Generation of Reactive Oxygen Species and Degradation of Pollutants in the Fe2+/O2/Tripolyphosphate System : Regulated by the Concentration Ratio of Fe2+ and Tripolyphosphate
Tripolyphosphate (TPP) has many advantages as a ligand for the optimization of the Fe2+/O2 system in environmental remediation applications. However, the relationship between remediation performance and the Fe2+/TPP ratio in the system has not been previously described. In this study, we report that the degradation mechanism of p-nitrophenol (PNP) in Fe2+/O2 systems is regulated by the Fe2+/TPP ratio under neutral conditions. The results showed that although PNP was effectively degraded at different Fe2+/TPP ratios, the results of specific reactive oxygen species (ROS) scavenging experiments and the determination of PNP degradation products showed that the mechanism of PNP degradation varies with the Fe2+/TPP ratio. When CFe2+ ≥ CTPP, the initially formed O2•- is converted to •OH and the •OH degrades PNP by oxidation. However, when CFe2+ < CTPP, the O2•- persists long enough to degrade PNP by reduction. Density functional theory (DFT) calculations revealed that the main reactive species of Fe2+ in the system include [Fe(TPP)(H2O)3]- and [Fe(TPP)2]4-, whose content in the solution is the key to achieve system regulation. Consequently, by controlling the Fe2+/TPP ratio in the solution, the degradation pathways of PNP can be selected. Our study proposed a new strategy to regulate the oxidation/reduction removal of pollutants by simply varying the Fe2+/TPP ratio of the Fe2+/O2 system.
| Medienart: |
E-Artikel |
|---|
| Erscheinungsjahr: |
2022 |
|---|---|
| Erschienen: |
2022 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:56 |
|---|---|
| Enthalten in: |
Environmental science & technology - 56(2022), 7 vom: 05. Apr., Seite 4367-4376 |
| Sprache: |
Englisch |
|---|
| Beteiligte Personen: |
Zhang, Chengwu [VerfasserIn] |
|---|
| Links: |
|---|
| Anmerkungen: |
Date Completed 06.04.2022 Date Revised 16.06.2022 published: Print-Electronic Citation Status MEDLINE |
|---|
| doi: |
10.1021/acs.est.1c07467 |
|---|
| funding: |
|
|---|---|
| Förderinstitution / Projekttitel: |
|
| PPN (Katalog-ID): |
NLM338064451 |
|---|
| LEADER | 01000naa a22002652 4500 | ||
|---|---|---|---|
| 001 | NLM338064451 | ||
| 003 | DE-627 | ||
| 005 | 20231225235828.0 | ||
| 007 | cr uuu---uuuuu | ||
| 008 | 231225s2022 xx |||||o 00| ||eng c | ||
| 024 | 7 | |a 10.1021/acs.est.1c07467 |2 doi | |
| 028 | 5 | 2 | |a pubmed24n1126.xml |
| 035 | |a (DE-627)NLM338064451 | ||
| 035 | |a (NLM)35275631 | ||
| 040 | |a DE-627 |b ger |c DE-627 |e rakwb | ||
| 041 | |a eng | ||
| 100 | 1 | |a Zhang, Chengwu |e verfasserin |4 aut | |
| 245 | 1 | 0 | |a Generation of Reactive Oxygen Species and Degradation of Pollutants in the Fe2+/O2/Tripolyphosphate System |b Regulated by the Concentration Ratio of Fe2+ and Tripolyphosphate |
| 264 | 1 | |c 2022 | |
| 336 | |a Text |b txt |2 rdacontent | ||
| 337 | |a ƒaComputermedien |b c |2 rdamedia | ||
| 338 | |a ƒa Online-Ressource |b cr |2 rdacarrier | ||
| 500 | |a Date Completed 06.04.2022 | ||
| 500 | |a Date Revised 16.06.2022 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status MEDLINE | ||
| 520 | |a Tripolyphosphate (TPP) has many advantages as a ligand for the optimization of the Fe2+/O2 system in environmental remediation applications. However, the relationship between remediation performance and the Fe2+/TPP ratio in the system has not been previously described. In this study, we report that the degradation mechanism of p-nitrophenol (PNP) in Fe2+/O2 systems is regulated by the Fe2+/TPP ratio under neutral conditions. The results showed that although PNP was effectively degraded at different Fe2+/TPP ratios, the results of specific reactive oxygen species (ROS) scavenging experiments and the determination of PNP degradation products showed that the mechanism of PNP degradation varies with the Fe2+/TPP ratio. When CFe2+ ≥ CTPP, the initially formed O2•- is converted to •OH and the •OH degrades PNP by oxidation. However, when CFe2+ < CTPP, the O2•- persists long enough to degrade PNP by reduction. Density functional theory (DFT) calculations revealed that the main reactive species of Fe2+ in the system include [Fe(TPP)(H2O)3]- and [Fe(TPP)2]4-, whose content in the solution is the key to achieve system regulation. Consequently, by controlling the Fe2+/TPP ratio in the solution, the degradation pathways of PNP can be selected. Our study proposed a new strategy to regulate the oxidation/reduction removal of pollutants by simply varying the Fe2+/TPP ratio of the Fe2+/O2 system | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a Research Support, Non-U.S. Gov't | |
| 650 | 4 | |a concentration regulation | |
| 650 | 4 | |a ferrous-polyphosphate complex | |
| 650 | 4 | |a molecular oxygen activation | |
| 650 | 4 | |a oxidation/reduction | |
| 650 | 7 | |a Environmental Pollutants |2 NLM | |
| 650 | 7 | |a Polyphosphates |2 NLM | |
| 650 | 7 | |a Reactive Oxygen Species |2 NLM | |
| 650 | 7 | |a Water Pollutants, Chemical |2 NLM | |
| 650 | 7 | |a Hydrogen Peroxide |2 NLM | |
| 650 | 7 | |a BBX060AN9V |2 NLM | |
| 650 | 7 | |a Iron |2 NLM | |
| 650 | 7 | |a E1UOL152H7 |2 NLM | |
| 650 | 7 | |a triphosphoric acid |2 NLM | |
| 650 | 7 | |a NU43IAG5BC |2 NLM | |
| 650 | 7 | |a Oxygen |2 NLM | |
| 650 | 7 | |a S88TT14065 |2 NLM | |
| 700 | 1 | |a Kong, Chuipeng |e verfasserin |4 aut | |
| 700 | 1 | |a Tratnyek, Paul G |e verfasserin |4 aut | |
| 700 | 1 | |a Qin, Chuanyu |e verfasserin |4 aut | |
| 773 | 0 | 8 | |i Enthalten in |t Environmental science & technology |d 1967 |g 56(2022), 7 vom: 05. Apr., Seite 4367-4376 |w (DE-627)NLM112374735 |x 1520-5851 |7 nnns |
| 773 | 1 | 8 | |g volume:56 |g year:2022 |g number:7 |g day:05 |g month:04 |g pages:4367-4376 |
| 856 | 4 | 0 | |u http://dx.doi.org/10.1021/acs.est.1c07467 |3 Volltext |
| 912 | |a GBV_USEFLAG_A | ||
| 912 | |a GBV_NLM | ||
| 951 | |a AR | ||
| 952 | |d 56 |j 2022 |e 7 |b 05 |c 04 |h 4367-4376 | ||