Manganese doped iron–carbon composite for synergistic persulfate activation: Reactivity, stability, and mechanism
The heterogeneous catalytic process has been under development for aqueous pollutant degradation, yet electron transfer efficiency often limits the effectiveness of catalytic reactions. In this study, a novel composite material, manganese doped iron–carbon (Mn–Fe–C), was tailor designed to promote t...
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| Published in | Journal of hazardous materials Vol. 405; p. 124228 |
|---|---|
| Main Authors | , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Netherlands
Elsevier B.V
05.03.2021
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| Subjects | |
| Online Access | Get full text |
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| Abstract | The heterogeneous catalytic process has been under development for aqueous pollutant degradation, yet electron transfer efficiency often limits the effectiveness of catalytic reactions. In this study, a novel composite material, manganese doped iron–carbon (Mn–Fe–C), was tailor designed to promote the catalytic electron transfer. The Mn–Fe–C composite, synthesized via a facile carbothermal reduction method, was characterized and evaluated for its performance to activate persulfate (PS) and degrade Rhodamine Blue (RhB) dye under different pH, catalyst dosages, PS dosages, and pollutant concentrations. Electron spin resonance, along with quenching results by ethanol, tert-butanol, phenol, nitrobenzene and benzoquinone, indicated that surface bounded SO4•− was the main contributor for RhB degradation, while the roles of aqueous SO4•− and •OH were very minor. Through characterization by XRD, XPS and FTIR analysis, it was determined that the electron transfer during activation of PS was accelerated by the oxygen functional groups on catalyst surface and the promoted redox cycle of Fe3+ and Fe2+ by Mn. Finally, the Mn–Fe–C composite catalyst exhibited an excellent reusability and stability with negligible leached Fe and Mn ions in solutions. Results of this study provide a promising design for heterogeneous catalysts that can effectively activate PS to remove organic pollutants from water at circumneutral pH conditions.
[Display omitted]
•Mn–Fe–C composite was tailor-designed to promote catalytic electron transfer.•Oxygen functional groups on catalyst promoted PS activation and RhB degradation.•Redox cycle of Fe3+ and Fe2+ was accelerated by Mn for electron transfer.•The Mn–Fe–C composite exhibited excellent stability and reusability. |
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| AbstractList | The heterogeneous catalytic process has been under development for aqueous pollutant degradation, yet electron transfer efficiency often limits the effectiveness of catalytic reactions. In this study, a novel composite material, manganese doped iron-carbon (Mn-Fe-C), was tailor designed to promote the catalytic electron transfer. The Mn-Fe-C composite, synthesized via a facile carbothermal reduction method, was characterized and evaluated for its performance to activate persulfate (PS) and degrade Rhodamine Blue (RhB) dye under different pH, catalyst dosages, PS dosages, and pollutant concentrations. Electron spin resonance, along with quenching results by ethanol, tert-butanol, phenol, nitrobenzene and benzoquinone, indicated that surface bounded SO
was the main contributor for RhB degradation, while the roles of aqueous SO
and
OH were very minor. Through characterization by XRD, XPS and FTIR analysis, it was determined that the electron transfer during activation of PS was accelerated by the oxygen functional groups on catalyst surface and the promoted redox cycle of Fe
and Fe
