Progresses in Study of Mercury Isotopic Compositions in the Ocean
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摘要: 海洋作为地球上最重要的汞储库之一，在调节全球汞循环中起着关键作用.近年来，汞同位素在研究海洋汞生物地球化学循环方面展现出明显优势，不但能示踪现代海洋汞污染来源及转化过程，还可重建古环境、古气候.总结了不同类型海洋样品汞同位素检测方法，系统归纳了其汞同位素数据，并重点阐述了海洋汞同位素分馏机制.总体上，目前海洋汞同位素数据还很有限，海洋汞循环关键过程的同位素分馏效应及潜在机理研究相对缺乏，精确源解析困难，难以对全球汞关键过程和循环通量进行准确验证和制约.未来还需要深入研究汞同位素分馏机理，进一步明确海洋中汞的来源、迁移及转化，为完善全球汞循环及精准防控海洋汞污染提供基础数据和理论支持.Abstract: Ocean, one of the most important reservoirs of mercury (Hg) on earth, plays a critical role in mediating the global Hg cycling. Recently, Hg isotope approach has shown significant advantages in studying the biogeochemical cycling of oceanic Hg, as it could be used not only to trace marine Hg sources and transformation processes, but also to reconstruct the paleoenvironment and paleoclimate. In this paper, it summarizes analytical methods for accurately measuring Hg isotopes in different marine samples, reported Hg isotopic compositions in seawater, marine sediments and biological samples of different regions worldwide, and elaborates the potential migration and transformation processes that fractionate Hg isotopes in the ocean.Overall, due to the fact that limited data are available for Hg isotopes in the ocean, and the studies on the potential mechanisms and processes fractionating Hg isotopes are still relatively scarce, the systematics of Hg in marine environment and thus the global Hg cycling model still could not be accurately established using Hg isotopes.In the future, it is still necessary to well investigate Hg isotope fractionation during potential biogeochemical processes such as the bioaccumulation and sedimentation, and to deeply decipher the source, migration and transformation of marine Hg using stable isotope approach, in order to provide basic data and theoretical support for improving the global Hg cycling and fairly preventing and controlling marine Hg pollution.
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Key words:
- seawater /
- marine sediment /
- marine biota /
- Hg stable isotope /
- Hg concentration /
- Hg speciation /
- oceanography
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图 1 不同类型海洋样品汞同位素测试装置示意图
Fig. 1. Schematic diagram of mercury isotope testing equipments for different marine samples
图 2 海水、海洋沉积物、海洋颗粒物以及海洋生物样品的δ202Hg vs. Δ199Hg
海洋沉积物据Balogh et al.（2015），Bonsignore et al.(2015, 2020)，Yin et al.(2015, 2018)，Gleason et al.（2017），Meng et al.(2019, 2020, 2021)，Sun et al.（2020b），Jung et al.（2022）；海洋生物据Gehrke et al.（2009），Point et al.（2011），Blum et al.(2013, 2020)，Balogh et al.（2015），Masbou et al.（2015），Yin et al.（2016），Madigan et al.（2018），Masbou et al.（2018），Motta et al.(2019, 2020)，Bonsignore et al.（2020），Orani et al.（2020），Sun et al.（2020a），Renedo et al.（2021），Jung et al.（2022）；海水据Štrok et al.(2014, 2015)，Meng et al.（2020），Jiskra et al.（2021），Liu et al.（2021c）；海洋颗粒物据Motta et al.（2019），Jiskra et al.（2021），Qiu et al.（2021）
