The Water-Sediment Regulation Scheme at Xiaolangdi Reservoir and Its Impact on Sulfur Cycling in the Yellow River Basin
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摘要: 陆地风化的硫酸盐（SO42-）通过河流体系输入海洋，其通量以及硫酸盐同位素组成（δ34SSO4和δ18OSO4）对全球硫循环及海洋SO42-同位素组成至关重要.河流体系SO42-含量及δ34SSO4和δ18OSO4组成不但受SO42-来源控制，而且受河流内部硫酸盐细菌还原及氧化过程影响，但其影响程度仍不明确，特别是拦河筑坝以及水沙调控过程对流域硫循环的影响仍不清楚.选择黄河小浪底水库作为研究对象，借助水化学、水体氢氧同位素（δDH2O和δ18OH2O）及δ34SSO4和δ18OSO4方法，通过对比分析水沙调控前后下泄河水SO42-含量及同位素组成差异，阐明水沙调控过程对河水SO42-通量及同位素组成的影响机制.结果表明：（1）2018年黄河小浪底水库水沙调控发生在7月份，8月份泥沙下泄与中游黄土高原降雨有关.两次排沙过程下泄水δ18OH2O均值分别为-8.1‰和-8.9‰，SO42-均值分别为1.43 mmol/L和1.77 mmol/L，δ34SSO4均值分别为8.3‰和7.4‰，δ18OSO4均值分别为5.4‰和5.7‰.（2）水沙调控开始前（6月份）下泄河水δ18OH2O均值为-7.0‰，SO42-均值为1.59 mmol/L，δ34SSO4均值为8.0‰，δ18OSO4均值为7.5‰；水沙调控结束后（10月份）下泄河水δ18OH2O均值为-9.2‰，SO42-均值为1.26 mmol/L，δ34SSO4均值为6.7‰，δ18OSO4均值为7.3‰.（3）黄河小浪底水库7月份水沙调控导致泥沙暴露，有机硫和来自硫酸盐细菌还原产生的硫化物发生氧化，造成下泄河水δ18OSO4值降低，但下泄河水在下游河道内流动过程中δ34SSO4和δ18OSO4变化不大.（4）2018年黄河小浪底水文站SO42-输出通量为0.061 Tmol/a，水沙调控过程SO42-输出通量占全年SO42-输出通量的比例为14.8%，入海δ34SSO4和δ18OSO4流量均值分别为7.6‰和6.8‰.黄河排沙过程改变原有水-沉积物界面环境，导致硫化物以及有机硫二次释放，改变了黄河入海硫酸盐通量以及硫和氧同位素组成.Abstract: Weathering-derived sulfate (SO42-) from the Continent could be transported to the Ocean by river systems, and sulfate flux coupled with sulfur and oxygen isotope compositions (δ34SSO4 and δ18OSO4) were vital to the global sulfur cycling and sulfate isotope compositions in ocean. SO42- contents together with δ34SSO4and δ18OSO4 values were not only controlled by SO42- sources, but affected by sulfate bacterial reduction (SBR) in internal riversystem, however, these effects were still unclear, and particularly the influences from dam and water-sediment regulation scheme (WSRS) on sulfur cycling in watershed were still unknown. The Xiaolangdi Reservoir in the Yellow River was selected to solve this problem, and hydrochemical compositions, water isotope compositions (δDH2O and δ18OH2O), and δ34SSO4and δ18OSO4 were determined to constrain the effects of WSRS on riverine sulfate flux and isotope compositions by comparing the SO42- contents and isotope compositions before and after the WSRS. The results indicated that (1) WSRS occurred in July 2018, sediment discharge in August was due to sediment scoured by precipitation in midstream of Yellow River. The discharged river water during these two sediment removal had average δ18OH2O values of -8.1‰ and -8.9‰, and average SO42- concentrations of 1.43 mmol/L and 1.77 mmol/L, and average δ34SSO4 values of 8.3‰ and 7.4‰, and average δ18OSO4 values of 5.4‰ and 5.7‰, respectively. (2) The dischared river water before the WSRS (June) had positive average 18OH2O value of -7.0‰, moderate average SO42- concentration of 1.59 mmol/L, positive average δ34SSO4 and δ18OSO4values of 8.0‰ and 7.5‰, resepectively. The dischared river water after the WSRS (October) had negative average δ18OH2O value of -9.2‰, low average SO42- concentration of 1.26 mmol/L, negative average δ34SSO4 value of 6.7‰ and positive average δ18OSO4value of 7.3‰, respectively. (3) The WSRS in July resulted in the exposure of sediment, and the organic sulfur and sulfide from SBR had been reoxidized to sulfate, during which water oxygen was incorporated into fresh sulfate with low oxygen isotope composition, but there was small varitaion of δ34SSO4 and δ18OSO4values in downstream river water. (4) The SO42- flux was about 0.061 Tmol/a in 2018, and the proporation of SO42- flux during WSRS was about 14.8%. The flow-weighted average δ34SSO4 and δ18OSO4values of SO42- into the Ocean were 7.6‰ and 6.8‰, respectively. The conclusion is that the WSRS had altered the water-sediment environment in the Yellow River, and corresponding organic and sulfide were released into the air and reoxidized, which changed the sulfate flux and sulfur and oxygen isotope compostion to the Ocean.
