수은 안정동위원소를 활용한 환경과학수사의 접근법 = Applications of Mercury Stable Isotopes in Environmental Forensics

다국어 초록 (Multilingual Abstract)

Mercury is a globally distributed toxic trace metal, which can travel long distances in the atmosphere and bioaccumulate to elevated levels in ecosystem food webs. Since 2013, various parts of the mercury life cycle, including the production, use, emissions, releases, as well as the environmental and ecosystem fate, have been governed via the global treaty on mercury, the Minamata Convention of Mercury. The convention also calls attention to the application of mercury stable isotopes for distinguishing between various mercury sources in environmental media and for identifying sources, which require targeted risk management. Here, we introduce ways in which mercury stable isotopes can be applied in the field of environmental forensics to identify sources responsible for local contamination and global cycling that require international governance. This review is divided into: 1) the general overview on the mercury speciation and cycling, 2) the nomenclature of mercury stable isotope systems, and 3) the introduction of case studies that have successfully utilized mercury isotopes to interpret legacy and recent mercury sources in atmospheric and freshwater environments. We conclude the review by making specific recommendations as to how mercury stable isotopes can be better utilized in the field of local and global environmental forensics. These recommendations include the development of comprehensive anthropogenic mercury source inventories and isotopic-based evidence on the transboundary transport of mercury.

국문 초록 (Abstract)

최근 기술의 발전에 따라 환경에서 수은을 비롯한 다양한 오염원의 발견 및 정화 조치를 위한 환경과학수사의 중요성이 강조되고 있다. 특히 수은은 자연환경에서 먹이사슬을 통해 축적되며, 체내에 잔류하여 강한 독성을 유발하는 중금속으로써 수은으로 인한 환경 보건적 위해성에 대한 우려가 높아 미나마타 국제 협약(Minamata Convention on Mercury)을 통해 수은의 생산 및 수출이 관리되고 있다. 따라서 수은 오염지역에 대한 관리와 오염원의 선별, 오염원에 특화된 정화 법 설정과 같은 판단의 증거로써, 환경과학수사의 역할이 더욱 중요시 될 뿐만 아니라 수은 안정동위원소를 활용한 환경과학수사에 대한 관심이 더욱 높아지고 있다. 본 논문에서는 수은의 화학종 및 순환에 대한 개요, 안정동위원소 비의 표기법과 오염원 추적법을 비롯하여 오염원별 기여도 산정에 관한 전반적인 지식을 제공하였다. 또한 문헌 고찰을 통해 선행 연구에서 도출한 배출원별 수은 안정동위원소 비의 분포 경향을 매체에 따라 정리하였다. 더 나아가, 국내외 수은 안정동위원소를 이용한 환경과학수사 사례를 소개함으로써 수은 안정동위원소의 활용 가치를 확인하고 미나마타 국제협약 이행과 더불어 향후 보다 발전된 환경과학수사를 수행하기 위하여 개선되어야 할 한계점 및 앞으로의 연구 방향을 총체적으로 제안하였다.

참고문헌 (Reference)

1 박광수 ; 김혁 ; 유석민 ; 노샘 ; 박유미 ; 석광설 ; 김민섭 ; 윤숙희 ; 김영희, "안정동위원소를 이용한 이동오염원에 의한 대기 중 NO2의 거동특성 연구" 한국분석과학회 32 (32): 17-23, 2019

2 김지영 ; 김명진 ; 유은진 ; 이강현 ; 이경석 ; 이원석 ; 최종우 ; 권오상, "다중 검출 유도결합 플라즈마 질량분석기를 이용한 납 및 카드뮴안정동위원소비 분석의 질량 편향 보정방법 비교" 한국환경분석학회 17 (17): 173-181, 2014

3 문종한 ; 주영지 ; 강정옥 ; 심민섭, "다검출기 유도결합 플라즈마 질량분석기를 이용한 미량시료의 황 동위원소 분석" 대한지질학회 57 (57): 99-108, 2021

4 X. Wang, "Using mercury isotopes to understand mercury accumulation in the montane forest floor of the Eastern Tibetan Plateau" 51 (51): 801-809, 2017

5 R. F. Lepak, "Use of stable isotope signatures to determine mercury sources in the Great Lakes" 2 (2): 335-341, 2015

6 C. A. Cooke, "Use and legacy of mercury in the Andes, Environ" 47 (47): 4181-4188, 2013

7 S. J. Balogh, "Tracking the fate of mercury in the fish and bottom sediments of Minamata Bay, Japan, using stable mercury isotopes" 49 (49): 5399-5406, 2015