Fig. 2. δ202Hg versus Δ199Hg for seawaters, marine sediments, marine particulate matters and marine biotas
图 4 实验室观察到的汞同位素分馏过程及其特征概述(Δ199Hg vs. δ202Hg)
箭头的方向指示每个反应中反应物或者产物的同位素分馏方向，箭头的颜色代表不同的反应（其中同种颜色的多个箭头则代表同一种反应在不同实验条件下得到的不同结果），具体如下：红色箭头表示液相Hg（Ⅱ）光化学还原反应物的同位素分馏特征（Bergquist and Blum, 2007；Zheng and Hintelmann, 2009；Rose et al., 2015）；绿色箭头表示液相甲基汞光化学降解反应物的同位素分馏特征（Bergquist and Blum, 2007；Rose et al., 2015）；深蓝色实线箭头表示氯自由基主导的气态Hg（0）光氧化反应物的同位素分馏特征（Sun et al., 2016）；深蓝色虚线箭头表示溴自由基主导的气态Hg（0）光氧化反应物的同位素分馏特征（Sun et al., 2016）；浅蓝色箭头表示微生物介导的Hg（Ⅱ）还原或甲基汞降解（Kritee et al., 2007, 2009），生物或者非生物甲基化（Rodríguez-González et al., 2009；Malinovsky and Vanhaecke, 2011；Jiménez-Moreno et al., 2013；Perrot et al., 2015），Hg（Ⅱ）吸附到针铁矿（Jiskra et al., 2012），Hg（Ⅱ）与巯基配位体络合（Wiederhold et al., 2010），HgS和HgO沉淀（Smith et al., 2015），Hg（0）挥发（Zheng et al., 2007）和Hg（0）扩散（Koster Van Groos et al., 2014）等一系列过程中反应物的同位素分馏特征；粉色箭头表示硫醇或腐殖酸存在下的液相Hg（0）暗氧化平衡分馏中产物的同位素分馏特征（Zheng et al., 2019）；深紫色箭头表示汞硫醇配体氙灯还原中反应物的同位素分馏特征（Zheng and Hintelmann, 2010a）；橙色箭头表示雪中Hg（Ⅱ）光化学还原中反应物的同位素分馏特征（Sherman et al., 2010）；浅紫色箭头表示硫醇或腐殖酸存在下的液相Hg（0）暗氧化动力学分馏中产物的同位素分馏特征（Zheng et al., 2019）
Fig. 4. Overview of the general patterns in mercury isotope fractionation that have been observed experimentally (Δ199Hg versus δ202Hg)
表 1 全球不同海域海水中总汞(THg)和甲基汞(MeHg)浓度数据
Table 1. THg and MeHg concentrations in seawaters from different regions of the world
海域 THg(pM) MeHg(pM) 参考文献 表层 中层 深层 总体 表层 中层 深层 总体 开阔大洋 大西洋 0.52±0.11
(n=6)0.54±0.15
(n=7)0.68±0.17
(n=9)0.59±0.17
(n=22)0.04±0.01
(n=6)0.19±0.13
(n=9)0.37±0.07
(n=9)0.23±0.16
(n=22)Jiskra et al., 2021 大西洋 1.51±0.82
(n=26)1.51±0.82
(n=26)Soerensen et al., 2013 热带太平洋 0.35±0.30
(n=70)0.90±0.29
(n=74)1.12±0.33
(n=88)0.82±0.44
(n=232)0.19±0.13
(n=56)0.41±0.32
(n=60)0.26±0.27
(n=66)0.29±0.27
(n=182)Munson et al., 2015 北冰洋中部 1.31±1.34
(n=22)0.81±0.24
(n=29)0.85±0.36
(n=32)0.96±0.76
(n=83)0.11±0.11
(n=22)0.17±0.12
(n=29)0.10±0.09
(n=32)0.12±0.10
(n=83)Heimbürger et al., 2015 南大洋 1.15±0.22
(n=10)1.35±0.39
(n=14)1.33±0.45
(n=71)0.44±0.17
(n=31)0.52±0.11
(n=19)0.29±0.21
(n=241)Cossa et al., 2011 地中海 0.86±0.09
(n=5)1.03±0.06
(n=6)0.99
(n=1)0.96±0.11
(n=12)0.17±0.10
(n=5)0.4±0.04
(n=6)0.29
(n=1)0.29±0.14
(n=12)Jiskra et al., 2021 地中海西部 2.56±1.67
(n=43)2.45±0.93
(n=17)2.20±0.17
(n=5)2.50±1.25
(n=65)Cossa et al., 1997 北大西洋 2.40±1.60
(n=27)Mason et al., 1998 北太平洋 0.64±0.26 1.10±0.31 1.15±0.86 Laurier et al., 2004 近海 中国渤海 5.80±2.74
(n=58)0.27±0.03 Wang et al., 2020 中国渤海 2.21±0.53
(n=4)Liu et al., 2021c 中国黄海 6.63±4.08
(n=23)Wang et al., 2020 中国东海 19.65±5.11
(n=351)1.00±0.55
(n=351)Liu et al., 2020 中国东海 7.22±3.08
(n=38)Wang et al., 2016 中国南海 6.15±1.73
(n=35)0.58±0.23
(n=33)Fu et al., 2010 东日本海 0.49±0.08 1.2±0.20 1.10±0.08 0.03±0.02 0.44±0.10 0.53±0.09 Yang et al., 2017 注：为便于比较，表中一些数据从原始浓度（ng/L）转换为摩尔单位（pM）. 汇总数据中，海洋分层情况为海洋表层（0~200 m）、海洋中层（200~1 000 m）、海洋深层（1 000 m以下）. 表中数据为THg±1SD或MeHg±1SD，n为样品个数. 