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图 1 2018年黄河小浪底水库水沙调控期间不同站点水流量、水位以及泥沙含量变化图
Fig. 1. Variations of discharge, water level and silt content during the water-sediment regulation scheme at Xiaolangdi Station in 2018
图 2 黄河小浪底水库下游河水采样点位置
Fig. 2. Locations of water samples in the downstream of the Xiaolangdi Reservoir in the Yellow River
图 3 黄河小浪底水库水沙调控过程水体氢氧同位素组成(a)及氧同位素(b)和氘盈余值(c)空间变化
Fig. 3. Water hydrogen and oxygen isotope relations (a) and the spatial variations of water oxygen (b) and dexcess values (c) during the water-sediment regulation by the Xiaolangdi Reservoir in the Yellow River
图 4 黄河小浪底水库水沙调控过程水体硫酸盐含量(a)、硫酸盐硫同位素(b)和氧同位素(c)时空变化
Fig. 4. Spatial and temporal variations of sulfate concentration (a), sulfur isotope (b) and oxygen isotope (c) values during the water-sediment regulation by the Xiaolangdi Reservoir in the Yellow River
图 5 研究区水体SO42- vs. δ34SSO4 (a), δ34SSO4 vs. δ18OSO4 (b)以及δ18OH2O vs. δ18OSO4 (c)关系图
Fig. 5. The relations between SO42- and δ34SSO4 (a), δ34SSO4 and δ18OSO4 (b), and δ18OH2O vs. δ18OSO4 (c)
表 1 黄河小浪底水库下游水体水化学及同位素组成
Table 1. Hydrochemical and isotope compositions of water samples in the downstream of the Xiaolangdi Reservoir
内容 单位 黄河干流河水 支流河水 地下水 排沙前 第一次排沙 第二次排沙 排沙结束后 沁河 伊洛河 日期 6月 7月 8月 10月 7/10 6/7/10 6/8/10 pH值 8.4±0.1 7.9±0.1 8.1±0.1 8.5±0.1 8.2±1.0 8.3±0.2 7.7±0.1 EC值 μS/cm 948±34 902±51 806±50 745±6 714±171 672±150 878±48 DO值 mg/L 6.96±0.26 3.59±1.72 nd 9.26±0.32 6.92 8.23±1.98 10.43 K+ mmol/L 0.13±0.00 0.13±0.01 0.13±0.00 0.12±0.01 0.11±0.05 0.13±0.04 0.08±0.02 Na+ mmol/L 4.32±0.21 3.90±0.32 3.97±0.17 2.84±0.14 1.77±0.23 1.63±0.75 2.24±0.31 Ca2+ mmol/L 1.36±0.06 1.29±0.14 1.44±0.07 1.37±0.07 1.99±0.81 1.57±0.46 2.06±0.29 Mg2+ mmol/L 1.18±0.04 1.10±0.12 1.17±0.05 1.05±0.05 1.07±0.19 1.02±0.18 1.57±0.20 HCO3- mmol/L 3.14±0.34 3.59±0.28 2.94±0.08 3.23±0.06 2.97±0.81 3.15±0.41 8.51±0.35 SO42- mmol/L 1.59±0.11 1.43±0.16 1.77±0.08 1.26±0.01 1.61±0.47 1.13±0.24 0.12±0.03 NO3- mmol/L 0.21±0.02 