Non-Heme Manganese Catalysts for On-Demand Production of Chlorine Dioxide in Water and Under Mild Conditions
- Authors
- Hicks, SD (Hicks, Scott D.); Kim, D (Kim, Doyeon); Xiong, SL (Xiong, Silei); Medyedey, GA (Medyedey, Grigor; Caruthers, J (Caruthers, James; Hong, S (Hong, Seungwoo); Abu-Omar, MM (Abu-Omar, Mandi; Nam, W (Nam, Wonwoo)
- Issue Date
- Mar-2014
- Publisher
- AMER CHEMICAL SOC
- Citation
- JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.136, no.9, pp 3680 - 3686
- Pages
- 7
- Journal Title
- JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
- Volume
- 136
- Number
- 9
- Start Page
- 3680
- End Page
- 3686
- URI
- https://scholarworks.sookmyung.ac.kr/handle/2020.sw.sookmyung/147338
- DOI
- 10.1021/ja5001642
- ISSN
- 0002-7863
1520-5126
- Abstract
- Two non-heme manganese complexes are used in the catalytic formation of chlorine dioxide from chlorite under ambient temperature at pH 5.00. The catalysts afford up to 1000 turnovers per hour and remain highly active in subsequent additions of chlorite. Kinetic and spectroscopic studies revealed a Mn-III(OH) species as the dominant form under catalytic conditions. A Mn-III(mu-O)Mn-IV dinuclear species was observed by EPR spectroscopy, supporting the involvement of a putative Mn-IV(O) species. First-order kinetic dependence on the manganese catalyst precludes the dinuclear species as the active form of the catalyst. Quantitative kinetic modeling enabled the deduction of a mechanism that accounts for all experimental observations. The chlorine dioxide producing cyde involves formation of a putative Mn-IV(O), which undergoes PCET (proton coupled electron-transfer) reaction with chlorite to afford chlorine dioxide. The ClO2 product can be efficiently removed from the aqueous reaction mixture via purging with an inert gas, allowing for the preparation of pure chlorine dioxide for on-site use and further production of chlorine dioxide.
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