全球氣候系統和陸源的風化作用構成一個相互影響的回饋機制。在地質時間尺度下，陸源風化作用會改變大氣中的二氧化碳含量，因此將擾動全球的氣候狀態；同時氣候狀態的改變抑會影響陸源風化的來源、速率及程度。這個交互作用的機制就取決於矽酸鹽風化所消耗的二氧化碳量及海洋碳酸鹽循環所釋出二氧化碳量的平衡。因此，釐清陸源風化的來源（矽酸鹽或是碳酸鹽風化）及研究風化作用的程度將有助於了解長時間尺度的氣候變遷。
第一章，結合放射性（87Sr/86Sr）及穩定（δ88/86Sr）鍶同位素系統的新方法，比過去單獨使用放射性鍶同位素系統，更能精確的評估冰期與間冰期尺度海洋鍶同位素的收支模型（marine Sr isotopic budget），進而探討地質時間尺度的風化趨勢及氣候變遷的相關議題。這是因為新方法同時結合87Sr/86Sr有效示蹤風化來源（對於海洋系統的貢獻），及δ88/86Sr的同位素分化評估海洋碳酸鈣沉澱時所移除海水鍶通量。不過，目前對於δ88/86Sr在陸源風化環境裡的研究著墨不多，分化機制也尚未明確，因此在應用這個新的同位素工具來解析海洋鍶同位素的收支模型的同時，必須先釐清幾個前提：
(1) 矽酸鹽與碳酸鹽的δ88/86Sr比值分佈範圍。
(2) 影響δ88/86Sr在陸源風化環境中分化的潛在機制為何？
(3) 控制陸源通量（河水）的δ88/86Sr比值的機制為何？
為有效評估上述問題，本研究透過研究自然樣品及實驗室控制實驗來釐清穩定鍶同位素系統在陸源風化過程中潛在的同位素分化行為。
第二章，本研究發展結合empirical external normalization（EEN）及 standard sample bracketing（SSB）的質量偏移（mass bias）修正技術在多接收器感應耦合電漿質譜儀（MC-ICP-MS）量測高精確、精準度的穩定鍶同位素比值（δ88/86Sr）。本章節深入探討Sr與Zr在MC-ICP-MS測量中的同位素分化行為，並評估使用92Zr/90Zr比值取代現行91Zr/90Zr比值作為δ88/86Sr量測時質量偏移修正的基準。結果顯示，92Zr/90Zr比值在質譜儀中產生的非質量偏移的效應（instrumental mass independent isotope fractionation）較91Zr/90Zr比值來得小，因此新的方法可提昇1.5倍的分析精確度。本研究所建立之新方法除了提供了相當於使用雙示蹤計（double spikes）質量偏移修正技術的精確度，並且提高了樣品的分析效率。
第三章，透過中國黃土高原經歷強烈成土作用的古土壤剖面，評估矽酸鹽礦物化學風化過程中可能的δ88/86Sr同位素分化。本研究運用化學序列萃取（sequential extraction）技術分析古土壤中可交換相（exchangeable）、氧化物相（oxides）及矽酸鹽相的δ88/86Sr比值。結果顯示，在矽酸鹽差異風化（silicate incongruent weathering）過程當中，較重的鍶同位素核種有被優先釋放至可交換相或土壤水的趨勢。這個現象進一步在實驗室透過矽酸鹽及黏土礦物標準品的稀酸淋溶（leaching）實驗獲得證實。
第四章，本研究透過碳酸鹽流域河水δ88/86Sr的時間序列監測評估次生碳酸鈣的沈澱及矽酸鹽礦物差異風化對於河水δ88/86Sr的影響。石灰岩洞穴河水的監測結果呈現了季節性的δ88/86Sr分佈趨勢，顯示在高溫多雨季節矽酸鹽的風化作用提供高放射性87Sr/86Sr及較重δ88/86Sr的來源。另一方面，至少有30%~55%溶解鈣離子在次生碳酸鈣沈澱時被移除，導致河水δ88/86Sr全面性約有0.1‰偏重的結果。這些數據強調次生碳酸鈣沉澱對於碳酸鹽流域河水富集較重δ88/86Sr的影響，以及受到高強度的矽酸鹽風化呈現較高87Sr/86Sr及δ88/86Sr比值的極端值。
第五章，統計目前所有公開發表的δ88/86Sr文獻數據（2006年至2015年初）及本研究的成果，用以評估哪些潛在的機制控制陸源風化通量的δ88/86Sr比值變化及變異程度對海洋鍶同位素收支模型的影響。統計結果顯示，矽酸鹽和碳酸鹽的δ88/86Sr比值分佈範圍顯著地比河流的分佈範圍輕，顯示河水的δ88/86Sr比值分佈不是單純反映岩性的變化。風化過程中相關的同位素分化機制，諸如次生碳酸鹽生成、矽酸鹽的差異風化及植被的攝取，都是潛在導致富集較重δ88/86Sr比值的因素。
在冰期與間冰期的時間尺度之下，陸源風化作用的來源與程度呈現差異將會對於整個海洋鍶同位素收支模型帶來顯著的影響。因此，更全面的評估現代河川δ88/86Sr比值時序及空間上的變異是一個相當重要的研究議題，能對於理解地質時間尺度上的陸源風化還有建構更精準的全球氣候變遷模式有正面的影響。

The relationship between global climate change and continental weathering is a cause-consequence feedback system. Global climate may be perturbed by any of processes controlling weathering through changing atmospheric CO2 abundance, and in turns to further affect the extent of weathering. In this iteration, the atmospheric CO2 fluctuation is controlled by the stoichiometric balance between the CO2 consumption by silicate mineral weathering and CO2 release by marine carbonate precipitation at long-term time scale. Thus, discriminating the terrestrial weathering sources from silicates and carbonates, and determining the extent of weathering are important and the fundamental knowledge for comprehending the long-term climatic evolution.
