황해 연안 갯벌 퇴적환경내 유기탄소의 시공간 분포 및 거동특성 규명

학위논문(박사) -- 서울대학교대학원 : 자연과학대학 지구환경과학부, 2022. 8. 김종성.전 세계적으로 염습지, 맹그로브, 잘피를 포함한 블루카본 생태계는 지구온난화가 가속화되는 상황에서 높은 이산화탄소 흡수율로 기후 변화를 완화하는데 중요한 역할을 한다. 그러나 기존의 블루카본 생태계의 이산화탄소 흡수 능력에 대해 많은 연구가 진행되었으나, 잠재적 탄소흡수원인 갯벌의 탄소 저장 능력과 그 조절 요인에 대한 연구는 미비한 실정이다. 이에 본 연구에서는 황해 갯벌 퇴적물내 유기탄소의 시공간분포와 거동요인에 미치는 영향을 평가하였다. 첫째로, 한국 조간대 표층퇴적물내 총유기탄소의 시공간적 분포와 거동을 평가하였다. 조간대 환경의 대표성과 객관적 비교를 담보하기 위해 전형적 자연 갯벌 4개소와 닫힌 하구 1개소를 대상으로 2018년 1월부터 12월까지 월별 조사를 수행하였다. 조사 및 분석결과, 총 유기탄소 함량은 퇴적물 입자크기(입도)를 대변하는 니질 함량에 따라 결정됨이 확인되었다. 가로림만과 순천만 퇴적물은 저서미세조류 대발생에 기인하여 겨울철 총 유기탄소 함량이 높았고, 특히 δ13C 값이 크게 증가했다. 반면 낙동강 하구 퇴적물은 장마철(9–10월)에 육상으로부터의 담수방류 영향으로 인해 δ13C와 δ15N 값이 감소하는 것이 확인되었다. 둘째로, 한국 전 연안 갯벌 퇴적물내 유기탄소 저장량과 유기탄소 침적률의 산정을 위해 현장조사 자료와 원격탐사 기법을 활용하였다. 조사지역은 동서남해 7개 시도(경기, 충남, 전북, 전남, 경남, 경북, 강원) 내 21개 지역이었으며, 2017년부터 2020년까지 코어퇴적물을 분석하였고, 원격 탐사기법을 통해 갯벌의 퇴적물 성상과 면적을 산정하였다. 염생식물이 서식하는 염습지에서는 식물의 일차생산을 통한 높은 탄소고정 능력으로 인해, 비식생 갯벌보다 상대적으로 높은 유기탄소 저장량을 보였다. 현장조사 자료와 원격탐사 기법을 통해, 국가 수준에서 한국 전 연안의 조간대 갯벌의 총 유기탄소 저장량 및 연간 유기탄소 침적률을 산정하였다. 셋째로, 외래식물 갯끈풀과 토착식물 갈대, 칠면초가 유기탄소 증가에 미치는 영향을 비교하기 위해 염생식물 종별 유기탄소 저장량 증가율을 분석하였다. 중국 7개지역과 한국 12개지역을 대상으로, 각 지역의 염생식물이 서식하는 염습지와 비식생 갯벌에서 조사를 실시하였다. 외래식물 갯끈풀이 우점하는 중국 염습지가 토착식물 갈대와 칠면초가 우점하는 한국 염습지보다 높은 유기탄소 저장량을 보였다. 동일 기간 동안 갯끈풀의 유기탄소 저장량 증가율은 칠면초와 갈대에 비해 높았으며, 이는 상대적으로 높은 일차생산량과 지하부 뿌리 생물량으로 인한 것으로 나타났다. 또한 갯끈풀 서식지는 비식생 갯벌과 갈대 서식지에 비해 온실가스 배출, 대형저서동물 먹이망, 퇴적물 안정도, 탄소침적의 관점에서 이점이 있는 것으로 확인되었다. 끝으로, 대규모 현장조사를 통해 황해 전 연안 갯벌의 유기탄소 저장량과 유기탄소 침적률을 산정하였다. 조사지역은 중국 5개 시도(랴오닝성, 허베이성, 톈진시, 산둥성, 장쑤성)내 19개 지역, 한국 5개 시도(경기, 충남, 전북, 전남, 경남)내 18개 지역에서 코어퇴적물을 채집하였다. 분석결과, 양식장, 도시 및 산업단지로부터 강을 통한 유기물질의 유입이 유기탄소 침적에 기여하는 것이 확인되었다. 황해 갯벌 퇴적물내 유기탄소 함량은 퇴적물 입도와 염생식물의 유무에 따라 결정되는 것으로 나타났다. 단위면적당 유기탄소 저장량과 갯벌 면적자료를 기반으로 황해 전 연안 갯벌의 총 유기탄소 저장량 21–171 Tg C과 연간 유기탄소 침적률 0.08–0.61 Tg C yr-1; 0.29–2.24 Tg CO2 eq. yr-1을 추정하였다. 기존의 블루카본 생태계와 비교하였을 때 갯벌은 상대적은 낮은 단위면적당 유기탄소 저장량과 침적률을 보이나, 전 세계적으로 광활한 면적과 해당 서식지의 일차생산자인 저서미세조류를 고려할 때 갯벌도 또한 중요한 탄소흡수원임을 시사한다. 이상의 연구결과를 종합 요약하면, 황해 갯벌 퇴적물내 유기탄소 분포는 퇴적물 입도와 식생의 유무에 의해 가장 많은 영향을 받으며, 유기탄소 기원은 염생식물 종과 육상-해양기원 유기물 유입에 따라 변화되는 것이 확인되었다. 결과적으로, 본 연구는 황해 갯벌의 블루카본 잠재성과 이에 영향을 미치는 생태학적 특성에 대한 정보를 제공하며, 향후 황해 갯벌 퇴적물내 탄소순환 연구에 대한 중요한 기초자료로 활용될 수 있음을 시사한다.Recently, blue carbon ecosystems (BCEs), including salt marshes, mangrove forests, and seagrass meadows, have been highlighted for their capacity to fix high quantities of carbon under global warming. Although these conventional BCEs are widely studied for their role as highly efficient CO2 sinks, holistic data analysis of carbon sink capacity and its controlling factors remain limited in the tidal flat ecosystems of the Yellow Sea. Thus, the current study evaluated the spatiotemporal distribution and fate of sedimentary organic carbon of tidal flat ecosystems in the Yellow Sea. Sedimentary organic carbon in the surface sediments of typical intertidal areas were investigated to address year-round monthly distributions and site-specific sources. Target areas included four natural tidal flats (Ganghwa, Garolim, Sinan, and Suncheon) and one artificially closed estuary (Nakdong River) in South Korea during 2018. Among the parameters monitored, mud content was a key factor controlling organic matter content, across varying habitats, with significant positive correlations to total organic carbon (TOC). Elevated TOC content and heavier carbon stable isotope ratios (δ13C) in the sediments of Garolim and Suncheon from February to April of 