Electron Hopping Enables Rapid Electron Transfer between Quinone-/Hydroquinone-Containing Organic Molecules in Microbial Iron(III) Mineral Reduction

对苯二酚 化学 电子转移 扩散 氧化还原 反应速率常数 电子供体 光化学 铁酸盐 电子传输链 分析化学(期刊) 分子 无机化学 动力学 物理化学 有机化学 催化作用 物理 吸附 生物化学 热力学 量子力学
作者
Yuge Bai,Tianran Sun,Largus T. Angenent,Stefan B. Haderlein,Andreas Kappler
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:54 (17): 10646-10653 被引量:43
标识
DOI:10.1021/acs.est.0c02521
摘要

The mechanism of long-distance electron transfer via redox-active particulate natural organic matter (NOM) is still unclear, especially considering its aggregated nature and the resulting low diffusivity of its quinone- and hydroquinone-containing molecules. Here we conducted microbial iron(III) mineral reduction experiments in which anthraquinone-2,6-disulfonate (AQDS, a widely used analogue for quinone- and hydroquinone-containing molecules in NOM) was immobilized in agar to achieve a spatial separation between the iron-reducing bacteria and ferrihydrite mineral. Immobilizing AQDS in agar also limited its diffusion, which resembled electron-transfer behavior of quinone- and hydroquinone-containing molecules in particulate NOM. We found that, although the diffusion coefficient of the immobilized AQDS/AH2QDS was 10 times lower in agar than in water, the iron(III) mineral reduction rate (1.60 ± 0.28 mmol L–1 Fe(II) d–1) was still comparable in both media, indicating the existence of another mechanism that accelerated the electron transfer under low diffusive conditions. We found the correlation between the heterogeneous electron-transfer rate constant (10–3 cm s–1) and the diffusion coefficient (10–7 cm2 s–1) fitting well with the "diffusion-electron hopping" model, suggesting that electron transfer via the immobilized AQDS/AH2QDS couple was accomplished through a combination of diffusion and electron hopping. Electron hopping increased the diffusion concentration gradient up to 106-fold, which largely promoted the overall electron-transfer rate during microbial iron(III) mineral reduction. Our results are helpful to explain the electron-transfer mechanisms in particulate NOM.
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