In chapter 1, the application of newly triple Sr isotopes, 87Sr/86Sr and δ88/86Sr ratios, was introduced and suggested to serve as a powerful isotopic tracer, rather than the 87Sr/86Sr alone, for simultaneously determining the continental weathering fluxes to the ocean and quantifying the Sr burial flux by the carbonate precipitation in the marine system at glacial and interglacial climatic cycles. Given that rivers are the largest Sr source to the ocean, however, there were only few attempts available for studying relevant controls on δ88/86Sr fractionation in riverine waters. In order to have confidence in interpretation based on the recent developed isotopic proxy, the following questions should be therefore clarified by the first order:
(1) The variability of δ88/86Sr for lithological specimens, i.e. silicates and carbonates.
(2) Potential physicochemical processes that controlling the δ88/86Sr fractionation in terrestrial environments.
(3) Lithology and/or fractionation control the variability of δ88/86Sr in riverine waters.
To address those fundamental questions, the following chapters provide a comprehensive evaluation of stable Sr isotope fractionation during continental weathering processes by natural specimens and laboratory experimental works.
In chapter 2, we demonstrated a highly precise and accurate δ88/86Sr determination by using multiple-collector inductively coupled plasma mass spectrometry (MC-ICP-MS) with empirical external normalization and standard sample bracketing (EEN-SSB) method for mass bias correction. In this chapter, we evaluated the fractionation behaviors of Sr and Zr isotopes during MC-ICP-MS determinations and established a modified procedure to apply 92Zr/90Zr instead of currently available 91Zr/90Zr for Sr isotopic mass bias correction. A factor of 1.5 was improved in precision of our δ88/86Sr determination that is likely owing to the smallest instrumental mass-independent fractionation between the isotopic pair of 88Sr/86Sr and 92Zr/90Zr. This new method allows 87Sr/86Sr and δ88/86Sr ratios to be measured simultaneously with high throughput and comparable precision and reproducibility with double spike (DS) applied MC-ICP-MS δ88/86Sr determinations.
In chapter 3, to evaluate the potential processes lead to δ88/86Sr fractionation during silicate mineral weathering, an intense pedogenic paleosol sequence was sampled in the Chinese Loess Plateau (CLP). Sequential extraction procedure was applied to isolate different geochemical phases of the soils to study the stable Sr isotopic distributions in the extracted exchangeable, reducible and silicate fractions. The results suggested that heavier δ88/86Sr was preferentially released during incongruent silicate mineral weathering. This is further evidenced by the acid leaching experiments using the soil silicate phase, primary silicate minerals and clay standards.
In chapter 4, an annual time-series monitoring of chemical and Sr isotopic compositions on a carbonate-dominated catchment was performed to evaluate the influences of secondary calcite precipitation and silicate mineral weathering on water δ88/86Sr. A seasonal systematic of karst cave stream water δ88/86Sr was detected showing coherent heavier δ88/86Sr and radiogenic 87Sr/86Sr ratios detected in the warm and rainfall period reflecting enhanced biological activities and intensive silicate weathering at that time. On the other hand, at least 30% to 55% of Ca was removed by the secondary calcite precipitation and lead to 0.1‰ heavier in water δ88/86Sr. Those time-series data emphasizes the critical role of secondary calcite precipitation on the comprehensive heavy δ88/86Sr ratios in waters draining carbonate-dominated catchments, and peak of related heavy δ88/86Sr ratios by intensive silicate weathering in wet season and extreme rainfall events.
In chapter 5 (conclusion), we compile all the currently published stable Sr isotope data from literature sources (2006 to early 2015) and this study for evaluating the potential mechanisms controlling the sensitivity and variability of δ88/86Sr of the continental weathering flux to the ocean and its implication for global Sr cycling. The data suggests that the variability of δ88/86Sr of the terrestrial silicate materials and carbonates are statistically lighter than that of riverine waters. In stead of lithology, fractionation of Sr stable isotopes during and post-weathering processes, such as secondary phase precipitated, incongruent silicate weathering, and vegetation uptake, might be more important factors and by the first order lead to the enrichment of heavy δ88/86Sr in the waters.
The degree of δ88/86Sr fractionation in continental weathering environments may have significant implications to the oceanic Sr isotopic budget at glacial-interglacial time scales. The variability of δ88/86Sr in modern rivers will still need to be better constrained for studying the global Sr cycling at geological time scales.

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