臺灣博碩士論文加值系統

在海洋循環系統中，海底湧泉-滲流環境所輸出的流體，為海洋內部系統提供極大量的水和物質輸入，且對於海洋物質平衡有極大的影響，此環境輸出之流體為極有效率的傳輸載體。而追蹤這些流體的運送及演變歷程，對於流體在整個海洋循環之輸入輸出（source-sink），扮演了極為重要的角色。本論文目的在於探討希臘米羅斯火山島及密西西比河輸出海域，其海洋湧泉-滲流系統之流體來源、化學組成、運送及演變歷程。
位於希臘愛琴海域之米羅斯島（Milos），為一個淺海的火山島海底熱液湧泉系統，本研究於2002及2003年採集總計有71個海底熱液湧泉流體，分析其硼（B）濃度，同位素分析，及主要與微量元素濃度。實驗結果發現有三種類型流體存在於此熱液系統、分別為Cave、Brine及類海水（seawater-like）流體。其中Cave流體具備特性為低pH、Cl及B濃度，流經海底裂隙並直接出露於海平面上。Brine流體具備特性為高鹽度、及高於海水十倍以上之B濃度。本研究分析認為此海底熱液系統，存在兩個不同端源母流體（reservoir fluid）循環：其一位於海平面下深度1-2 km，而另一則位於深度較淺位置（約0.5 km）。較深之端源母流體，具備高溫約313 °C特性，且發生次臨界相分離作用（subcritical phase separation），此作用分餾出含相對低量B的氣相及富含高濃度B的高鹽液相流體，且無造成顯著同位素分異。相分離後之氣相流體，直接迅速沿著岩石裂隙往上流動，最後形成所觀察到之Cave流體。同時分離後之高鹽液相流體，由於密度較高，因此緩慢沿著裂隙往海底表面傳輸，並於傳輸過程混入向下滲流之海水，最後形成所觀察之Brine流體。另一深度較淺之端源母流體，具備稍低約248 °C之反應溫度，此循環形成之類海水流體，具備較海水稍低B濃度及接近海水之B同位素值。
此外，本研究發現Cave流體有較海水異常之Br/Cl比值（約低56%），而Brine流體同樣表現約低於海水31%。另外兩類型流體之I/Cl比值則遠高於十倍海水，但落於深海中洋脊（Mid-Ocean Ridge）及海底沈積熱液系統（Sediment-hosted Ridge）的比值範圍間。此高I/Cl比值顯示，深部端源母流體應於進行相分離作用前，即受到沈積物作用影響。相分離作用於深部持續進行，並將分餾出較高Br/Cl比值之氣相流體，而存留於深部之高鹽液相流體，則會呈現持續降低之Br/Cl比值。本研究之B濃度及同位素數據，整合過去研究文獻，對於火山系統、其他海底熱液系統及實驗室模擬相分離之研究數據，認為Milos海底熱液系統之深部端源母流體（高B/Cl比值，低δ11B），有受到火山岩漿後期演化流體參入之可能，並計算得出約有18-47%的比例。
另外，本研究於密西西比河輸出海域（Mississippi River plume），於2006及2007兩航次採集表水及垂直剖面水樣（129個樣本）。結果可發現此海域水體，主要由河水及高鹽流體混合海水形成。淡水源自於密西西比河河水注入，含有低鹽度、低主要極微量元素濃度，但含有高濃度Ba及較高之87Sr/86Sr同位素比值，其流經路徑由密西西比河口沿著近岸向西流動，且有逆時針方向之渦流產生，此流徑主要是由風所帶動。另外高鹽流體皆可於幾個站的深部水體觀察到，具備有高鹽度、高濃度Sr、B、Ba等特性。此流體來源可能為來自岩層中古鹽體（salt dome），複雜之流體-高鹽滷液反應，然後從海底裂隙滲流至海底表面，抑或是藉由高鹽度海底地下水（Submarine Groundwater Discharge）注入至此海域。

The discharges of fluid in vent-seep subsurface environment are efficient media to transport materials to the hydrosphere and affect the chemical mass balance in the ocean. Tracing fluid transport and evolution plays a major role and is of major interest to a variety of research works. This study aims to evaluate the origins, chemical compositions, evolution and transport of seep and vent fluids in Milos system and Mississippi River plume system.
