长江干流丰水期河水硫酸盐同位素组成特征及其来源解析

李小倩; 刘运德; 周爱国; 张彬

doi:10.3799/dqkx.2014.147

长江干流丰水期河水硫酸盐同位素组成特征及其来源解析

doi: 10.3799/dqkx.2014.147

李小倩^{1, 2,},
刘运德²,
周爱国^{1, 2, ,},
张彬¹

1.
中国地质大学环境学院, 湖北武汉 430074
2.
中国地质大学生物地质与环境地质国家重点实验室, 湖北武汉 430074

基金项目:

国家自然科学基金项目 41202169

中国博士后基金项目 2014M552114

中央高校基本科研业务费专项资金资助项目 CUGL140407

详细信息

作者简介:
李小倩(1982-), 博士, 讲师, 主要从事同位素地球化学与环境地球化学研究.E-mail: lixiaoqian2007@gmail.com

通讯作者:
周爱国, E-mail: aiguozhou@cug.edu.cn

中图分类号: P736.5
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出版历程
- 收稿日期: 2014-04-29
- 刊出日期: 2014-11-01

Sulfur and Oxygen Isotope Compositions of Dissolved Sulfate in the Yangtze River during High Water Period and Its Sulfate Source Tracing

Li Xiaoqian^{1, 2
,},
Liu Yunde²,
Zhou Aiguo^{1, 2
, ,},
Zhang Bin¹

1.
School of Environmental Studies, China University of Geosciences, Wuhan 430074, China
2.
State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, Wuhan 430074, China

摘要

摘要: 碳酸盐岩的硫酸风化机制及其与碳循环的关系是全球碳循环研究中最为关注的科学问题之一, 其关键问题是识别硫酸盐来源.通过分析长江干流丰水期SO₄^2-浓度及其硫、氧同位素组成特征, 探讨长江硫酸盐的来源及其主要控制因素.长江河水SO₄^2-含量呈现逐年增加的趋势, 并且年增幅度逐渐加大.δ³⁴S_SO4和δ¹⁸O_SO4变化范围为-3.5‰~5.6‰和3.7‰~9.2‰, 二者呈现显著的线性负相关关系.δ¹⁸O_SO4值从上游到下游的增加趋势受长江水δ¹⁸O_H2O值的空间组成特征的影响.研究表明, 大气降水(酸雨)和硫化物氧化是控制长江干流丰水期河水硫、氧同位素组成及其来源的主要机制, 为研究长江流域化学风化侵蚀作用和碳循环过程提供重要的理论依据.
- 硫同位素 /
- 氧同位素 /
- 硫酸盐来源 /
- 长江 /
- 地球化学
Abstract: Crustal weathering by sulfuric acid and its relationship with carbon cycling is a subject of greatest concern in the domain of global carbon cycling, with its key issue of the identification of riverine sulfate sources. In this study, stable sulfur and oxygen isotope compositions of riverine sulfate in the mainstream of the Yangtze River during rainy season are determined to trace the riverine sulfate sources and controlling factors. The SO₄^2-concentration keeps increasing with ever-increasing annual growth rate. The isotope compositions of dissolved sulfate in the Yangze River range from -3.5‰ to 5.6‰ for δ³⁴S_SO4 and from 3.7‰ to 9.2‰ for δ¹⁸O_SO4, showing a significantly negative linear correlation between δ³⁴S_SO4 and δ¹⁸O_SO4. The tendency of increased δ¹⁸O_SO4 values from upstream to downstream is controlled by δ¹⁸O_H2O values of the Yangtze River water. It is indicated that atmospheric acid deposition and sulfide oxidation are dominant sources of dissolved sulfate in the Yangze River. This study offers theoretical basis which facilitates further environmental explorations for chemical weathering of carbonate and carbon cycling.
- sulfur isotope /
- oxygen isotope /
- sulfate source /
- the Yangtze River /
- geochemistry

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图 1 长江流域采样点分布(据丁悌平等(2013)修改)

Fig. 1. A sketch map of the Yangtze River drainage area with sampling locations

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图 2 长江干流丰水期河水SO₄^2-浓度沿径流途径的变化曲线

Fig. 2. Plots showing spatial variations of SO₄^2- concentrations from the mainstream of the Yangtze River during high water period

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图 3 长江干流丰水期河水硫酸盐硫和氧同位素组成沿径流途径的变化曲线

Fig. 3. The special δ³⁴S_SO4 and δ¹⁸O_SO4 variations of dissolved sulfate in the water from the mainstream of the Yangtze River during high water period

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图 4 长江干流丰水期SO₄^2-的δ³⁴S_SO4和δ¹⁸O_SO4关系

Fig. 4. δ³⁴S_SO4 vs. δ¹⁸O_SO4 of dissolved sulfate in the water of the Yangtze River during high water period

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图 5 长江水的δ¹⁸O_H2O与硫酸盐的δ¹⁸O_SO4的关系

Fig. 5. δ¹⁸O_H2O of water vs. δ¹⁸O_SO4 of dissolved sulfate in the water of the Yangtze River

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表 1 长江干流丰水期河水主要离子与同位素组成的分析结果

Table 1. Chemical and isotopic compositions of Yangtze River during high water period

