Effect of Organic Matter on Iodine Mobilization in Groundwater of Datong Basin
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摘要: 地下水系统中有机质对碘迁移转化起着至关重要的作用，为深入分析地下水溶解性有机质（dissolved organic matter，DOM）对地下水碘迁移转化的影响，研究选取我国大同盆地浅、中层高碘地下水为研究对象，运用傅里叶变换离子回旋共振质谱（FT-ICR-MS）对地下水DOM分子结构进行分析表征.结果表明，地下水总碘浓度变化范围为1.97~926.10 μg/L，碘离子是地下水中碘的主要赋存形态；总碘浓度与DOM呈一定正相关关系（r=0.84），与可生物降解有机质含量呈负相关关系（r=-0.71）.研究区高碘地下水中有机质生物降解程度较高；高低碘地下水DOM分子组成差异表明，在降解过程中，微生物优先利用CHO、CHON1、CHON2类小分子可生物降解化合物，促使与之结合的碘迁移释放进入地下水；还原环境下地下水中碘主要来源于铁（氢）氧化物的还原性溶解和有机质的降解，且伴随有碘的形态转化，而氧化环境下地下水中碘可能与有机质的分子转化有关.Abstract: Organic matter plays an important role in the mobilization of iodine in groundwater system. In this study, the high iodine groundwater from shallow and middle aquifers in Datong basin in China was collected to perform the effect of dissolved organic matter (DOM) on iodine mobilization in groundwater. The structure of dissolved organic matter (DOM) in groundwater was characterized by Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS). The results show that the range of total iodine concentration in groundwater is 1.97-926.10 μg/L. Iodide is the main species of iodine in groundwater. The total iodine concentration has a positive correlation with DOM (r=0.84) and a negative correlation with biodegradable organic matter (r=-0.71), indicating that the organic matter in high iodine groundwater experience more intensive biodegradation. The differences of DOM molecular composition between high and low iodine groundwater further show that microorganisms preferentially use small molecular biodegradable compounds such as CHO, CHON1 and CHON2 to promote the release of bound iodine into groundwater during degradation. The hydrochemical fate of groundwater iodine under the reducing environment is mainly related to the reductive dissolution of iron (hydrogen) oxides and the biodegradation of organic matter, during which iodine species changed, while under oxidizing environment, it could be related to the transformation of natural organic matter.
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图 3 地下水碘形态三元图(a)和Eh对无机碘分布的影响(b)
Fig. 3. Ternary diagram of iodine species in groundwater (a) and effect of redox conditions on the species of inorganic iodine (b)
图 5 地下水中碘浓度与DOC浓度关系图
Fig. 5. Variation of iodine concentration with DOC of groundwater
图 6 地下水碘浓度与可生物降解DOM分子数(a)和HCO3-浓度(b)的关系图以及低、高碘地下水中不同元素组成的可生物降解DOM分子数箱型图(c)
Fig. 6. Variation of iodine concentration with the number of biodegradable DOM molecules (a) and HCO3- (b) of groundwater and box diagram of the number of biodegradable DOM molecules of different elemental compositions in low and high iodine groundwater (c)
图 7 总碘、不同形态碘浓度与地下水中DOM分子峰强度的相关性图
Fig. 7. Correlation between the concentration of total iodine, different forms of iodine and DOM molecule peak intensity in groundwater
表 1 FT-ICR-MS数据处理
Table 1. Data processing of FT-ICR-MS
参数 计算公式 意义 参考文献 双键当量(DBE) $ \frac{1+\left(2\mathrm{C}-\mathrm{H}+\mathrm{N}\right)}{2} $ 化合物分子中双键数和环状脂肪族化合物数的和，用来表征DON分子的不饱和度. Qiao et al. (2020) 芳香性指数(AImod) $ \frac{1+\mathrm{C}-0.5\mathrm{O}-\mathrm{S}-0.5\mathrm{H}}{\mathrm{C}-0.5\mathrm{O}-\mathrm{S}-\mathrm{N}-\mathrm{P}} $ 反映分子中可能存在的所有的C=C，C-O和C=O键，AImod > 0.5和AImod≥0.67分别代表芳香性结构和缩合芳香性结构. Xu et al. (2019) 标准氧化态(NOSC) $ 4-\frac{4\mathrm{C}+\mathrm{H}-3\mathrm{N}-2\mathrm{O}+5\mathrm{P}-2\mathrm{S}}{\mathrm{C}} $ 反映化合物的潜在能量，具有高NOSC值的有机分子在热力学上更有利于降解，并且形成易被微生物利用的基质. Pracht et al. (2018) 注：式中C、H、N、O、S、P分别代表分子中C、H、N、O、S、P原子的数目. 