by Mn. Finally, the Mn-Fe-C composite catalyst exhibited an excellent reusability and stability with negligible leached Fe and Mn ions in solutions. Results of this study provide a promising design for heterogeneous catalysts that can effectively activate PS to remove organic pollutants from water at circumneutral pH conditions. The heterogeneous catalytic process has been under development for aqueous pollutant degradation, yet electron transfer efficiency often limits the effectiveness of catalytic reactions. In this study, a novel composite material, manganese doped iron-carbon (Mn-Fe-C), was tailor designed to promote the catalytic electron transfer. The Mn-Fe-C composite, synthesized via a facile carbothermal reduction method, was characterized and evaluated for its performance to activate persulfate (PS) and degrade Rhodamine Blue (RhB) dye under different pH, catalyst dosages, PS dosages, and pollutant concentrations. Electron spin resonance, along with quenching results by ethanol, tert-butanol, phenol, nitrobenzene and benzoquinone, indicated that surface bounded SO4•- was the main contributor for RhB degradation, while the roles of aqueous SO4•- and •OH were very minor. Through characterization by XRD, XPS and FTIR analysis, it was determined that the electron transfer during activation of PS was accelerated by the oxygen functional groups on catalyst surface and the promoted redox cycle of Fe3+ and Fe2+ by Mn. Finally, the Mn-Fe-C composite catalyst exhibited an excellent reusability and stability with negligible leached Fe and Mn ions in solutions. Results of this study provide a promising design for heterogeneous catalysts that can effectively activate PS to remove organic pollutants from water at circumneutral pH conditions.The heterogeneous catalytic process has been under development for aqueous pollutant degradation, yet electron transfer efficiency often limits the effectiveness of catalytic reactions. In this study, a novel composite material, manganese doped iron-carbon (Mn-Fe-C), was tailor designed to promote the catalytic electron transfer. The Mn-Fe-C composite, synthesized via a facile carbothermal reduction method, was characterized and evaluated for its performance to activate persulfate (PS) and degrade Rhodamine Blue (RhB) dye under different pH, catalyst dosages, PS dosages, and pollutant concentrations. Electron spin resonance, along with quenching results by ethanol, tert-butanol, phenol, nitrobenzene and benzoquinone, indicated that surface bounded SO4•- was the main contributor for RhB degradation, while the roles of aqueous SO4•- and •OH were very minor. Through characterization by XRD, XPS and FTIR analysis, it was determined that the electron transfer during activation of PS was accelerated by the oxygen functional groups on catalyst surface and the promoted redox cycle of Fe3+ and Fe2+ by Mn. Finally, the Mn-Fe-C composite catalyst exhibited an excellent reusability and stability with negligible leached Fe and Mn ions in solutions. Results of this study provide a promising design for heterogeneous catalysts that can effectively activate PS to remove organic pollutants from water at circumneutral pH conditions. The heterogeneous catalytic process has been under development for aqueous pollutant degradation, yet electron transfer efficiency often limits the effectiveness of catalytic reactions. In this study, a novel composite material, manganese doped iron-carbon (Mn-Fe-C), was tailor designed to promote the catalytic electron transfer. The Mn-Fe-C composite, synthesized via a facile carbothermal reduction method, was characterized and evaluated for its performance to activate persulfate (PS) and degrade Rhodamine Blue (RhB) dye under different pH, catalyst dosages, PS dosages, and pollutant concentrations. Electron spin resonance, along with quenching results by ethanol, tert-butanol, phenol, nitrobenzene and benzoquinone, indicated that surface bounded SO₄•⁻ was the main contributor for RhB degradation, while the roles of aqueous SO₄•⁻ and •OH were very minor. Through characterization by XRD, XPS and FTIR analysis, it was determined that the electron transfer during activation of PS was accelerated by the oxygen functional groups on catalyst surface and the promoted redox cycle of Fe³⁺ and Fe²⁺ by Mn. Finally, the Mn-Fe-C composite catalyst exhibited an excellent reusability and stability with negligible leached Fe and Mn ions in solutions. Results of this study provide a promising design for heterogeneous catalysts that can effectively activate PS to remove organic pollutants from water at circumneutral pH conditions. The heterogeneous catalytic process has been under development for aqueous pollutant degradation, yet electron transfer efficiency often limits the effectiveness of catalytic reactions. In this study, a novel composite material, manganese doped iron–carbon (Mn–Fe–C), was tailor designed to promote the catalytic electron transfer. The Mn–Fe–C composite, synthesized via a facile carbothermal reduction method, was characterized