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研究生： 郭慈穎
Kuo, Tzu-Ying
論文名稱： 南中國海沉積物鍶、釹、鉿、鉛同位素對北呂宋島弧地函交代換質作用之制約
Sr-Nd-Hf-Pb isotopic constraints on the role of South China Sea sediments in mantle wedge metasomatism beneath the North Luzon Arc
指導教授： 楊懷仁
Yang, Huai-Jen
李德春
Lee, Der-Chuen
學位類別： 碩士
Master
系所名稱： 理學院 - 地球科學系
Department of Earth Sciences
論文出版年： 2007
畢業學年度： 95
語文別： 英文
論文頁數： 95
中文關鍵詞： 地函交代換質作用 、鍶、釹、鉿、鉛同位素 、南中國海沉積物 、北呂宋島弧
外文關鍵詞： Sr-Nd-Hf-Pb isotope, North Luzon Arc, South China Sea sediments, Mantle metasomatism
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    • 隱沒沉積物(Sediments)在地殼、地函交換中扮演著重要角色，包括對於聚合邊界之火成作用、地函異質性、地殼的組成及生長之瞭解都需經由隱沒沉積物之化學分析。然而，分佈於全球隱沒帶區沉積物之成份差異極巨，加上隱沒角度及隱沒板塊年齡亦會造成不同化學效應，因此，區域性隱沒沉積物對地函交代換質作用影響之深入研究更顯重要。本文以北呂宋島弧(North Luzon Arc, NLA)為研究區域，分析由海洋鑽探計畫(ODP)取得之38個南中國海沉積物的鍶、釹、鉿、鉛同位素及微量元素成份，進而探討南中國海沉積物在北呂宋島弧區域地函交代換質作用中所扮演的角色。
    利用沉積物、虧損地函及北呂宋島弧岩漿在此四個同位素系統中的相對位置，模擬三種地函交代換質作用之同位素特徵，分別為：(一) 地函受沉積物交代換質、(二) 地函受沉積物岩漿(sediment- derived melts)交代換質、(三) 地函受沉積物及隱沒海洋地殼岩漿(sediment- and AOC- derived melts)交代換質。第一種交代換質模式在鍶-釹及鍶-鉿同位素系統中之混合曲線落於地函陣列，無法解釋偏離之北呂宋島弧岩漿，在鉛同位素系統中，混合曲線之趨勢亦無法符合。第二種交代換質模式的模擬結果顯示，鍶-釹及鍶-鉿的分化在沉積物岩漿中較原始沉積物為明顯，使混合曲線更加偏離北呂宋島弧岩漿，此外，鉛、釹及鉿在沉積物與岩漿間的分配係數相近，故其同位素混合曲線與第一種交代換質模式非常相近而同樣無法解釋北呂宋島弧岩漿，鉛與鍶同位素系統中之混合曲線之趨勢亦無法解釋北呂宋島弧。第三種模擬結果顯示其混合曲線在大多數的同位素系統中最能符合北呂宋島弧岩漿之北島(N-islands)及南島(S-islands)，模擬結果指示，當約0.0016-0.0032%殘餘鋯石自沉積物分出時，北島岩漿需加入50-80%碎屑沉積物源(detrital sediments)岩漿及20-50%海洋地殼源岩漿，而南島岩漿需加入10-40%混合沉積物源岩漿及90-60%海洋地殼源岩漿，此混合沉積物即包含碎屑沉積物及海水自生沉積物(authigenic sediments)，然而，巴丹島(Batan island)岩漿除了需加入約70:30的碎屑沉積物源及海洋地殼源岩漿外，需有約0.005%的鋯石自海洋地殼岩漿分出而殘留於地函，始能符合巴丹島岩漿成份。
    此次研究發現兩個不同於現有研究之結果：(一) 現有針對北呂宋島弧區域之研究從未討論隱沒海洋地殼所扮演的角色，而本文提出海洋地殼源岩漿亦為此區重要的交代換質介質之一；(二) 現有文獻認為此區受到遠洋沉積物之交代換質，而此研究發現南中國海之半遠洋沉積物即可解釋北呂宋島弧之鍶、釹、鉿、鉛同位素特徵；(三) 南中國海板塊之年紀（~35 Ma）及地函擄獲岩中發現之埃達克質（adakitic）包裹體皆支持隱沒海洋地殼源岩漿之加入。

    Subducted sediments are key components in crustal-mantle recycling. Understandings on convergent margin magmatism, mantle heterogeneity, crustal composition, and crustal growth all require constraints on the chemical fluxes of subducted sediments. However, the compositions of the subducted sediments vary significantly among subduction zones. Moreover, their chemical effects also depend on the nature of subduction, such as subduction angle and age of the subducted plate. Consequently, there is a clear need to characterize the chemical flux in individual subduction zones. This study aims to determine the role of the subducting South China Sea (SCS) sediments in mantle metasomatism beneath the North Luzon Arc (NLA) using Sr-Nd-Hf-Pb isotope systematics.