2018 reflected microphybenthos blooms during winter, indicating a primary influence of marine sources. In comparison, δ13C and δ15N were depleted in the sediments of Nakdong River estuary during the flood season (September–October), indicating the direct influence of terrestrial organic input through freshwater discharge. To estimate current organic carbon stocks and sequestration rates in the coastal areas of the West Sea, South Sea, and East Sea of South Korea, field surveys were conducted over 4 years combined with remote sensing technology were conducted encompassing entire intertidal areas. Twenty-one intertidal flats were targeted across seven provinces (Gyeonggi, Chungnam, Jeonbuk, Jeonnam, Gyeongnam, Gyeongbuk, and Gangwon). Organic carbon stocks measured in salt marshes (i.e., upper intertidal zone) reflected the high carbon fixation capacity of halophytes through primary production. The texture of different sediments was classified based on remotely sensed imagery, and was confirmed to be closely correlated with field-based classification data. Using field and remote sensing results, total organic carbon stocks and sequestration rates were estimated in the tidal flats of South Korea. This investigation was conducted to address the effects of an invasive halophyte (i.e., Spartina alterniflora) on sedimentary organic carbon compared to native halophyte habitats (i.e., Suaeda japonica and Phragmites australis) in South Korea and China. Out of the two countries, salt marshes in China tended to have higher organic carbon stocks compared to those in Korea, which was attributed to different rates of increase in TOC by halophyte species. Spartina alterniflora contributed to higher carbon accumulation rates in sediments (3.4 times), through higher primary production and greater root biomass, compared to S. japonica (2.5 times) and P. australis (2.4 times) over the same period. In addition, compared to P. australis and bare tidal flats, S. alterniflora had advantages with respect to greenhouse gas emissions, the food web, sediment erodibility, and carbon burial. Finally, a large-scale investigation was conducted to demonstrate the distribution of total organic carbon stocks and sequestration rates of coastal sediments along the Yellow Sea. Riverine inputs of anthropogenic organic matter from aquaculture, municipal, and industrial areas contributed to the burial of sedimentary organic carbon. Out of the evaluated environmental parameters, sediment mud contents and halophytes were confirmed as key factors affecting organic carbon levels in coastal sediment. Based on the assimilated data, total organic carbon stocks (21–171 Tg C) and sequestration rates (0.08–0.61 Tg C yr-1; 0.29–2.24 Tg CO2 eq. yr-1) were evaluated in the Yellow Sea. Of note, tidal flats had relatively lower carbon stocks due to having lower net primary production (NPP) compared to conventional BCEs. Nevertheless, given the extensive areal coverage and microphytobenthos (MPB), tidal flats could be significant carbon sinks, and also terminal reservoirs of detritus organic matter from adjacent vegetated coastal ecosystems. Overall, the distribution of sedimentary organic carbon varied in the sediment mud content and vegetation of tidal flats in the Yellow Sea. Furthermore, the sources affecting the differences in its origin included halophyte species and terrestrial-marine inputs. In conclusion, the present study provides a relatively large-scale baseline on the carbon dynamics of coastal sediments along the Yellow Sea, contributing to the global database of “Blue Carbon” science.CHAPTER. 