Facile Synthesis of Atomic Fe-N-C Materials and Dual Roles Investigation of Fe-N Sites in Fenton-Like Reactions

Overview

Journal Adv Sci (Weinh)

Specialty Biomedical Engineering

Date 2021 Oct 13

PMID 34643069

Citations 8

Authors

Jun Wang

Bin Li

Yang Li

Xiaobin Fan

Fengbao Zhang

Guoliang Zhang

Wenchao Peng

Affiliations

Soon will be listed here.

Abstract

Fenton-like reactions with persulfates as the oxidants have attracted increasing attentions for the remediation of emerging antibiotic pollutions. However, developing effective activators with outstanding activities and long-term stabilities remains a great challenge in these reactions. Herein, a novel activator is successfully synthesized with single iron atoms anchored on porous N-doped carbon (Fe-N-PC) by a facile chemical vapor deposition (CVD) method. The single Fe atoms are coordinated with four N atoms according to the XANES, and the Fe-N -PC shows enhanced activity for the activation of peroxymonosulfate (PMS) to degrade sulfamethoxazole (SMX). The experiments and density functional theory (DFT) calculations reveal that the introduction of single Fe atoms will regulate the main active sites from graphite N into Fe-N , thus could enhance the stability and tune the PMS activation pathway from non-radical into radical dominated process. In addition, the N atoms connected with single Fe atoms in the Fe-N -C structure can be used to enhance the adsorption of organic molecules on these materials. Therefore, the Fe-N -C here has dual roles for antibiotics adsorption and PMS activation. The CVD synthesized Fe-N -C shows enhanced performance in persulfates based Fenton-like reactions, thus has great potential in the environmental remediation field.

Citing Articles

Robust Fe-N-CO single atom sites for efficient PMS activation and enhanced Fe = O reactivity.

Chen T, Zhang G, Sun H, Hua Y, Yang S, Zhou D Nat Commun. 2025; 16(1):2402.

PMID: 40064929 PMC: 11894199. DOI: 10.1038/s41467-025-57643-7.

Advanced Characterization Techniques and Theoretical Calculation for Single Atom Catalysts in Fenton-like Chemistry.

Xiong Z, Pan Z, Wu Z, Huang B, Lai B, Liu W Molecules. 2024; 29(16).

PMID: 39202799 PMC: 11357653. DOI: 10.3390/molecules29163719.

Precise coordination of high-loading Fe single atoms with sulfur boosts selective generation of nonradicals.

Jiang X, Zhou B, Yang W, Chen J, Miao C, Guo Z Proc Natl Acad Sci U S A. 2024; 121(4):e2309102121.

PMID: 38232287 PMC: 10823248. DOI: 10.1073/pnas.2309102121.

A polymer tethering strategy to achieve high metal loading on catalysts for Fenton reactions.

Wang L, Rao L, Ran M, Shentu Q, Wu Z, Song W Nat Commun. 2023; 14(1):7841.

PMID: 38030639 PMC: 10687042. DOI: 10.1038/s41467-023-43678-1.

Electron Delocalization Realizes Speedy Fenton-Like Catalysis over a High-Loading and Low-Valence Zinc Single-Atom Catalyst.

Xin S, Ni L, Zhang P, Tan H, Song M, Li T Adv Sci (Weinh). 2023; 10(34):e2304088.

PMID: 37840391 PMC: 10700237. DOI: 10.1002/advs.202304088.

References

Li H, Shan C, Pan B . Fe(III)-Doped g-CN Mediated Peroxymonosulfate Activation for Selective Degradation of Phenolic Compounds via High-Valent Iron-Oxo Species. Environ Sci Technol. 2018; 52(4):2197-2205. DOI: 10.1021/acs.est.7b05563. View

Wang J, Li B, Li Y, Fan X, Zhang F, Zhang G . Facile Synthesis of Atomic Fe-N-C Materials and Dual Roles Investigation of Fe-N Sites in Fenton-Like Reactions. Adv Sci (Weinh). 2021; 8(22):e2101824. PMC: 8596112. DOI: 10.1002/advs.202101824. View

Zhou Z, Li M, Kuai C, Zhang Y, Smith V, Lin F . Fe-based single-atom catalysis for oxidizing contaminants of emerging concern by activating peroxides. J Hazard Mater. 2021; 418:126294. DOI: 10.1016/j.jhazmat.2021.126294. View

Ren W, Xiong L, Nie G, Zhang H, Duan X, Wang S . Insights into the Electron-Transfer Regime of Peroxydisulfate Activation on Carbon Nanotubes: The Role of Oxygen Functional Groups. Environ Sci Technol. 2019; 54(2):1267-1275. DOI: 10.1021/acs.est.9b06208. View

