期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY LETTERS
卷 6, 期 12, 页码 781-786出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.estlett.9b00682
关键词
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资金
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDA23010400]
- National Natural Science Foundation of China [21876049]
- U.S. National Institute for Environmental Health Sciences Superfund Research Program (NIEHS) at the University of California, Berkeley [P42 ES004705]
- US/China Clean Energy Research Center for Water-Energy Technologies
- International Postdoctoral Exchange Fellowship Program of China [20150074]
Under the conditions employed when in situ chemical oxidation is used for contaminant remediation, high concentrations of H2O2 (e.g., up to similar to 10 M) are typically present. Using C-13 NMR, we show that in carbonate-rich systems, these high concentrations of H2O2 result in a reaction with HCO3- to produce peroxymonocarbonate (HCO4-). After formation, HCO4- reacts with phenol to produce di- and trihydroxyl phenols. HCO4- reacts with substituted phenols in a manner consistent with its electrophilic character. Exchanging an electron-donating substituent in the para position of a phenolic compound with an electron-withdrawing group decreased the reaction rate. Results of this study indicate that HCO4- is a potentially important but previously unrecognized oxidative species generated during H2O2 in situ chemical oxidation that selectively reacts with electron-rich organic compounds. Under conditions in which HO center dot formation is inefficient (e.g., relatively high concentration of HCO3-, low total Fe and Mn concentrations), the fraction of the phenolic compounds that is transformed by HCO4- could be similar to or greater than the fraction transformed by HO center dot. It may be possible to adjust treatment conditions to enhance the formation of HCO4- as a means of accelerating rates of contaminant removal.
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