样品编号	采集时间	采样地点	经纬度坐标	pH	EC(μS/cm)	SO₄^2-	Cl^-	HCO₃^-	K⁺+Na⁺	Ca²⁺	Mg²⁺	δ³⁴S_SO4(‰ vs. VCDT)	δ¹⁸O_SO4(‰ vs. VSMOW)	δ¹⁸O_H2O(‰ vs. VSMOW)
样品编号	采集时间	采样地点	经纬度坐标	pH	EC(μS/cm)	(mg/L)						δ³⁴S_SO4(‰ vs. VCDT)	δ¹⁸O_SO4(‰ vs. VSMOW)	δ¹⁸O_H2O(‰ vs. VSMOW)
CJ1	2013.8.14	宜宾	E104°36′50.65″, N28°45′23.84″	8.19	317	37.3	24.9	124.4	22.4	31.3	7.7	3.5	5.0	-14.6
CJ2	2013.8.15	泸州	E105°26′07.41″, N28°52′13.31″	8.07	306	37.9	20.1	127.7	19.8	32.1	7.5	-0.8	5.9	-13.9
CJ3	2013.8.16	重庆	E106°31′28.72″, N29°31′39.03″	7.90	319	41.3	19.4	129.6	19.4	34.6	7.3	2.7	5.0	-13.7
CJ4	2013.8.17	涪陵	E107°23′20.32″, N29°42′53.31″	7.96	312	39.5	18.0	128.3	18.0	35.4	7.3	-	-	-13.2
CJ5	2013.8.19	万州	E108°22′54.51″, N30°48′34.17″	7.88	312	28.8	14.6	127.0	17.0	36.0	6.9	0.8	6.0	-12.7
CJ6	2013.8.20	奉节	E109°27′23.70″, N31°00′05.66″	7.86	319	41.9	16.8	132.9	17.0	36.8	6.8	1.5	6.9	-12.7
CJ7	2013.8.20	巴东	E110°19′46.73″, N31°02′55.35″	7.80	328	45.4	15.0	130.3	16.0	39.6	6.8	5.4	4.5	-11.9
CJ8	2013.8.20	宜昌	E111°16′50.94″, N30°45′16.03″	8.01	329	43.1	16.4	133.6	17.6	37.6	7.2	3.7	5.7	-11.8
CJ9	2013.8.22	沙市	E112°14′19.51″, N30°18′22.67″	7.84	335	42.2	17.3	128.3	17.0	37.0	7.0	5.2	3.7	-11.1
CJ23	2013.8.14	监利	E110°03′51.87″, N29°26′44.78″	7.96	324	36.1	14.8	130.0	17.4	37.3	6.9	-0.4	8.0	-11.5
CJ10	2013.8.23	岳阳	E113°31′00.27″, N29°49′53.60″	7.88	312	30.4	14.2	124.1	16.5	36.4	6.6	1.3	7.6	-12.3
CJ11	2013.8.22	洪湖	E114°14′27.08″, N30°30′15.16″	7.88	321	30.7	15.3	130.6	15.1	31.3	5.6	-3.5	9.2	-10.1
CJ12	2013.8.22	武汉	E115°03′58.39″, N30°14′48.88″	7.82	312	33.3	12.6	126.7	14.5	38.9	6.3	5.6	5.2	-10.7
CJ13	2013.8.7	黄石	E116°00′32.40″, N29°44′30.52″	7.77	313	35.8	12.4	128.3	15.1	38.3	6.4	3.8	7.0	-10.3
CJ14	2013.8.6	九江	E117°03′09.14″, N30°30′10.59″	7.73	293	34.5	11.8	117.3	14.2	35.5	6.0	-0.5	8.0	-9.5
CJ15	2013.8.5	安庆	E117°43′51.69″, N30°51′09.96″	7.78	304	33.9	12.7	123.8	14.7	36.5	6.0	4.8	5.1	-9.6
CJ16	2013.8.4	铜陵	E118°21′03.37″, N31°20′21.64″	7.73	306	35.0	12.9	122.2	15.1	37.7	6.1	-0.3	7.0	-9.5
CJ17	2013.8.4	芜湖	E118°29′11.98″, N31°45′58.97″	7.73	317	36.8	13.0	126.7	14.9	39.0	6.4	-1.5	8.4	-9.4
CJ18	2013.8.3	马鞍山	E118°37′08.29″, N31°56′32.31″	7.73	319	38.0	12.8	128.7	14.8	39.7	6.5	2.4	6.3	-8.5
CJ19	2013.8.2	南京	E119°22′47.55″, N32°13′55.79″	7.73	330	39.3	15.1	123.1	17.4	39.1	6.6	0.8	6.3	-9.1
CJ20	2013.7.31	镇江	E120°48′09.53″，N32°01′03.04″	7.81	319	36.9	15.4	114.0	21.3	45.7	7.6	-0.8	8.4	-9.2
CJ21	2013.7.30	南通	E121°36′44.00″, N31°21′29.00″	7.58	409	37.4	34.9	123.5	35.4	39.4	7.4	1.7	7.0	-8.4
CJ22	2013.7.28	上海	E113°01′25.00″, N29°31′44.50″	7.78	338	48.9	13.5	137.5	17.0	39.7	7.0	-2.3	8.8	-7.6

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表 2 铜陵-芜湖段SO₄^2-含量与历史数据的对比

Table 2. Comparisons of SO₄^2- concentration and its growth rate in the lower Tongling-Wuhu area

取样地点	取样时间	SO₄^2-(mg/L)	年增幅(mg/(L·a))
铜陵-芜湖段	2013年8月	35.0~36.8(35.9)^a	1.00^b
大通附近	2007年7月	29.6~30.1(29.9)(夏学齐等, 2008)	0.85^c
大通	1958—1990年平均值	11.9(Chen et al., 2002)	0.22^d
a.本研究的数据，括号内为铜陵-芜湖段数据的平均值；b.2007—2013年的SO₄^2-增加速率；c.1990—2007年的SO₄^2-增加速率.其中，1990年SO₄^2-含量(15.4mg/L)是结合1958—1990年SO₄^2-含量平均值(11.9mg/L)及其年增幅估算的；d.1958—1990年的SO₄^2-增加速率，数据来源于Chen et al.(2002).

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