Citation: Xiaokang Hou, Huanxin Ma, Mengmeng Zhao, Chunhua Feng, Shishu Zhu. Unveiling role of Cu(Ⅱ) in photochemical transformation and reactive oxygen species production of schwertmannite in the presence of tartaric acid[J]. Chinese Chemical Letters, ;2025, 36(7): 110332. doi: 10.1016/j.cclet.2024.110332 shu

Unveiling role of Cu(Ⅱ) in photochemical transformation and reactive oxygen species production of schwertmannite in the presence of tartaric acid

The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, School of Environment and Energy, South China University of Technology, Guangzhou 510006, China

zhushishu@scut.edu.cn

Received Date: 5 May 2024
Revised Date: 7 July 2024
Accepted Date: 9 August 2024
Available Online: 11 August 2024

Figures(5)

Light exposure can accelerate phase transformation of Schwertmannite (Sch) coexisting with low-molecular-weight organic acids (LMWOAs), affecting the cycling of Fe in acid mine drainage (AMD). However, it is still unclear how this process relates to the fate of heavy metal contaminants. The study comprehensively reports the significant role and speciation redistribution of Cu(Ⅱ) during the photochemical transformation of a Sch/tartaric acid (TA) system. Based on X-ray diffractometer and Fourier transform infrared spectra results, the presence of TA in simulated AMD significantly promoted photoreductive dissolution and phase transformation of Sch to magnetite (Mt) and goethite (Gt) under anoxic and oxic conditions, respectively. With the addition of 10–30 mg/L Cu(Ⅱ), this transformation of Sch/TA system was significantly inhibited, i.e., only Gt occurred as product under anoxic conditions and even no phase transformation under oxic conditions. The results of EPR and adsorbed Fe(Ⅱ) indicated that the coexistence of Cu(Ⅱ) suppressed the amount of adsorbed Fe(Ⅱ) available for the transformation of Sch via competitive adsorption with Fe(Ⅱ) and inhibition of ligand-to-metal charge transfer (LMCT) of Sch-TA complexes. Chemical speciation and X-ray photoelectron spectroscopy analysis revealed the proportions of adsorbed and structural Cu(Ⅱ) of Sch/TA system were observably enhanced due to an increase in pH and recrystallization/nucleation growth of newly formed Gt. Under anoxic conditions, 62.7%-75.88% of Cu(Ⅱ) was adsorbed on the mineral surface, and during the nucleation and growth of secondary mineral phases, 15.49%-17.01% of Cu(Ⅱ) was incorporated into their crystal structure. The changes in distribution of Cu(Ⅱ) further suggested the photochemical transformation of Sch facilitated the sequestration of heavy metals and reduced their bioavailability. These findings enhance the understanding of role and redistribution of Cu(Ⅱ) during the transformation of Sch/LMWOA system in euphotic zone of AMD and provid insights of exploring engineered strategies of AMD remediation.
- Acid mine drainage,
- Photochemical transformation,
- Reactive oxygen species,
- Heavy metals,
- Ligand-to-metal charge transfer
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