Fluctuating redox conditions accelerate the electron storage and transfer in magnetite and production of dark hydroxyl radicals
文献类型：期刊论文
| 作者 | Li, Dan3,4,5; Sun, Jieyi5; Fu, Yibo5; Hong, Wentao5; Wang, Heli2,3,4; Yang, Qian2,3,4; Wu, Junhong2,3,4; Yang, Sen2,3,4; Xu, Jianhui5; Zhang, Yunfei5 |
| 刊名 | WATER RESEARCH
 |
| 出版日期 | 2024 |
| 卷号 | 248页码:11 |
| 关键词 | Magnetite Dark hydroxyl radicals Fluctuating redox conditions Electron storage and transfer Dissolved organic matter |
| ISSN号 | 0043-1354 |
| DOI | 10.1016/j.watres.2023.120884 |
| 英文摘要 | Magnetite (Fe3O4), known as a geo-battery that can store and transfer electrons, often co-occurs with sulfide in subsurface environments with fluctuating redox conditions. However, little is known about how fluctuating redox conditions (e.g., sulfidation-oxidation) affect the electron storage and transfer in Fe3O4 that was associated with the production of dark hydroxyl radicals (center dot OH) and the oxidation of dissolved organic matter (DOM). This study revealed that Fe3O4 sulfidated by sulfide (S-Fe3O4) at neutral pH exhibited higher center dot OH production upon oxygenation than Fe3O4, in which the cumulative center dot OH concentration increased with increasing initial S/Fe ratio (<= 0.50), sulfidation duration and number of sulfidation-oxidation cycle. X-ray photoelectron spectroscopy and wet-chemical analyses of Fe and S species of S-Fe3O4 showed that sulfidation enables electron storage in Fe3O4 by increasing both structural and surface Fe(II). Sulfide was converted into S0, acid volatile sulfur (AVS), and chromium-reducible sulfur (CRS) during Fe3O4 sulfidation. S-Fe3O4 with lower AVS/CRS ratio exhibited higher reactivity to produce center dot OH, indicating the important role of CRS in transferring electrons from Fe(II) to O2. Based on quenching experiments and electron paramagnetic resonance analysis, a one-step two-electron transfer mechanism was proposed for O2 reduction during S-Fe3O4 oxygenation, and surface-bound rather than free center dot OH were identified as the primary reactive oxygen species. The center dot OH from S-Fe3O4 oxygenation was shown to be efficient in degradation of DOM. Overall, these results suggested that sulfidation-oxidation can accelerate the electron storage and transfer in Fe3O4 for dark center dot OH production, having an important impact on the carbon cycling in subsurface environments. |
| WOS研究方向 | Engineering ; Environmental Sciences & Ecology ; Water Resources |
| 语种 | 英语 |
| WOS记录号 | WOS:001127552400001 |
| 源URL | [http://ir.gig.ac.cn/handle/344008/75424]  |
| 专题 | 有机地球化学国家重点实验室 |
| 通讯作者 | Zhong, Yin |
| 作者单位 | 1.Guangdong Prov Acad Environm Sci, Guangdong Key Lab Contaminated Sites Environm Mana, Guangzhou 510045, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Chinese Acad Sci, Guangdong Hong Kong Macao Joint Lab Environm Pollu, Guangdong Prov Key Lab Environm Protect & Resource, State Key Lab Organ Geochem,Guangzhou Inst Geochem, Guangzhou 510640, Peoples R China 4.Guangdong Prov Key Lab Environm Protect & Resource, Guangzhou 510640, Peoples R China 5.Dongguan Univ Technol, Sch Environm & Civil Engn, Dongguan 523808, Peoples R China |
| 推荐引用方式 GB/T 7714 | Li, Dan,Sun, Jieyi,Fu, Yibo,et al. Fluctuating redox conditions accelerate the electron storage and transfer in magnetite and production of dark hydroxyl radicals[J]. WATER RESEARCH,2024,248:11. |
| APA | Li, Dan.,Sun, Jieyi.,Fu, Yibo.,Hong, Wentao.,Wang, Heli.,...&Peng, Ping'an.(2024).Fluctuating redox conditions accelerate the electron storage and transfer in magnetite and production of dark hydroxyl radicals.WATER RESEARCH,248,11. |
| MLA | Li, Dan,et al."Fluctuating redox conditions accelerate the electron storage and transfer in magnetite and production of dark hydroxyl radicals".WATER RESEARCH 248(2024):11. |
入库方式： OAI收割
来源：广州地球化学研究所
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