1. Introduction 1 1.1. Backgrounds 2 1.2. Objectives 8 CHAPTER. 2. Natural and anthropogenic signatures on sedimentary organic matters across varying intertidal habitats in the Korean waters 11 2.1. Introduction 12 2.2. Materials and methods 15 2.2.1. Study area 15 2.2.2. Sampling and laboratory analyses 18 2.2.3. Data analysis 21 2.3. Results and discussion 22 2.3.1. Spatiotemporal distributions of sedimentary organic matter 22 2.3.2. Effects of the mud contents on sedimentary TOC and TN 29 2.3.3. Effects of benthic microalgae on sedimentary TOC and TN 32 2.3.4. Site-specific variabilities in sources of sedimentary organic matters 36 2.3.5. Factors affecting complex dynamics of sedimentary organic matter 39 CHAPTER. 3. The first national scale evaluation of organic carbon stocks and sequestration rates of coastal sediments along the West Sea, South Sea, and East Sea of South Korea 42 3.1. Introduction 43 3.2. Materials and methods 46 3.2.1. Study area 46 3.2.2. Tidal flat delineation using remote sensing 58 3.2.3. Validation of sediment textural types using remote sensing 62 3.2.4. Sampling and laboratory analyses 63 3.2.5. Calculation of organic carbon stock 69 3.2.6. Calculation of organic carbon sequestration rate 73 3.2.7. Statistical analyses 74 3.3. Results and discussion 75 3.3.1. Spatiotemporal distribution of organic carbon stocks per unit area 75 3.3.2. Environmental factors affecting the complex dynamics of sedimentary organic carbon stocks 78 3.3.3. Effects of mud content and vegetation on sedimentary TOC 81 3.3.4. Validation of tidal flat areas and sediment textural types using remote sensing classification 86 3.3.5. Estimation of organic carbon stocks and sequestration rates in South Korea 90 CHAPTER. 4. The effect of exotic S. alterniflora invasion on sedimentary organic carbon across the coastal areas of the Yellow Sea 99 4.1. Introduction 100 4.2. Materials and methods 103 4.2.1. Data packages 103 4.2.2. Air temperature anomaly 105 4.2.3. Sedimentary organic carbon stocks per unit area 106 4.2.4. Benthic community after Spartina alterniflora eradication 109 4.2.5. CO2 and CH4 emissions 110 4.2.6. Relatively contribution of primary diet 111 4.2.7. Statistical analysis 112 4.3. Results and discussion 113 4.3.1. Elevated temperature affecting the spread of Spartina alterniflora in the Yellow Sea 113 4.3.2. Effects of Spartina alterniflora invasion on sedimentary organic carbon 117 4.3.3. Effect of eradication on Spartina alterniflora and macrobenthos community 124 4.3.4. Comparision of ecological functions between bare tidal flat, native Phragmites australis, and invasive Spartina alterniflora 127 CHAPTER. 5. Spatial variation of sedimentary organic carbon in the coastal areas of the Yellow Sea 135 5.1. Introduction 136 5.2. Materials and methods 138 5.2.1. Study area 138 5.2.2. Sampling and laboratory analyses 140 5.2.3. Data analyses 146 5.3. Results and discussion 147 5.3.1. Spatial distribution of organic carbon stocks per unit area 147 5.3.2. Environmental factors affecting the complex dynamics of sedimentary organic carbon stocks 149 5.3.3. Halophyte species-specific variability in the sources of sedimentary organic matter 151 5.3.4. Organic carbon stocks and carbon sequestration rates in the coastal areas of the Yellow Sea 153 CHAPTER. 6. Conclusions 157 6.1. Summary 158 6.2. Environmental implications and limitations 163 6.3. Future research directions 166 BIBLIOGRAPHY 169 ABSTRACT (IN KOREAN) 186박