Seventy-one vent fluids collected during two field excursions in 2002 and 2003 from a shallow-water hydrothermal system at Milos in Aegean Sea, were analyzed for B, δ11B and major/trace elements. Three types of hydrothermal vent fluids were identified as cave, submarine-brine, and seawater-like fluids. The cave fluids discharge through rock fissures near sea-level, and have lower pH, chlorinity, and B concentrations. The submarine-brine fluids are characterized by high Cl, and contain 〉10 times seawater B concentrations. A scenario involving a two-cells circulation occurs at 1-2 km and at shallower depth is proposed. The deeper saline reservoir with a reaction temperature of 313 °C has experienced subcritical phase separation, distributing B depletion in vapor and enrichment in brine with no detectable isotopic fractionation. The vapors rise directly to form the cave vents, whereas the saline fluids transport in different pathways and are influenced by seawater mixing to form the variable submarine-brine fluids.
Large temporal variations (56% depletion relative to seawater) in Br/Cl ratios are detected in the cave fluids. On the other hand, the submarine-brine fluids are characterized by small temporal Br/Cl variability (31% depletion). The I/Cl ratios in both cave and submarine-brine fluids are more than 10 times higher than in seawater. The high I/Cl data suggests that the fluids were influenced by sediment diagenesis prior to phase separation. The phase separation boils off vapor with high Br/Cl continuously at deep seated reservoir to create low Br/Cl brines. In addition tidal regulation at shallow depths may have an effect if halite diagenesis occurs. These end-member fluids were characterized with high B/Cl ratios (1~5) and extreme low δ11B (3.34~7.24 ‰) except the seawater-like fluids (~22‰). This supports addition of magmatic water (6.9 mM and -2.5‰) to deep reservoir. Using a simple binary mixing model of the evolved seawater and the magmatic water, the latter was estimated to contribute 18 to 47% of B in Milos fluids.
For estuarine waters in Mississippi River plume in the northern Gulf of Mexico (GOM), surface and depth profile seawater specimens were collected from several transect stations of two cruises in 2006 and 2007. Several end-member fluids with distinct chemical compositions were identified, including saline water, seawater and freshwater. The fresh water have low salinity, low concentration of major and minor elements (e.g. B, Br, U, Sr), but high Ba and 87Sr/86Sr ratio and flows from west Birfoot delta region and moves westward along the coast, as well as occurrence of some counterclockwise eddies induced dominantly by wind forcing. There are saline waters with high salinity, Sr, B and Ba contents relative to seawater distributed at bottom depth of several stations during both sampling cruises, as well as different 87Sr/86Sr ratios of 0.708899 and 0.709395 from seawater in April 2006. These saline waters possibly originate from complicate mixture of several brines involved with halite dissolution and reaction with halite/anhydrite from ancient evaporitic salt. Alternatively, these saline seepages are potentially sourced from formation water associated with oil and gas extraction and/or seawater recirculation via submarine groundwater discharge (SGD).