    Based on Sr-Nd-Hf-Pb isotope variations, three mantle metasomatism models are considered for the sources of NLA lavas. They are: (I) addition of bulk sediments to depleted mantle, (II) depleted mantle metasomatized by sediment-derived melts, and (III) depleted mantle metasomatized by melts derived from sediments and altered oceanic crust (AOC). Although not considered in model calculations, the contributions of sediment-derived and AOC-derived fluids are also addressed qualitatively. The first metasomatism model results in mixing curves overlapping with the mantle array in Sr versus Nd and Hf isotope plots, inconsistent with the distributions of the NLA lavas, which deviate from mantle array to lower 143Nd/144Nd and 176Hf/177Hf values. This model also fails to explain the NLA lavas in Pb versus Sr, Nd and Hf isotopes spaces. The involvement of sediment-derived melts (Model II) leads to source compositions with larger deviation from the NLA lavas in Sr versus Nd and Hf isotope plots, because sediment-derived melts have higher Sr/Nd and Sr/Hf ratios than their sources. Since Pb has similar compatibility to Nd and Hf, this model results in comparable mixing curves to model I. The mixing curves derived from model III with variable amounts of residual zircons provide the best fit to most NLA lavas. Specifically, with 0.0016-0.0032% residual zircons in the subducted sediments, 20-50% AOC-derived melts and 50-80% sediment-derived melts can explain the N-island lavas, whereas the S-island lavas can be derived from sources metasomatized by 90-60% AOC-derived melts and 10-40% sediment-derived melts. The sources of Batan island lavas can be explained by ~30% AOC-derived melts in equilibrium with 0.005% residual zircons and ~70% sediment-derived melts. In all three models, the addition of AOC-derived fluids can improve the model fits to the NLA data. However, the contribution of AOC-derived fluids to the trace element budgets in the metasomatized mantle should be far less significant compared to that of the slab-derived melts due to their low trace element abundances.
    Two major differences between the existing and the proposed metasomatism models are: (1) the involvement of AOC-derived melts which were not considered by existing models can be the depleted metasomatic agents that satisfactorily explain most NLA lavas, and (2) the melts derived from SCS hemipelagic sediments can be the appropriate long-term enriched component. There is no need to postulate involvements of liquids from pelagic sediments, which is absent in the present-day NLA tectonic setting. In addition, the requirement of AOC-derived melts is consistent with the subduction of young SCS plate (~35 Ma) and the occurrence of the adakitic glass inclusions in mantle xenoliths. Finally, more rock samples from the NLA, specifically Lutao island, have to be analyzed for Sr, Nd, Hf, and Pb isotope ratios to justify the linear trends of these lavas in the Sm/Hf-143Nd/144Nd and Sm/Hf-176Hf/177Hf plots of Marini et al. (2005) and to re-evaluate the role of crustal contamination.

    摘要--I Abstract--III 誌謝--V Table of contents--i List of tables--iii List of figures--iv Chapter 1 Introduction--1 Chapter 2 Geological setting and samples--10 Chapter 3 Analytical techniques and procedures--14 3.1 Leaching--14 3.1.1 Method 1: Hot HCl leaching--14 3.1.2 Method 2: Two step leaching by acetic acid and aqua regia--17 3.1.3 Method 2: HCl leaching by ultrasonic vibration--21 3.2 Digestion--21 3.3 Chemical separations--21 3.3.1 Pb separation--22 3.3.2 Hf separation--24 3.3.3 Sr and Nd separations--24 3.4 Measurements--31 3.4.1 MC-ICP-MS--31 3.4.2 TIMS--33 3.4.3 Q-ICP-MS--33 Chapter 4 Results--38 4.1 Trace element abundances--38 4.2 Isotope compositions--38 4.3 Isotopic systematics--47 Chapter 5 Discussion--51 5.1 Identifying metasomatic agents--51 5.1.1 Model I--55 5.1.2 Model II--60 5.1.3 Model III--64 5.2 Differences between the existing and newly proposed metasomatism models for NLA lavas--65 5.3 Constraining relative contributions of metasomatic agents--70 5.4 Physical aspects of the proposed metasomatism model--71 5.4.1 The nature of the subducted slab--71 5.4.2 Compare with geophysical data--79 5.5 Comparisons between the NLA and other arc systems--81 Chapter 6 Conclusions--85 References--87 Fig. 1-1 The sketch of mantle metasomatism at a subduction zone. 2 Fig. 1-2 The 10Be/Be atom ratio vs. B/Be from Morris et al. (1990). 