0.25±0.02 0.22±0.02 0.12±0.03 0.22±0.07 0.26±0.07 0.01±0.01 Cl- mmol/L 2.92±0.19 2.54±0.38 2.24±0.07 1.36±0.22 1.25±0.14 1.18±0.44 1.39±0.06 TZ+ meq/L 9.55±0.39 8.85±0.69 9.35±0.39 7.82±0.36 8.04±1.76 6.95±1.82 9.65±1.35 TZ- meq/L 9.48±0.52 9.24±0.51 8.98±0.22 7.13±0.49 7.69±1.66 6.87±1.32 10.17±0.46 NICB* % 0.7±3.2 -4.9±8.6 3.9±3.2 8.5±8.7 4.3±0.3 0.0±6.6 -6.4±11.5 δDH2O ‰ -56±1 -56±0 -62±0 -64±0 -52±3 -52±2 -71±0 δ18OH2O ‰ -7.0±0.1 -8.1±0.2 -8.9±0.1 -9.2±0.1 -7.4±0.4 -7.5±0.4 -10.1±0.1 δ34SSO4 ‰ 8.0±0.3 8.3±0.1 7.4±0.2 6.7±0.1 9.1±2.1 10.9±2.9 44.3±1.3 δ18OSO4 ‰ 7.5±0.6 5.4±0.6 5.7±0.3 7.3±0.3 5.8±1.9 6.0±1.4 12.8±0.5 注：*.NICB=（TZ+-TZ-）/TZ+×100%，其中TZ+=K++Na++2Ca2++2Mg2+，TZ-=HCO3-+2SO42-+NO3-+Cl-，单位：meq/L；nd=no detected. 
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表 2 黄河流域河水硫酸盐潜在来源的δ34SSO4和δ18OSO4组成
Table 2. Sulfur and oxygen isotope values of potential riverine sulfate sources in the Yellow River Basin
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表 3 研究区地表水硫酸盐来源混入比例计算结果Fig. 3 The mixing ratios of variable sulfate sources in surface water in studied area
来源 排沙前下泄河水(6月) 第一次排沙下泄水(7月) 第二次排沙下泄水(8月) 排沙结束后下泄水(10月) 均值±标准偏差(%) 均值±标准偏差(%) 均值±标准偏差(%) 均值±标准偏差(%) 大气降水 9.0±6.8 14.2±10.6 9.6±6.9 15.9±9.2 沉积岩黄铁矿 15.9±2.7 24.9±11.3 27.6±2.0 16.6±1.9 黄土石膏溶解 61.4±10.0 37.4±17.8 48.4±14.9 49.6±10.4 生活污水 9.7±7.5 16.0±12.4 9.5±6.5 12.4±7.4 化学肥料 4.1±2.7 7.5±5.4 4.9±3.2 5.5±3.2
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表 4 2018年黄河小浪底水库下泄水流量、硫酸盐含量以及硫和氧同位素组成、人为输出硫酸盐通量
Table 4. Water discharge, sulfate concentration, sulfur and oxygen isotope values of river water from Xiaolangdi Reservoir and anthropogenic sulfate fluxes
时期 下泄水流量 SO42- δ34SSO4 δ18OSO4 SO42-通量 人为输入SO42- 108 m3 mmol/L ‰ ‰ Tmol Tmol 1月~6月 161.9 1.59 8.0 7.5 0.026 0.003 6 7月 64.7 1.43 8.3 5.4 0.009 0.002 1 8月 56.1 1.77 7.4 5.7 0.010 0.001 4 9月~12月 127.5 1.26 6.7 7.3 0.016 0.002 9 全年 410.2 1.49a 7.6a 6.8a 0.061 0.010 0 注：a. 流量均值.
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