Song P, Huang G, An C, Xin X, Zhang P, Chen X . Exploring the decentralized treatment of sulfamethoxazole-contained poultry wastewater through vertical-flow multi-soil-layering systems in rural communities. Water Res. 2020; 188:116480. DOI: 10.1016/j.watres.2020.116480. View

Wang J, Li B, Li Y, Fan X, Zhang F, Zhang G . Easily Regenerated CuO/γ-AlO for Persulfate-Based Catalytic Oxidation: Insights into the Deactivation and Regeneration Mechanism. ACS Appl Mater Interfaces. 2021; 13(2):2630-2641. DOI: 10.1021/acsami.0c19013. View

Qi C, Liu X, Li Y, Lin C, Ma J, Li X . Enhanced degradation of organic contaminants in water by peroxydisulfate coupled with bisulfite. J Hazard Mater. 2017; 328:98-107. DOI: 10.1016/j.jhazmat.2017.01.010. View

Wang Z, Jiang J, Pang S, Zhou Y, Guan C, Gao Y . Is Sulfate Radical Really Generated from Peroxydisulfate Activated by Iron(II) for Environmental Decontamination?. Environ Sci Technol. 2018; 52(19):11276-11284. DOI: 10.1021/acs.est.8b02266. View

Duan X, Sun H, Wang S . Metal-Free Carbocatalysis in Advanced Oxidation Reactions. Acc Chem Res. 2018; 51(3):678-687. DOI: 10.1021/acs.accounts.7b00535. View

10.

Michael I, Hapeshi E, Michael C, Varela A, Kyriakou S, Manaia C . Solar photo-Fenton process on the abatement of antibiotics at a pilot scale: Degradation kinetics, ecotoxicity and phytotoxicity assessment and removal of antibiotic resistant enterococci. Water Res. 2012; 46(17):5621-5634. DOI: 10.1016/j.watres.2012.07.049. View

11.

Qi C, Liu X, Ma J, Lin C, Li X, Zhang H . Activation of peroxymonosulfate by base: Implications for the degradation of organic pollutants. Chemosphere. 2016; 151:280-8. DOI: 10.1016/j.chemosphere.2016.02.089. View

12.

Yang C, Tsai L, Chang B . Anaerobic degradation of sulfamethoxazole in mangrove sediments. Sci Total Environ. 2018; 643:1446-1455. DOI: 10.1016/j.scitotenv.2018.06.305. View

13.

Jiang N, Xu H, Wang L, Jiang J, Zhang T . Nonradical Oxidation of Pollutants with Single-Atom-Fe(III)-Activated Persulfate: Fe(V) Being the Possible Intermediate Oxidant. Environ Sci Technol. 2020; 54(21):14057-14065. DOI: 10.1021/acs.est.0c04867. View

14.

Zhang T, Zhu H, Croue J . Production of sulfate radical from peroxymonosulfate induced by a magnetically separable CuFe2O4 spinel in water: efficiency, stability, and mechanism. Environ Sci Technol. 2013; 47(6):2784-91. DOI: 10.1021/es304721g. View

15.

Guo Z, Xie Y, Xiao J, Zhao Z, Wang Y, Xu Z . Single-Atom Mn-N Site-Catalyzed Peroxone Reaction for the Efficient Production of Hydroxyl Radicals in an Acidic Solution. J Am Chem Soc. 2019; 141(30):12005-12010. DOI: 10.1021/jacs.9b04569. View

16.

Du J, Guo W, Wang H, Yin R, Zheng H, Feng X . Hydroxyl radical dominated degradation of aquatic sulfamethoxazole by Fe/bisulfite/O: Kinetics, mechanisms, and pathways. Water Res. 2018; 138:323-332. DOI: 10.1016/j.watres.2017.12.046. View

17.

Li X, Huang X, Xi S, Miao S, Ding J, Cai W . Single Cobalt Atoms Anchored on Porous N-Doped Graphene with Dual Reaction Sites for Efficient Fenton-like Catalysis. J Am Chem Soc. 2018; 140(39):12469-12475. DOI: 10.1021/jacs.8b05992. View

18.

Lee H, Kim H, Weon S, Choi W, Hwang Y, Seo J . Activation of Persulfates by Graphitized Nanodiamonds for Removal of Organic Compounds. Environ Sci Technol. 2016; 50(18):10134-42. DOI: 10.1021/acs.est.6b02079. View

19.

Zhang T, Chen Y, Wang Y, Le Roux J, Yang Y, Croue J . Efficient peroxydisulfate activation process not relying on sulfate radical generation for water pollutant degradation. Environ Sci Technol. 2014; 48(10):5868-75. DOI: 10.1021/es501218f. View

20.

Teel A, Ahmad M, Watts R . Persulfate activation by naturally occurring trace minerals. J Hazard Mater. 2011; 196:153-9. DOI: 10.1016/j.jhazmat.2011.09.011. View