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表 2 全球不同海域沉积物中的THg和MeHg浓度(ng/g)
Table 2. THg and MeHg concentrations in marine sediments from different regions of the world (ng/g)
研究区域 样品量n THg范围 THg平均值 MeHg范围 MeHg平均值 MeHg/THg 参考文献 大洋海域 西北太平洋 50 19.0~158.0 77.0 Sattarova and Aksentov, 2018 西北太平洋深海 466 8.0~170.0 68.8 Aksentov and Sattarova, 2020 北大西洋 233 1.9~112.1 18.2 Kita et al., 2016 西地中海深海 86 9.0~100.0 47.1 Cossa et al., 2021 北冰洋 35 22.0~169.0 72.2 Gleason et al., 2017 地中海 56 12.0~447.3 54.1 0.09~3.71 1.09 2% Ogrinc et al., 2007 大西洋中部 22 0.54~78.8 42.3 0.01~1.24 0.62 1.1% Hollweg et al., 2010 近海 中国近海 611 1.10~398.0 35.2 Meng et al., 2014; Jeong et al., 2021 韩国近海 53 12.0~98.0 42.4 Jeong et al., 2021 东西伯利亚海 35 13.0~92.0 36.0 Aksentov et al., 2021 北大西洋边缘海 49 8.00~1 351 106.5 Vieira et al., 2021 卡塔尔海岸线 11 8.00~34.3 21.6 Hassan et al., 2019 波罗的海 91 1.20~341.8 84.0 Kwasigroch et al., 2021 南大洋边缘海 188 12.6~86.6 41.6 Zaferani et al., 2018 中国渤海和黄海 83 4.70~100.6 27.3 0.01~0.71 0.16 0.6% Yu et al., 2021 中国东海 35 53.0~157.0 79.4 0.20~1.10 0.72 1.1% 刘畅等, 2018 东北大西洋比斯开湾 24 18~973 243.2 0.07~2.03 0.70 0.4% Azaroff et al., 2019 亚得里亚海 22 680~9 950 4 350 0.47~7.85 3.48 0.08% Acquavita et al., 2012 拉普捷夫海 18 30.9~96.1 51.2 0.03~3.14 0.53 0.7% Liem-Nguyen et al., 2022 波罗的海 47 4.0~294.0 106.8 0.02~2.36 0.45 0.48% Siedlewicz et al., 2020
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表 3 全球不同海域海洋生物中的THg和MeHg浓度(ng/g)
Table 3. THg and MeHg concentrations in marine biotas from different regions of the world (ng/g)
区域 样品类型 样品数n THg范围 THg平均值 MeHg范围 MeHg平均值 MeHg/THg 参考文献 南大洋 鱼类 83 100~1 940 500 Queirós et al., 2020 南大洋* 鱼类 194/74 58~476 167 33~512 144 86% Seco et al., 2020 西北地中海 鱼类 48 210~4 420 1 162 Koenig et al., 2013 太平洋 鱼类 300 50~790 384 Meador et al., 2005 印度洋 鱼类 187 210~3 970 Kojadinovic et al., 2007 大西洋（加纳近海） 鱼类 56 4~122 Voegborlo and Akagi, 2007 东北大西洋沿岸 鱼类 706 50~7 473 988 Chouvelon et al., 2012 东北大西洋 鱼类 53 30~6 350 1 609 20~4 780 1 257 76% Romero-Romero