8 M. S. Choi, "Tracing the sources of pollutants in aquatic environment using heavy metal stable isotopes (II)" National Institute of Environmental Research 2013

9 V. Perrot, "Tracing sources and bioaccumulation of mercury in fish of Lake Baikal- Angara River using Hg isotopic composition" 44 (44): 8030-8037, 2010

10 X. Feng, "Tracing mercury contamination sources in sediments using mercury isotope compositions" 44 (44): 3363-3368, 2010

11 D. Foucher, "Tracing mercury contamination from the Idrija mining region (Slovenia) to the Gulf of Trieste using Hg isotope ratio measurements" 43 (43): 33-39, 2009

12 M. X. Bailon, "Total mercury, methyl mercury, and heavy metal concentrations in Hyeongsan River and its tributaries in Pohang city, South Korea" 190 (190): 1-16, 2018

13 D. G. Streets, "Total mercury released to the environment by human activities" 51 (51): 5969-5977, 2017

14 W. F. Fitzgerald, "The case for atmospheric mercury contamination in remote areas" 32 (32): 1-7, 1998

15 World Health Organization, "Ten Chemicals of Major Public Health Concern"

16 AMAP, "Technical Background Report for the Global Mercury Assessment 2018" Arctic Monitoring and Assessment Programme, Oslo, Norway/UN Environment Programme, Chemicals and Health Branch 2019

17 J. Nilsen, "Status of the Environment Report" Hudson Bay Mining and Smelting Co. Ltd 2003

18 R. Yin, "Stable mercury isotope variation in rice plants (Oryza sativa L.) from the Wanshan mercury mining district, SW China" 47 (47): 2238-2245, 2013

19 R. S. Smith, "Stable Hg isotope signatures in creek sediments impacted by a former Hg mine" 49 (49): 767-776, 2015

20 P. Rodríguez-González, "Species-specific stable isotope fractionation of mercury during Hg (II) methylation by an anaerobic bacteria (Desulfobulbus propionicus) under dark conditions" 43 (43): 9183-9188, 2009

21 M. Jiménez-Moreno, "Sources and fate of mercury pollution in Almadén mining district (Spain):Evidences from mercury isotopic compositions in sediments and lichens" 147 : 430-438, 2016

22 M. Jiskra, "Source tracing of natural organic matter bound mercury in boreal forest runoffwith mercury stable isotopes" 19 (19): 1235-1248, 2017

23 M. Jiskra, "Solution speciation controls mercury isotope fractionation of Hg (II) sorption to goethite" 46 (46): 6654-6662, 2012

24 M. Jiskra, "Solution speciation controls mercury isotope fractionation of Hg (II) sorption to goethite" 46 (46): 6654-6662, 2012

25 J. E. Sonke, "Sedimentary mercury stable isotope records of atmospheric and riverine pollution from two major European heavy metal refineries" 279 (279): 90-100, 2010

26 J. Rolison, "Salters, Isotopic composition of species-specific atmospheric Hg in a coastal environment"

27 R. P. Mason, "Role of the ocean in the global mercury cycle" 16 (16): 1093-, 2002

28 J. D. Blum, "Reporting of variations in the natural isotopic composition of mercury" 388 (388): 353-359, 2007

29 J. D. Blum, "Recent developments in mercury stable isotope analysis" 82 (82): 733-757, 2017

30 G. E. Woerndle, "New insights on ecosystem mercury cycling revealed by stable isotopes of mercury in water flowing from a headwater peatland catchment" 52 (52): 1854-1861, 2018

31 Ministry of Environment, "Ministry of Environment"

32 M. Harada, "Minamata disease: methylmercury poisoning in Japan caused by environmental pollution" 25 (25): 1-24, 1995

33 J. W. Choi, "Method development for tracing mercury sources and route of long-range transport using stable isotopes" National Institute of Environmental Research 2015

34 I. G. Petrisor, "Mercury-hazards and forensic perspectives" 7 : 289-292, 2006

35 S. Y. Kwon, "Mercury stable isotopes for monitoring the effectiveness of the Minamata Convention on Mercury" 203 : 103111-, 2020

36 Y. H. Kim, "Mercury stable isotope study of source and exposure pathways of mercury from air to watershed (II)" National Institute of Environmental Research 2018

