Mechanistic insights into sulfate and phosphate-mediated hexavalent chromium removal by tea polyphenols wrapped nano-zero-valent iron

Du, Changsheng; Xu, Nan; Yao, Zihan; Bai, Xu; Gao, Yuxi; Peng, Lei; Gu, Baohua; Zhao, Jiating

doi:10.1016/j.scitotenv.2022.157996

Title: Mechanistic insights into sulfate and phosphate-mediated hexavalent chromium removal by tea polyphenols wrapped nano-zero-valent iron

Journal Article · Fri Aug 12 00:00:00 EDT 2022 · Science of the Total Environment

DOI:https://doi.org/10.1016/j.scitotenv.2022.157996· OSTI ID:1968705

Du, Changsheng ^[1]; Xu, Nan ^[1]; Yao, Zihan ^[1]; Bai, Xu ^[2]; Gao, Yuxi ^[2]; Peng, Lei ^[1];

^[3]; Zhao, Jiating ^[2]

Suzhou University of Science and Technology (China)
Institute of High Energy Physics, Beijing (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Environmental Sciences Division

Nano zero-valent iron via green synthesis (g-nZVI) has great potential in removing toxic hexavalent Cr(VI) from industrial wastewater. Sulfate and phosphate in wastewater can influence Cr(VI) removal by g-nZVI. Here, in this study, the Cr(VI) removal kinetics by different g-nZVI materials were investigated with the existence of sulfate and/or phosphate, and the corresponding mechanisms were first revealed using multiple characterizations, including X-ray absorption near-edge spectra (XANES) and X-ray photoelectron spectroscopy (XPS). The results showed that Cr(OH)₃ was the dominant species initially formed on the surface of g-nZVI particles before transforming to Cr₂O₃ during the reaction of g-nZVI with Cr(VI). Sulfate in wastewater can promote the reduction from Cr(VI) to Cr(OH)₃ by g-nZVI, because sulfate triggers the release of Fe(II) and tea polyphenols (from tea extracts) from the g-nZVI surface due to the corrosion of Fe⁰ core, which is in line with an obvious increase in pseudo-second-order rate constant (k₂) and subtle change in Cr(VI) removal capacity (q_e). However, phosphate impedes the g-nZVI corrosion and inhibits q_e because of the inner-sphere complexation of phosphate onto g-nZVI decreasing the released Fe(II) for Cr₂O₃ production. When sulfate and phosphate coexisted in contaminated water, the inhibition effect of phosphate in Cr(VI) removal by g-nZVI was stronger than the promotion of sulfate. Accordingly, q_e value of g-nZVI declined from 93.4 mg g^–1 to 77.5 mg g^–1, while k₂ remained constant as the molar ratio of phosphate/sulfate increased from 0.1 to 10 in water. This study provides new insights into applying g-nZVI in efficient Cr(VI) removal from contaminated water with enrichment of sulphates and phosphates.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE; National Natural Science Foundation of China (NSFC); Chinese Academy of Sciences

Grant/Contract Number:: AC05-00OR22725; 21777110

OSTI ID:: 1968705

Alternate ID(s):: OSTI ID: 1961907

Journal Information:: Science of the Total Environment, Vol. 850, Issue 12; ISSN 0048-9697

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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chromium
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Title: Mechanistic insights into sulfate and phosphate-mediated hexavalent chromium removal by tea polyphenols wrapped nano-zero-valent iron

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