et al., 2022 大西洋（亚述儿群岛） 鱼类 70 190~1 440 900 Afonso et al., 2007 韩国马山湾 底栖生物 399/89 6~1 290 135 1~1 290 131 65% Hilgendag et al., 2022 加拿大坎伯兰湾 底栖生物 71 20~3 170 763 McMeans et al., 2015 大西洋岸 哺乳动物 344/344 50~3 440 862 50~3 160 819 94% Wagemann et al., 1998 南大洋公海 海鸟 110 180~15 160 2 474 180~11 570 2 220 88% Renedo et al., 2020 西北冰洋 哺乳动物 69/19 400~119 320 21 080 570~3 380 1 560 14% Masbou et al., 2018 北太平洋阿拉斯加湾 哺乳动物 53/18 87~13 900 2 786 30~370 134 9% Masbou et al., 2015 中国南海 鱼类 166/96 11.9~1 772 152 6.22~358 105 69% Liu et al., 2014 中国渤海 鱼类 67 2.05~344 63.8 Liu et al., 2013 中国渤海 鱼类 55 9~270 60 7~131 25 42% Qu et al., 2022 中国东海 鱼类 148 20~660 260 10~590 180 74% Cheng et al., 2009 注：*测定的是有机汞浓度, 而非甲基汞浓度.
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表 4 海洋汞输入源和输出源的通量和同位素组成(Δ199Hg和δ202Hg)
Table 4. Fluxes and isotope compositions (Δ199Hg and δ202Hg) of Hg input sources and output sources in the ocean
类别 通量
(t/y)通量范围
(t/y)Δ199Hg
(‰)Δ199Hg±1SD
(‰)δ202Hg±1SD
(‰)数据量
(n)输入源 河流输入1, i 1 000 893~1224 ‒0.29 ‒0.29±0.12 ‒1.82±0.39 156 热液输入2, ⅱ 100 < 600 0.00 0.00±0.00 0.00±0.00 大气Hg(Ⅱ)沉降2, ⅲ 1 500 912~1 900 0.41 0.41±0.34 ‒0.43±0.77 172 大气Hg(0)沉降2, ⅲ 2 200 1 900~2 888 ‒0.19 ‒0.19±0.10 0.37±0.65 220 F输入 4 800 F输入×Δ199Hg输入 ‒93 输出源 埋藏于沿海沉积物1, ⅳ 730 410~1 100 0.06 0.06±0.11 ‒1.19±0.43 546 埋藏于深海沉积物2, ⅴ 600 200~600 0.10 0.10±0.10 ‒0.99±0.39 92 埋藏于海沟3, ⅵ 164 101~227 0.24 0.24±0.07 ‒1.19±0.43 19 海洋Hg(0)逃逸2, ⅶ 3 400 2 900~4 000 ‒0.07 ‒0.07±0.10 0.44±0.02 61 F输出 4 894 F输出×Δ199Hg输出 ‒94.84 注：通量数据：1据 Liu et al. (2021b) ；2据Outridge et al. (2018) ；3据Liu et al. (2021a) . 同位素数据：i据Yin et al. (2018) ；ⅱ据Smith et al. (2008) ,Sherman et al. (2009) 和Kim et al.(2022) ；ⅲ据Jiskra et al. (2021) ；ⅳ据Balogh et al.(2015) ,Bonsignore et al.(2015 , 2020),Yin et al.(2015 , 2018),Gleason et al.(2017) ,Meng et al.(2019 , 2020, 2021),Sun et al.(2020b) 和Jung et al.(2022) ；ⅴ据Jiskra et al.(2021) ；ⅵ据Liu et al.(2021a) ；ⅶ据Zheng et al.(2007) .
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