37 R. Sun, "Mercury stable isotope fractionation in six utility boilers of two large coal-fired power plants" 336 : 103-111, 2013

38 K. Kritee, "Mercury stable isotope fractionation during reduction of Hg (II) to Hg (0) by mercury resistant microorganisms" 41 (41): 1889-1895, 2007

39 R. Yin, "Mercury speciation and mercury isotope fractionation during ore roasting process and their implication to source identification of downstream sediment in the Wanshan mercury mining area, SW China" 336 (336): 2013

40 J. D. Blum, "Mercury isotopes in earth and environmental sciences" 42 : 249-269, 2014

41 J. D. Demers, "Mercury isotopes in a forested ecosystem: Implications for air‐surface exchange dynamics and the global mercury cycle" 27 (27): 222-238, 2013

42 R. Yin, "Mercury isotope variations between bioavailable mercury fractions and total mercury in mercury contaminated soil in Wanshan Mercury Mine, SW China" 336 : 80-86, 2013

43 S. Y. Kwon, "Mercury isotope study of sources and exposure pathways of methylmercury in estuarine food webs in the Northeastern US" 48 (48): 10089-10097, 2014

44 J. G. Wiederhold, "Mercury isotope signatures in contaminated sediments as a tracer for local industrial pollution sources" 49 (49): 177-185, 2015

45 D. Foucher, "Mercury isotope fractionation in waters and sediments of the Murray Brook mine watershed (New Brunswick, Canada): Tracing mercury contamination and transformation" 336 : 87-95, 2013

46 J. E. Gray, "Mercury isotope fractionation during ore retorting in the Almadén mining district, Spain" 357 : 150-157, 2013

47 N. Estrade, "Mercury isotope fractionation during liquid-vapor evaporation experiments" 73 (73): 2693-2711, 2009

48 W. Zheng, "Mercury isotope compositions across North American forests" 30 (30): 1475-1492, 2016

49 L. C. Motta, "Mercury cycling in the North Pacific Subtropical Gyre as revealed by mercury stable isotope ratios" 33 (33): 777-794, 2019

50 J. Ma, "Mercury concentrations and mercury isotope composition in lake sediment cores from the vicinity of a metal smelting facility in Flin Flon, Manitoba" 336 : 96-102, 2013

51 C. T. Driscoll, "Mercury as a global pollutant: sources, pathways, and effects" 47 (47): 4967-4983, 2013

52 L. S. Sherman, "Mass-independent fractionation of mercury isotopes in Arctic snow driven by sunlight" 3 (3): 173-177, 2010

53 B. A. Bergquist, "Mass-dependent and-independent fractionation of Hg isotopes by photoreduction in aquatic systems" 318 (318): 417-420, 2007

54 W. F. Fitzgerald, "Marine biogeochemical cycling of mercury" 107 (107): 641-662, 2007

55 S. Y. Kwon, "Isotopic study of mercury sources and transfer between a freshwater lake and adjacent forest food web" 532 : 220-229, 2015

56 P. M. Donovan, "Isotopic composition of inorganic mercury and methylmercury downstream of a historical gold mining region" 50 (50): 1691-1702, 2016

57 B. Yu, "Isotopic composition of atmospheric mercury in China: new evidence for sources and transformation processes in air and in vegetation" 50 (50): 9262-9269, 2016

58 S. Noh, "Isotopic composition of atmospheric mercury at urban and rural sites in Korea: sources and transport pathways" 96 : 2019

59 L. E. Gratz, "Isotopic composition and fractionation of mercury in Great Lakes precipitation and ambient air" 44 (44): 7764-7770, 2010

60 S. J. Washburn, "Isotopic characterization of mercury downstream of historic industrial contamination in the South River, Virginia" 51 (51): 10965-10973, 2017

61 S. Jung, "Isotope investigation of mercury sources in a creek impacted by multiple anthropogenic activities" 282 : 130947-, 2021

62 W. Zheng, "Isotope fractionation of mercury during its photochemical reduction by low-molecular-weight organic compounds" 114 (114): 4246-4253, 2010

63 L. S. Sherman, "Investigation of local mercury deposition from a coal-fired power plant using mercury isotopes" 46 (46): 382-390, 2012