Abstract I
摘要（Abstract in Chinese） III
Acknowledgements VI
Table of Contents VIII
List of Tables XII
List of Figures XIV
Chapter 1 1
General Introduction 1
1.1 Identifying vent-seep subsurface environment 1
1.2 Shallow-water hydrothermal vent system- Milos Island 3
1.3 Submarine seeps system- Mississippi River plume system 5
1.4 Purpose and structure of this dissertation 7
Chapter 2 11
Two-cells phase separation in shallow submarine hydrothermal system at Milos Island, Greece: Boron isotopic evidence 11
Abstract 12
2.1 Introduction 13
2.2 Geological setting and sample descriptions 14
2.3 Sampling and analytical methods 15
2.4 Results 16
2.5 Discussion 16
2.5.1 Deep fluids reservoir 16
2.5.2 Shallow fluid reservoir 18
2.5.3 Vent fluid circulation at Milos 19
2.5.4 Genesis of magmatic heat source 20
Chapter 3 29
Br/Cl and I/Cl systematics in the shallow-water hydrothermal system at Milos Island, Hellenic Arc 29
Abstract 30
3.1 Introduction 32
3.2 Geological settings and samples 34
3.3 Sampling and analytical methods 36
3.4 Results 37
3.5 Discussion 38
3.5.1 Distribution of Br/Cl and I/Cl in vent fluids 38
3.5.2 Br/Cl fractionation in hydrothermal fluids at Milos 39
3.5.2.1 Br/Cl in low-Cl fluids 39
3.5.2.2 Br/Cl in high-Cl brine fluids 41
3.5.3 Effect of sediment contribution 42
3.6 Conclusions 45
Chapter 4 59
Magmatic Water Contribution in Milos Submarine Hydrothermal Fluids: New Boron Isotopic Evidences 59
Abstract 60
4.1 Introduction 62
4.2 Background 63
4.2.1 Phase separation 63
4.2.2 Water/rock/sediment interaction 65
4.2.3 Magmatic water contribution 66
4.3 Samples and experimental procedures 67
4.3.1 Geological settings 67
4.3.2 Sample information 68
4.3.3 Sample collection and analytical methods 69
4.4 Results 71
4.5 Discussion 72
4.5.1 Origin of deep reservoir fluids at Milos 72
4.5.2 Role of phase separation 73
4.5.3 Influence of sediments and/or magmatic water 74
4.5.4 Evolution of brine reservoir 77
4.6 Conclusions 77
Chapter 5 91
Tracing the freshwater and saline fluids of the Mississippi River plume and adjacent estuary in the northern Gulf of Mexico continental shelf: major/trace element and Sr isotopic distribution 91
Abstract 92
5.1 Introduction 93
5.2 Geological setting and samples 97
5.3 Sample preparation and analyses 98
5.3.1 Elemental concentration determination in estuarine fluids 98
5.3.2 Isotopic Sr analysis in estuarine fluids 98
5.4 Results 99
5.4.1 Chemistry of fluids 99
5.4.1.1 Major, trace element chemistry and salinity gradient 99
5.4.1.2 Sr isotopes 99
5.5 Discussion 100
5.5.1 Freshwater inputs 100
5.5.2 Distribution of saline water 102
5.5.3 SGD? 104
5.6 Conclusions 105
Chapter 6 125
Concluding remarks 125
References 131
Appendix A 159
Porewater geochemistry and authigenic barite formation in methane-rich sediments from continental margins offshore southwestern Taiwan 159
Abstract 160
A.1 Introduction 161
A.2 Geological setting and sample collection 163
A.3 Methods 164
A.3.1 Pore water and extraction of barite in sediments 164
A.3.2 Chemical analysis 165
A.3.3 Diffusive flux calculation 165
A.4 Results 166
A.4.1 Pore fluids chemistry 166
A.4.1.1 Dissolved sulfate and barium 166
A.4.1.2 Alkaline earth elements 167
A.4.2 Extracted labile-Ba2+ of barite phase in sediments 168
A.5 Discussion 168
A.5.1 Diffusion of Ba2+ and SO42- in pore waters 168
A.5.2 Authigenic minerals and barite formation 170
A.5.2.1 Removal of Ca, Mg and Sr in pore fluids 170
A.5.2.2 Evaluation of barite saturation 171
A.5.2.3 Anomalous labile-Ba2+ enrichment in MD-052913 173
A.5.2.4 Sources of Ba2+ in sediments 174
A.5.3 SMT evolution and significances 175
A.5.3.1 Methane migration offshore southwestern Taiwan 175
A.5.3.2 SMT variations and influence of barite formation 175
A.6 Conclusions 176
A.7 References 178

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