and evaluated for its performance to activate persulfate (PS) and degrade Rhodamine Blue (RhB) dye under different pH, catalyst dosages, PS dosages, and pollutant concentrations. Electron spin resonance, along with quenching results by ethanol, tert-butanol, phenol, nitrobenzene and benzoquinone, indicated that surface bounded SO4•− was the main contributor for RhB degradation, while the roles of aqueous SO4•− and •OH were very minor. Through characterization by XRD, XPS and FTIR analysis, it was determined that the electron transfer during activation of PS was accelerated by the oxygen functional groups on catalyst surface and the promoted redox cycle of Fe3+ and Fe2+ by Mn. Finally, the Mn–Fe–C composite catalyst exhibited an excellent reusability and stability with negligible leached Fe and Mn ions in solutions. Results of this study provide a promising design for heterogeneous catalysts that can effectively activate PS to remove organic pollutants from water at circumneutral pH conditions. [Display omitted] •Mn–Fe–C composite was tailor-designed to promote catalytic electron transfer.•Oxygen functional groups on catalyst promoted PS activation and RhB degradation.•Redox cycle of Fe3+ and Fe2+ was accelerated by Mn for electron transfer.•The Mn–Fe–C composite exhibited excellent stability and reusability. |
| ArticleNumber | 124228 |
| Author | Song, Zhijun Shi, Yuejing Zhang, Yu Wu, Liguang Wang, Qian Cai, Meiqiang Dong, Chunying Wu, Wentao Dionysiou, Dionysios D. Jin, Micong Wei, Zongsu |
| Author_xml | – sequence: 1 givenname: Meiqiang orcidid: 0000-0002-2566-276X surname: Cai fullname: Cai, Meiqiang email: caimeiqiang@163.com organization: School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, China – sequence: 2 givenname: Yu surname: Zhang fullname: Zhang, Yu organization: School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, China – sequence: 3 givenname: Chunying surname: Dong fullname: Dong, Chunying organization: School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, China – sequence: 4 givenname: Wentao surname: Wu fullname: Wu, Wentao organization: School of Materials Science and Engineering, Taiyuan University of Science and Technology, 030024, China – sequence: 5 givenname: Qian surname: Wang fullname: Wang, Qian organization: School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, China – sequence: 6 givenname: Zhijun surname: Song fullname: Song, Zhijun organization: School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, China – sequence: 7 givenname: Yuejing surname: Shi fullname: Shi, Yuejing organization: School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, China – sequence: 8 givenname: Liguang surname: Wu fullname: Wu, Liguang organization: School of Environmental Science and Engineering, Zhejiang Gongshang University, Hangzhou 310018, China – sequence: 9 givenname: Micong surname: Jin fullname: Jin, Micong organization: Key Laboratory of Health Risk Appraisal for Trace Toxic Chemicals of Zhejiang Province, Ningbo Municipal Center for Disease Control and Prevention, Ningbo 315010, China – sequence: 10 givenname: Dionysios D. surname: Dionysiou fullname: Dionysiou, Dionysios D. organization: Environmental Engineering and Science Program, Department of Chemical and Environmental Engineering (ChEE), University of Cincinnati, Cincinnati, OH 45221, USA – sequence: 11 givenname: Zongsu surname: Wei fullname: Wei, Zongsu email: zwei@eng.au.dk organization: Centre for Water Technology (WATEC), Department of Engineering, Aarhus University, Hangøvej 2, DK-8200 Aarhus N, Denmark |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/33246821$$D View this record in MEDLINE/PubMed |
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| Keywords | Mn doped Fe–C composite Iron redox cycle Surface bounded SO4 Reusability Persulfate Surface bounded SO4(•−) |
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| SubjectTerms | benzoquinones catalysts catalytic activity composite materials dyes electron paramagnetic resonance spectroscopy electron transfer ethanol Iron redox cycle manganese Mn doped Fe–C composite nitrobenzenes oxygen Persulfate phenol pollutants Reusability rhodamines Surface bounded SO4 |
| Title | Manganese doped iron–carbon composite for synergistic persulfate activation: Reactivity, stability, and mechanism |
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