황해 연안지역 퇴적물 내 잔류성독성물질의 시공간 분포 및 대형저서동물 군집에 대한 영향

학위논문 (박사) -- 서울대학교 대학원 : 자연과학대학 지구환경과학부, 2021. 2. 김종성.Sediments in the coastal areas of the Yellow Sea have been contaminated by persistent toxic substances (PTSs) over the last 30 years. This study evaluated the spatiotemporal distribution of classic and emerging PTSs in sediment and their impact on the macrofaunal community in the coastal areas of the Yellow Sea. PTSs included polycyclic aromatic hydrocarbons (PAHs), alkylphenols (APs), polychlorinated biphenyls (PCBs), metals, emerging PTS (styrene oligomers (SOs), emerging-PAHs (E-PAHs), and halogenated-PAHs (Hl-PAHs). The distribution of PTSs varied in relation to chemical and station, with that of PAHs being generally high. PAH concentrations in Nantong, Huludao, and Qinhuangdao (China) present potential risks to aquatic organisms. Over the last decade, PAH contamination has declined in Korea, while that of PAHs in general has increased in China. Thus, PTS contamination is likely ongoing with high potential risk, especially in China. Historical records of classic and emerging PTSs over the 100 years showed that contamination of both classic and emerging PTSs was high from the 1970s to 1990s. Fluxes of classic and emerging PTSs showed a similar trend to concentrations of PTSs; however, since the 2000s, the rate of decrease has been relatively low, indicating the continuous input of PTSs to the Yellow Sea. The impact of PTSs has been low, despite the relatively high concentrations of classic and emerging PTSs in hotspots. The macrofaunal community inhabiting the upper intertidal zone, estuaries, and coastal areas was more impacted by salinity, sediment grain size, and chlorophyll-a, rather than PTSs. However, the great potential ecological risk of PTSs was found in some areas, which suggested that continuous monitoring is required. Overall, the contamination by sedimentary PTSs in the coastal areas of the Yellow Sea has decreased compared to the past; however, contamination remains high in certain areas. The impacts of PTSs on the macrofaunal community were weak, despite the high PTS concentrations in some areas. In conclusion, This study provides baseline information on PTS contamination and ecological impacts, suggesting that selecting priorities for pollution management and implementation of pollution reduction policies in Korea and China are necessary.황해 연안지역 퇴적물은 지난 30여년간 잔류성오염물질에 의해 오염되어 왔다. 본 연구에서는 최초로 황해 전체 연안지역 퇴적물 내 기존 (다환방향족탄화수소, 알킬페놀, 폴리염화비페닐, 중금속) 및 신규 (스티렌올리고머와 아미노, 알킬 또는 할로겐으로 치환된 다환방향족탄화수소) 잔류성오염물질의 시공간분포와 대형저서동물 군집에 미치는 영향을 평가하였다. 잔류성오염물질의 분포는 화합물과 정점에 따라 다양하게 나타났고, 다환방향족탄화수소의 농도가 상대적으로 높게 나타났다. 특히, 중국의 후루다오, 친황다오, 난통지역 내 다환방향족탄화수소의 농도는 수 생태계에 잠재적 위해성을 가지는 것으로 확인되었다. 지난 10여년간 한국에서 다환방향족탄화수소 농도는 감소하였지만, 중국에서는 유입원의 변화와 함께 최근 더 높은 농도가 검출되었다. 연대가 측정된 주상퇴적물 분석한 결과, 지난 100여년간 기존 및 신규 잔류성오염물질이 존재하였고, 1970년대부터 1990년대에 가장 높은 농도로 분포한 것이 확인되었다. 잔류성오염물질의 유입량은 1990년대 이후에도 상대적으로 높게 나타나, 황해 연안지역의 오염이 지속되고 있음을 시사하였다. 잔류성오염물질에 의한 영향은 농도나 지역에 관계없이 상대적으로 작다는 것이 확인되었다. 상부조간대, 하구, 연안 지역에 서식하는 대형저서동물 군집은 환경요인 중 잔류성오염물질 보다 염분, 퇴적물 입자크기에 가장 영향을 받았다. 하지만 일부 지역에서 잔류성오염물질의 잠재적 위험도가 높게 나타나 지속적인 관찰이 요구된다. 이상의 연구결과를 종합 요약하면, 첫째, 황해 연안 퇴적물내 잔류성오염물질은 과거에 비해 최근 감소했으나, 일부 지역에서 여전히 높은 오염도를 보였고, 둘째, 대형저서동물의 군집구조는 잔류성오염물질보다는 서식지 내 물리 화학적 환경요인에 의해 더 영향을 받는 것으로 나타났다. 