2 Fig. 1-3 The geological map of the region of North Luzon Arc (NLA). 4 Fig. 1-4 Nd-Sr isotopic plot from Chen et al. (1990). 6 Fig. 1-5 87Sr/86Sr vs. 143Nd/144Nd plot of McDermott et al. (1993). 6 Fig. 1-6 Three groups of the NLA lavas define distinct Sm/Hf-143Nd/144Nd and Sm/Hf-176Hf/177Hf arrays. 8 Fig. 1-7 εHf vs. εNd diagram comparing NLA lavas to the field of MORB, Fe-Mn crusts and nodules, SCS sediments and lithogenous-hemipelagic sands and clays. 8 Fig. 2-1 Geographic distribution of NLA islands and their radiometric ages (numbers shown in boxes, Ma) from Yang et al. (1996). 11 Fig. 2-2 Age-depth relationship for sediments from Leg 184 sites from Wang et al.(1999, 2000). 12 Fig. 3-1 Sketch for analytical procedures for Sr, Nd, Hf and Pb isotope and trace element abundances. 15 Fig. 3-2 Sketch for hot HCl-leaching procedures (method 1). 15 Fig. 3-3 Comparison between temporal variation of 87Sr/86Sr ratios of seawater (McArthur et al., 2001) and that of sample A21 leachates from different HCl concentrations. 16 Fig. 3-4 Sketch of the two-step leaching procedure; acetic-acid leaching followed by aqua- regia leaching. 19 Fig. 3-5 Comparison between 87Sr/86Sr of seawater and leachates 1 and 2 from the two-step leaching procedure. 20 Fig. 3-6 Sequence for Pb, Hf, Sr and Nd separations. 22 Fig. 3-7 Sketch of procedures for Pb separations. 23 Fig. 3-8 Sketch of first column procedures for HFSE separation. 25 Fig. 3-9 Sketch of second column procedured for separating Hf from Ti and Zr. 26 Fig. 3-10 Elution curves from second column procedures for Hf separation. 27 Fig. 3-11 Sketch of first column procedures for collecting Sr and REE aliquot. 29 Fig. 3-12 Sketch of Sr-spec and Ln column procedures. 30 Fig. 3-13 Sketch and photo of Nu Plasma MC-ICP-MS. 32 Fig. 3-14 Sketch and photo of Finnigan MAT 262 TIMS. 34 Fig. 3-15 Long-term (8/8/2005-6/19/2007) measurements on the 143Nd/144Nd and 87Sr/86Sr ratios of standard ALTA and SRM 987. 35 Fig. 3-16 Sketch and photo of Agilent 7500ce Q-ICP-MS. 37 Fig. 4-1 Tempral variations of Pb, Sr and Nd abundances. 40 Fig. 4-2 Tempral variations of Hf abundances. 41 Fig. 4-3 Tempral variations of isotopic ratios. 45 Fig. 4-4 Sr-Nd-Hf isotopic systematics of leached and un-leached SCS sediments. 48 Fig. 4-5 Pb isotopic ratios versus 87Sr/86Sr, 143Nd/144Nd and 176Hf/177Hf ratios of leached SCS sediments. 49 Fig. 5-1 Sr-Nd-Hf-Pb isotopic plots of Model I results with SCS sediments and NLA lavas. 57 Fig. 5-2 Sr-Nd-Hf-Pb isotopic plots of Model II results with SCS sediments and NLA lavas. 61 Fig. 5-3 Sr-Nd-Hf-Pb isotopic plots of Model III results with SCS sediments and NLA lavas. 66 Fig. 5-4 PM-normalized REE patterns of (a) NLA lavas, and (b) pelagic sediments. 72 Fig. 5-5 Comparisons between Sr-Nd-Hf-Pb isotopic systematics of N-islands and results from metasomatism model III. 73 Fig. 5-6 Comparisons between Sr-Nd-Hf-Pb isotopic systematics of S-islands and results from metasomatism model III. 75 Fig. 5-7 Comparisons between Sr-Nd-Hf-Pb isotopic systematics of Batan islands and results frommetasomatism model III. 77 Fig. 5-8 The slab subduction angles at N-island, Batan island and S-islands. 80 Fig. 5-9 The seismicity distribution and focal mechanism solutions from Bautista et al. 80 Fig. 5-10 The sketch of the transportation of metasomatized mantle from 70 km to sub-NLA mantle at 100 km. 84 Fig. 5-11 Generalized map of the Trans-Mexican Volcanic Belt (TMVB). 84 Table 3-1 87Sr/86Sr and 143Nd/144Nd ratios of leached and un-leached aliquots of sample A21 16 Table 3-2 87Sr/86Sr and 143Nd/144Nd ratios of leachate 1 and 2 of six selective samples 20 Table 4-1 Trace element abundances of leached and un-leached aliquots. 39 Table 4-2 Isotopic ratios of leached and un-leached aliquots. 42 Table 5-1 The trace element and isotope composition of the depleted and enriched components. 53 Table 5-2 Partition coefficients for calculating dehydration and partial melting. 54

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