Insights to PFOS elimination with peroxydisulfate activation mediated by boron modified Fe/C catalysts: Enhancing mechanism of boron and PFOS degradation pathway

Yanting Jiang; Zhendong Yu; Yuancai Lv; Xiaojuan Li; Chunxiang Lin; Xiaoxia Ye; Guifang Yang; Yifan Liu; Leilei Dai; Minghua Liu; Roger Ruan

doi:10.1016/j.jcis.2023.08.198

Insights to PFOS elimination with peroxydisulfate activation mediated by boron modified Fe/C catalysts: Enhancing mechanism of boron and PFOS degradation pathway

J Colloid Interface Sci. 2023 Dec 15;652(Pt B):1743-1755. doi: 10.1016/j.jcis.2023.08.198. Epub 2023 Sep 1.

Authors

Yanting Jiang¹, Zhendong Yu², Yuancai Lv³, Xiaojuan Li⁴, Chunxiang Lin⁵, Xiaoxia Ye⁶, Guifang Yang⁷, Yifan Liu⁸, Leilei Dai⁹, Minghua Liu¹⁰, Roger Ruan¹¹

Affiliations

¹ Fujian Provincial Engineering Research Center of Rural Waste Recycling Technology, College of Environment & Safety Engineering, Fuzhou University, Fuzhou 350116, China. Electronic address: 210627043@fzu.edu.cn.
² Fujian Provincial Engineering Research Center of Rural Waste Recycling Technology, College of Environment & Safety Engineering, Fuzhou University, Fuzhou 350116, China. Electronic address: n190627064@fzu.edu.cn.
³ Fujian Provincial Engineering Research Center of Rural Waste Recycling Technology, College of Environment & Safety Engineering, Fuzhou University, Fuzhou 350116, China. Electronic address: yclv@fzu.edu.cn.
⁴ Fujian Provincial Engineering Research Center of Rural Waste Recycling Technology, College of Environment & Safety Engineering, Fuzhou University, Fuzhou 350116, China. Electronic address: lixiaojuan@fzu.edu.cn.
⁵ Fujian Provincial Engineering Research Center of Rural Waste Recycling Technology, College of Environment & Safety Engineering, Fuzhou University, Fuzhou 350116, China. Electronic address: lcx2010@fzu.edu.cn.
⁶ Fujian Provincial Engineering Research Center of Rural Waste Recycling Technology, College of Environment & Safety Engineering, Fuzhou University, Fuzhou 350116, China. Electronic address: yexiaoxia@fzu.edu.cn.
⁷ Fujian Provincial Key Laboratory of Ecology-Toxicological Effects & Control for Emerging Contaminants, Putian University, Putian 351100, China. Electronic address: abc396550322@163.com.
⁸ Fujian Provincial Engineering Research Center of Rural Waste Recycling Technology, College of Environment & Safety Engineering, Fuzhou University, Fuzhou 350116, China; Indoor Environment Engineering Research Center of Fujian Province, Fujian University of Technology, Fuzhou 350118, China. Electronic address: yfanym@fzu.edu.cn.
⁹ Center for Biorefining, and Department of Bioproducts and Biosystems Engineering, University of Minnesota Twin Cities, St. Paul, MN 55108, United States of America. Electronic address: dai00087@umn.edu.
¹⁰ Fujian Provincial Engineering Research Center of Rural Waste Recycling Technology, College of Environment & Safety Engineering, Fuzhou University, Fuzhou 350116, China; Fujian Provincial Key Laboratory of Ecology-Toxicological Effects & Control for Emerging Contaminants, Putian University, Putian 351100, China. Electronic address: mhliu2000@fzu.edu.cn.
¹¹ Center for Biorefining, and Department of Bioproducts and Biosystems Engineering, University of Minnesota Twin Cities, St. Paul, MN 55108, United States of America. Electronic address: ruanx001@umn.edu.

PMID: 37672977
DOI: 10.1016/j.jcis.2023.08.198

Abstract

In this study, the boron-doped iron-carbon composite (Fe@B/C-2) was prepared via a simple solvothermal and secondary calcination process by using iron metal-organic frameworks (Fe-MOFs) as precursor. The obtained Fe@B/C-2 possessed abundant active sites and low iron ion leaching, and exhibited excellent performance on peroxydisulfate (PDS) activation for efficient PFOS (10 mg/L) degradation (94 %) in 60 min, with 0.2 g/L of catalyst dosage, 1.0 g/L of PDS dosage and at 5.0 of initial pH. The radical scavenging and electron paramagnetic resonance (EPR) tests demonstrated that SO₄·^- and ·OH were the primary active species during PFOS elimination. Under the attack of these species, PFOS was first transformed into PFOA, followed by a sequential defluorination process, and lastly mineralized into CO₂ and F^-. Notably, DFT results revealed that Fe species, -BC₃/-BC₂O structures on the carbon matrix performed crucial roles in PDS activation. The extraordinary catalytic activity of Fe@B/C-2 was attributable to the synergistic effects of Fe nanoparticles and the B-doped on carbon matrix. The doped B not only could activate the inert carbon skeleton and provided more catalytic centers, but also could accelerate the electron transfer efficiency, leading to a boost in PDS decomposition.

Keywords: Boron-doping; Degradation; Fe-based catalyst; Perfluorooctane sulfonic acid; Peroxydisulfate activation.