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表 2 研究区地下水化学组分
Table 2. Chemical composition of groundwater samples from study area
参数 最小值 最大值 中位值 均值 pH 7.76 9.29 8.26 8.24 Eh(mV) -187.0 259.0 83.9 48.9 TDS(mg/L) 241.6 3 865 871.2 1124 K+(mg/L) 0.6 23.2 2.1 3.5 Na+(mg/L) 9.8 1 216 271.8 285.0 Ca2+(mg/L) 5.4 98.6 44.0 44.2 Mg2+(mg/L) 13.7 183.2 30.5 50.2 SO42-(mg/L) 0.9 1 469 148.9 280.4 HCO3-(mg/L) 180.4 1 424 373.6 508.4 Cl-(mg/L) 7.0 1 045 148.8 207.0 Br-(μg/L) 19.8 3 473 298.7 584.6 Fe总(mg/L) < 0.02 2.83 0.06 0.33 Fe2+(mg/L) < 0.02 0.67 0.03 0.08 I总(μg/L) 1.87 926.1 95.8 166.7 I-(μg/L) < 0.01 887.2 60.1 146.5 IO3-(μg/L) < 0.01 169.4 5.4 24.0 DOC(mg/L) 1.93 31.08 4.2 6.5
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表 3 FT-ICR-MS分析数据
Table 3. Analysis data of FT-ICR-MS
样品号 I
(μg/L)DOC
(mg/L)DOM分子总数 Eh
(mV)H/Cwa O/Cwa DBEwa NOSCwa (AImod)wa 低碘地下水
(I<100μg/L)DT20-05 28.44 5.21 4 751 -105.3 1.31 0.37 9.89 -0.45 0.26 DT20-07 15.92 3.34 5 217 -78.7 1.27 0.38 9.93 -0.45 0.28 DT20-08 11.65 3.57 5 153 75.0 1.29 0.38 9.8 -0.5 0.26 DT20-10 1.87 4.11 5 739 143.5 1.3 0.39 10.55 -0.36 0.22 DT20-17 66.13 6.8 5 738 -92.1 1.22 0.38 10.02 -0.4 0.29 DT20-18 11.1 4.22 4 067 109.5 1.29 0.37 10.4 -0.54 0.25 DT20-19 27.1 2.67 4 138 138.9 1.28 0.35 10.69 -0.54 0.26 高碘地下水
(I > 100μg/L)DT20-06 160.52 9.34 5 633 -107.1 1.16 0.39 10.77 -0.27 0.34 DT20-11 157.40 2.76 4 650 58.1 1.19 0.39 9.99 -0.4 0.29 DT20-25 160.12 8.62 6 407 -99.7 1.18 0.46 11.34 -0.23 0.29 DT20-12 519.64 9.5 5 655 -121.1 1.01 0.38 9.86 -0.38 0.27 DT20-20 323.16 15.8 6 211 -79.3 1.16 0.40 10.35 -0.32 0.34 DT20-27 321.08 6.97 6 209 -110.4 1.18 0.39 10.37 -0.31 0.33 DT20-30 326.20 2.28 6 767 12.1 1.21 0.42 10.20 -0.18 0.28 DT20-31 590.95 16.1 6 226 -160.0 1.19 0.47 10.76 -0.24 0.28 注：H/Cwa、O/Cwa、DBEwa、NOSCwa、(AImod)wa均为水样中DOM分子的峰强度加权平均值，双键当量(DBE)、标准氧化态(NOSC)、芳香性指数(AImod)的计算方法见表 2.
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