64 B. L., Murphy, "Introduction to environmental forensics" Elsevier 2014

65 J. W. Choi, "Improvement of precision and accuracy in hazardous heavy metal stable isotopic analysis by MC-ICP-MS (II)" National Institute of Environmental Research 2013

66 P. M. Donovan, "Identification of multiple mercury sources to stream sediments near Oak Ridge, TN, USA" 48 (48): 3666-3674, 2014

67 D. Foucher, "High-precision measurement of mercury isotope ratios in sediments using cold-vapor generation multi-collector inductively coupled plasma mass spectrometry" 384 (384): 1470-1478, 2006

68 N. Pirrone, "Global mercury emissions to the atmosphere from anthropogenic and natural sources" 10 (10): 5951-5964, 2010

69 N. E. Selin, "Global biogeochemical cycling of mercury: a review" 34 : 43-63, 2009

70 E. G. Pacyna, "Global anthropogenic mercury emission inventory for 2000" 40 (40): 4048-4063, 2006

71 D. G. Streets, "Global and regional trends in mercury emissions and concentrations, 2010-2015" 201 : 417-427, 2015

72 UN-Environment, "Global Mercury Assessment 2018"

73 S. Huang, "Fractionation of mercury stable isotopes during coal combustion and seawater flue gas desulfurization" 76 : 159-167, 2017

74 R. F. Lepak, "Factors affecting mercury stable isotopic distribution in piscivorous fish of the Laurentian Great Lakes" 52 (52): 2768-2776, 2018

75 B. G. Marshall, "Evidence of transboundary mercury and other pollutants in the Puyango-Tumbes River basin" 20 (20): 632-641, 2018

76 S. Ghosh, "Estimation of nuclear volume dependent fractionation of mercury isotopes in equilibrium liquid–vapor evaporation experiments" 336 : 5-12, 2013

77 J. G. Wiederhold, "Equilibrium mercury isotope fractionation between dissolved Hg (II) species and thiol-bound Hg" 44 (44): 4191-4197, 2010

78 G. Bartov, "Environmental impacts of the Tennessee Valley Authority Kingston coal ash spill. 1. Source apportionment using mercury stable isotopes" 47 (47): 2092-2099, 2013

79 S. Jung, "Elucidating sources of mercury in the west coast of Korea and the Chinese marginal seas using mercury stable isotopes" 814 : 152598-, 2022

80 X. Fu, "Domestic and transboundary sources of atmospheric particulate bound mercury in remote areas of China: evidence from mercury isotopes, Environ" 53 (53): 1947-1957, 2019

81 N. E. Selin, "Chemical cycling and deposition of atmospheric mercury: Global constraints from observations" 112 (112): 2007

82 CCME, "Canada-wide standards for mercury emissions, Canadian Council of Ministers of the Environment, endorsed by CCME Council of Ministers"

83 K. Kritee, "Blum, Mass dependent stable isotope fractionation of mercury during mer mediated microbial degradation of monomethylmercury" 73 (73): 1285-1296, 2009

84 W. H. Schroeder, "Atmospheric mercury-an overview" 32 (32): 809-822, 1998

85 M. Enrico, "Atmospheric mercury transfer to peat bogs dominated by gaseous elemental mercury dry deposition" 50 (50): 2405-2412, 2016

86 A. Rua-Ibarz, "Assessment of Hg pollution released from a WWII submarine wreck (U-864) by Hg isotopic analysis of sediments and Cancer pagurus tissues" 50 (50): 10361-10369, 2016

87 D. G. Streets, "Anthropogenic mercury emissions in China" 39 (39): 7789-7806, 2005

88 R. P. Philp, "An overview of environmental forensics" 12 (12): 363-374, 2014

89 P. M. Donovan, "An isotopic record of mercury in San Francisco Bay sediment" 349 : 87-98, 2013

90 G. Schudel, "An investigation of mercury sources in the Puyango-Tumbes River: Using stable Hg isotopes to characterize transboundary Hg pollution" 202 : 777-787, 2018

91 M. Meng, "An integrated model for input and migration of mercury in Chinese coastal sediments" 53 (53): 2460-2471, 2019

92 G. Liu, "Adsorption of mercury on solids in the aquatic environment" 1 : 367-387, 2012

93 Y. H. Kim, "A study on mercury deposition monitoring on the background sites for effective evaluation of the Minamata Convention (II)" National Institute of Environmental Research 2016

94 J. M. Pacyna, "1995 global anthropogenic emissions of mercury" 37 : 109-117, 2003