결과적으로, 본 연구는 황해 연안 지역의 오염과 생태학적 영향에 대한 정보를 제공하며, 향후 한국과 중국의 오염관리를 위한 우선순위 선택 및 오염감소 정책 실행이 필요함을 시사한다.ABSTRACT I TABLE OF CONTENTS II LIST OF ABBREVIATIONS VI LIST OF TABLES IX LIST OF FIGURES XII CHAPTER. 1. Introduction 1 1.1. Background 2 1.2. Objectives 10 CHAPTER. 2. Distributions Of Persistent Organic Contaminants In Sediments And Their Potential Impact On Macrobenthic Faunal Community Of The Geum River Estuary And Saemangeum Coast, Korea 12 2.1. Introduction 13 2.2. Materials and Methods 15 2.2.1. Sampling strategy 15 2.2.2. Analyses of PTSs and carbon stable isotope ratio 15 2.2.3. Macrobenthic fauna analysis 19 2.2.4. Quality assurance and quality control 19 2.2.5. Data analysis 19 2.3. Results and Discussion 21 2.3.1. Spatial distribution of persistent organic contaminants 21 2.3.2. Composition and sources of persistent organic contaminants 26 2.3.3. Sources and distribution of organic matter 31 2.3.4. Association of POCs contamination to the macrofaunal community 35 2.4. Summary 42 CHAPTER. 3. Macrozoobenthic community responses to sedimentary contaminations by anthropogenic toxic substances in the Geum River Estuary, South Korea 2014 43 3.1. Introduction 44 3.2. Materials and Methods 47 3.2.1. Study area and sampling 47 3.2.2. PTS analyses 49 3.2.3. Environment parameters and macrobenthic fauna analyses 53 3.2.4. Data analyses 53 3.3. Results and Discussion 55 3.3.1. Spatiotemporal distributions of metals and the metalloid 55 3.3.2. Spatiotemporal distributions of PAHs and APs 66 3.3.3. Spatiotemporal patterns of macrofaunal assemblages 72 3.3.4. Key factors influencing the spatiotemporal pattern of macrofaunal assemblages 76 3.4. Summary 83 CHAPTER. 4. Large-Scale Monitoring And Ecological Risk Assessment Of Persistent Toxic Substances In Riverine, Estuarine, And Coastal Sediments Of The Yellow And Bohai Seas 84 4.1. Introduction 85 4.2. Materials and Methods 89 4.2.1. Study area and sampling 89 4.2.2. Chemicals and reagents 92 4.2.3. PTSs analyses 94 4.2.4. TOC, TN, and stable isotopes analyses 97 4.2.5. Positive matrix factorization receptor model 98 4.2.6. Macrobenthic fauna analysis 99 4.2.7. Data analyses 99 4.3. Results and Discussion 100 4.3.1. Distributions of PTSs in sediments of Yellow and Bohai seas 100 4.3.2. Assessment of potential ecological risks 108 4.3.3. Compositions and sources of PTSs 109 4.3.4. PTSs distributions by land-use types 117 4.3.5. Comparison of PTSs contaminations between 2008 and 2018 123 4.3.6. Macrobenthic fauna community 127 4.4. Summary 130 CHAPTER. 5. Historical Sedimentary Record And Flux Of Classic And Emerging Persistent Toxic Substances In Intertidal Sediment Cores From The Yellow And Bohai Seas 131 5.1. Introduction 132 5.2. Materials and Methods 135 5.2.1. Sampling 135 5.2.2. Target chemicals 137 5.2.3. Analyses of persistent toxic substances 137 5.2.4. Sediment dating and PTSs flux 142 5.2.5. Macrobenthic fauna analysis 145 5.2.6. Data analyses 145 5.3. Results and Discussion 146 5.3.1. Concentrations and fluxes of classic PTSs 146 5.3.2. Concentrations and fluxes of emerging PTSs 151 5.3.3. Compositional profiles and sources of PTSs 154 5.3.4. Deposition flux and mass inventory 162 5.3.5. Macrobenthic fauna community 164 5.4. Summary 167 CHAPTER. 6. Conclusions 168 6.1. Summary 169 6.2. Environmental implications and Limitations 177 6.3. Future Research Directions 184 BIBLIOGRAPHY 186 ABSTRACT (IN KOREAN) 208 APPENDIX 209Docto

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