REPOSITORIES: biostudies-literature

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Integrating hydrogen production with anodic selective oxidation of sulfides over a CoFe layered double hydroxide electrode.

Ma Lina L Zhou Hua H Xu Ming M Hao Peipei P Kong Xianggui X Duan Haohong H

Chemical science 20201111 3

Replacing the sluggish oxygen evolution reaction (OER) with oxidation reactions for the synthesis of complex pharmaceutical molecules coupled with enhanced hydrogen evolution reaction (HER) is highly attractive, but it is rarely explored. Here, we report an electrochemical protocol for selective oxidation of sulfides to sulfoxides over a CoFe layered double hydroxide (CoFe-LDH) anode in an aqueous-MeCN electrolyte, coupled with 2-fold promoted cathodic H<sub>2</sub> productivity. This protocol d ...[more]

PMID: 34163860

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Project description:Environmental pollution resulting from the use of pesticides such as fenuron poses significant health risks due to the carcinogenic and teratogenic properties of these compounds. There is an urgent need to develop rapid and cost-effective detection methods for quantifying fenuron. In this study, an inorganic-organic composite material was obtained by intercalating sodium dioctylsulfosuccinate (DSS) within the interlayer space of a nickel-aluminum-layered double hydroxide (NiAl-LDH). The pristine and modified LDHs (NiAl-LDH) were characterized using Fourier transform infrared, X-ray diffraction, and thermogravimetric analysis, confirming the successful intercalation of DSS in the mineral structure. The modified LDH was used to elaborate a sensor for detecting fenuron herbicide via differential pulse voltammetry (DPV) employing a carbon paste electrode (CPE). The electrochemical procedure for fenuron analysis consisted of immersing the working electrode in an electrolytic solution containing the appropriate amount of fenuron, followed by voltammetry detection without any preconcentration step. Compared to CPE modified by pristine LDH, the peak current obtained on the organo-LDH-modified CPE was twice as high. The increase in the fenuron signal was attributed to the high organophilic feature of this composite material induced by DSS modification. To optimize the sensitivity of the organo-LDH modified electrode, the effects of several experimental parameters such as pH of the medium and proportion of the modifier in the paste on the stripping response were examined. Linear calibration curves were obtained for the fenuron concentrations ranging from 0.5 × 10-6 to 1 × 10-6 mol.L-1 and 1 × 10-6 to 5 × 10-6 mol.L-1. The limit of detection (LOD) calculated on the basis of a signal-to-noise ratio of 3 was found to be 1.8 × 10-8 mol.L-1 for the low concentration range with a limit of quantification (LOQ) which was 6 × 10-8 mol.L-1. Furthermore, the interference effect of several inorganic ions and other pesticides potentially affecting fenuron stripping was explored, and the method's applicability was confirmed by determining fenuron levels in a river sample taken from down-town Yaoundé.

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Integrating hydrogen production with anodic selective oxidation of sulfides over a CoFe layered double hydroxide electrode.

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Integrating hydrogen production with anodic selective oxidation of sulfides over a CoFe layered double hydroxide electrode.

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