TY - JOUR
T1 - Insight into degradation mechanism of sulfamethoxazole by metal-organic framework derived novel magnetic Fe@C composite activated persulfate
AU - Pu, Mengjie
AU - Wan, Jinquan
AU - Zhang, Fengzhen
AU - Brusseau, Mark L.
AU - Ye, Daqi
AU - Niu, Junfeng
N1 - Funding Information:
This study was financially supported by the National Key Research and Development Project (No. 2018YFE0110400 ), the National Natural Science Foundation of China (Grant No. 51908127 ), the National Natural Science Fund for Distinguished Young Scholars (No. 51625801 ), the Guangdong Innovation Team Project for Colleges and Universities (No. 2016KCXTD023), and Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme (2017). The contributions of Mark L. Brusseau were supported by the National Institute of Environmental Health Sciences , United States Superfund Research Program ( P42 ES04940 ).
Publisher Copyright:
© 2021 Elsevier B.V.
PY - 2021/7/15
Y1 - 2021/7/15
N2 - Novel Fe@C composites derived from metal-organic framework (MOF) were synthesized. Being subject to pyrolysis under different temperatures endows these Fe@Cs diverse physical-chemical properties, including morphology, crystal structure, defect level, magnetism, and most importantly, iron phase composition. Fe@C-800 consists mainly of Fe3C and α-Fe, thus possesses strong ferromagnetic properties, which imparts the ability to be separated and recycled. Its catalytic activity towards the activation of persulfate (PS) and the decomposition of sulfamethoxazole (SMX) was found to be the best among all the Fe@Cs, and this activity can be regenerated by simple heat treatment. Given the mixed form of iron and N-doped carbon, α-Fe/Fe3C species provide electrons for PS to decompose and generate sulfate radical (SO4·−), hydroxyl radical (·OH), and superoxide radical (O2·−), initiating the radical pathway for partial SMX degradation. The positively charged C atoms on PS bonded Fe@C, as well as the conversion of O2·− give rise to the generation of singlet oxygen (1O2), which was responsible for the non-radical pathway for SMX degradation. As a consequence, SMX was degraded to intermediates through five degradation pathways, and finally mineralized to inorganic molecules. The results indicate that Fe@C-800 has great potential to serve as a promising activator for persulfate-mediated environmental remediation.
AB - Novel Fe@C composites derived from metal-organic framework (MOF) were synthesized. Being subject to pyrolysis under different temperatures endows these Fe@Cs diverse physical-chemical properties, including morphology, crystal structure, defect level, magnetism, and most importantly, iron phase composition. Fe@C-800 consists mainly of Fe3C and α-Fe, thus possesses strong ferromagnetic properties, which imparts the ability to be separated and recycled. Its catalytic activity towards the activation of persulfate (PS) and the decomposition of sulfamethoxazole (SMX) was found to be the best among all the Fe@Cs, and this activity can be regenerated by simple heat treatment. Given the mixed form of iron and N-doped carbon, α-Fe/Fe3C species provide electrons for PS to decompose and generate sulfate radical (SO4·−), hydroxyl radical (·OH), and superoxide radical (O2·−), initiating the radical pathway for partial SMX degradation. The positively charged C atoms on PS bonded Fe@C, as well as the conversion of O2·− give rise to the generation of singlet oxygen (1O2), which was responsible for the non-radical pathway for SMX degradation. As a consequence, SMX was degraded to intermediates through five degradation pathways, and finally mineralized to inorganic molecules. The results indicate that Fe@C-800 has great potential to serve as a promising activator for persulfate-mediated environmental remediation.
KW - FeC
KW - Ferromagnetic
KW - MOF
KW - PS
KW - SMX
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U2 - 10.1016/j.jhazmat.2021.125598
DO - 10.1016/j.jhazmat.2021.125598
M3 - Article
C2 - 34030424
AN - SCOPUS:85102302403
SN - 0304-3894
VL - 414
JO - Journal of Hazardous Materials
JF - Journal of Hazardous Materials
M1 - 125598
ER -