Abstract:
:Direct charge transfer (DCT) and •OH attack played important roles in contaminant degradation by BDD electrochemical oxidation. Their separate contributions and potential bond-cleavage processes were required but lacking. Here, we carried out promising compound-specific isotope fractionation analysis (CSIA) to explore 13C and 2H isotope fractionation of atrazine (ATZ), followed by assessing the reaction pathway by BDD anode. The correlation of 2H and 13C fractionation allows to remarkably differentiate DCT process and •OH attack, with Λ values of 18.99 and 53.60, respectively. Radical quenching identified that •OH accounted for 79.0%-88.5% in the whole reaction. While CSIA methods provided biased results, which suggested that ATZ degradation exhibited two stages with •OH contributions of 24.6% and 84.3% respectively, confirming CSIA was more sensitive and provided more possibilities to estimate degradation processes. Combined with Fukui index and intermediate products identification, we deduced that dechlorination-hydroxylation mainly occurred in the first 30 min by DCT reaction. While lateral chain oxidation with C-N broken was the governing route once •OH was largely generated, with the production of DEA (m/z 188), DIA (m/z 174), DEIA (m/z 146) and DEIHA (m/z 128). Our results demonstrated that isotope fractionation can offer "isotopic footprints" for identifying the rate-limiting steps and bond breakage process, and opens new avenues for degradation pathways of contaminants.
journal_name
Chemospherejournal_title
Chemosphereauthors
Wang T,Huang T,Jiang H,Ma Rdoi
10.1016/j.chemosphere.2021.129754subject
Has Abstractpub_date
2021-01-22 00:00:00pages
129754eissn
0045-6535issn
1879-1298pii
S0045-6535(21)00223-Xjournal_volume
273pub_type
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