非傳統穩定鍶同位素在陸地風化過程中所產生的同位素分化作用( V )

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科技部補助專題研究計畫成果報告

期末報告

非傳統穩定鍶同位素在陸地風化過程中所產生的同位素分化作

用(5/5)

計畫類別：個別型計畫

計畫編號： MOST 105-2116-M-006-011- 執行期間： 105年08月01日至106年07月31日執行單位：國立成功大學地球科學系（所）

計畫主持人：游鎮烽

計畫參與人員：學士級-專任助理：程安琪

博士後研究-博士後研究：鍾全雄

報告附件：移地研究心得報告

出席國際學術會議心得報告

中　華　民　國　106　年　09　月　05　日

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中文摘要：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。

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技術分析古土壤中可交換相、氧化物相及矽酸鹽相的

δ88/86Sr比值。結果顯示，在矽酸鹽差異風化過程當中，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實驗獲得證實。

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。

中文關鍵詞：穩定鍶同位素, δ88/86Sr, 矽酸鹽差異風化, 成土作用, 次生碳酸鹽沈澱, 鍶同位素分化

英文摘要： 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.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). The 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

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minerals and clay standards.

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.

英文關鍵詞： Stable Sr isotopes, δ88/86Sr, incongruent silicate

weathering, pedogenesis, secondary calcite precipitation, Sr isotope fractionation

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Figures

Fig 1. Locations of the collected loess-paleosol sequence in the Chinese Loess Plateau (the Weinan section) and around desert sands.

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Fig. 2. Downcore distribution of magnetic susceptibility (A), mean grain size (B), and δ^88/86Sr of the processed geochemical fractions (C-F) for the Weinan section and the potential source of desert sands. Loess-paleosol stratigraphy (S1-3 and L2) is constrained by magnetic susceptibility and mean grain size data according to Sun et al.

(2010) and identified as grey color bar. Error bars are 2σ.

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Fig. 3. Fractionation of stable Sr isotopes during surface exchange processes via Fe- oxides and clay standards in (A) pH and sorbent/solution controlled experiments, (B) temperature controlled experiments.

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Fig. 4. Results of laboratory leaching experiments by (A) clay standards and USGS primary mineral standards, and (B) natural specimens of the Weinan section and desert sand.

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Fig. 5. The relationship of Mg/Na molar ratios and δ^88/86Sr in the Weinan silicate post- experiment dissolved phase.

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Fig. 6. Stable Sr isotopic distributions of the processed specimens of standard rock materials, clay standards, and various geochemical fractions of the Weinan section and desert sands.

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Fig. 7. Mg/Ca and Mn/Ca ratios of the exchangeable fraction and silicate partial dissolution fraction in the Weinan section and potential source regions. The end- members of primary carbonates in the desert sands, carbonates in the CLP, and secondary carbonates in the Luochuan section are based on Li et al. (2013).

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Fig. 8. Plots of ⁸⁷Sr/⁸⁶Sr versus δ^88/86Sr of the processed geochemical fractions in the Weinan section and potential source regions.

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科技部補助專題研究計畫執行國際合作與移地研究心得報告

日期：106 年 6 月 28 日

計畫編號 MOST 105－2116－M－006－011－

計畫名稱非傳統穩定鍶同位素在陸地風化過程中所產生的同位素分化作用(5/5)

出國人員

姓名鍾全雄服務機構

及職稱

國立成功大學地球科學系

博士後研究員

出國時間

106 年 6 月 18 日

至

106 年 6 月 23 日

出國地點日本東京

出國研究

目的

□實驗 □田野調查 □採集樣本 □國際合作研究 █使用國外研究設施

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一、執行國際合作與移地研究過程

1.目的

為重建地質年代中，過去大氣中氧氣含量的變動趨勢，需進行定年分析。沉積

岩中的磷灰石是難得的定年材料，但全世界僅少數實驗室能針對岩石薄片中的磷

灰石進行鈾鉛同位素分析。東京大學海洋與大氣研究所的高解析度離子探針分析

實驗室為其中的佼佼者。此次日本行的主要工作為使用該所的 NanoSIMS 二次離

子質譜儀，分析磷灰石樣品之鈾、鉛同位素比值，以進行定年研究。

2. 過程

於 2017/06/18(周日)中午 10:00 分搭乘日本航空 JL802 班機於桃園機場出發，當

地時間 14:20 降落日本成田國際機場，入境後利用當地大眾運輸系統，於 19:00 分抵達

東京大學 Kashiwa 校區。隔日(周一)早上 8:00 開始於實驗室進行儀器調整及標準樣樣

品分析，下午進行樣品定位，傍晚獲得第一筆數據。為把握難得的儀器時間，周二

8:00~周四 23:30 密集進行樣品分析。周五(06/23)早上 8:00 至 12:00 進行初步數據處

理，並於 13:30 搭車前往東京成田國際機場，搭乘日本航空 JL809 班機於 18:00 起飛，

20:55 返抵國門。

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二、研究成果

總計分析了 15 個磷灰石樣品，104 個分析點，獲得超過一萬筆鈾鉛同位素數據。

圖一為分析所使用的儀器相片。圖二為標準樣品與聯輝實驗品的游離行為比較。圖三

為所獲得的鈾鉛同位素分析資料圖。

圖一、東京大學海洋與大氣研究所的 NanoSIMS 二次離子質譜儀

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圖二、標準樣品(圓點)與樣品(X)之游離行為比較

圖三、樣品之鈾鉛同位素組成

y = 0.2587x - 0.0006

0.00 0.05 0.10 0.15 0.20 0.25 0.30

0.00 0.20 0.40 0.60 0.80 1.00 1.20 1.40 1.60

206

Pb * /UO

UO

₂

/UO

0.0 5.0 10.0 15.0 20.0 25.0

0.000 0.010 0.020 0.030 0.040 0.050

204

Pb/

²⁰⁶

Pb

238

U/

206

Pb

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三、建議

東京大學設備先進、學風自由且為了基礎研究投入大量資源，難怪其研究成績斐

然。筆者在日本期間，僅受訓數十分鐘，研究室負責人就能放心讓筆者獨立操作造價

近五百萬美金的設備，這種為了研究數據不惜承擔儀器損壞風險的態度，值得我們效

法。國內研究經費有限，無力建立及維護類似實驗室，應多多補助學者或學生出國進

行研究。

四、本次出國若屬國際合作研究，雙方合作性質係屬：(可複選)

□分工收集研究資料

□交換分析實驗或調查結果

□共同執行理論建立模式並驗証

□共同執行歸納與比較分析

□元件或產品分工研發

□其他 (請填寫) _______

五、其他

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科技部補助專題研究計畫出席國際學術會議心得報告

日期： 105 年 10 月 03 日 計畫編號 MOST 105－2116－M－006－011－

計畫名稱非傳統穩定鍶同位素在陸地風化過程中所產生的同位素分化作用

(5/5) 出國人員

姓名鍾全雄服務機構及

職稱

成功大學地球科學系

會議時間 105 年 9 月 12 日至

105 年 9 月 15 日會議地點美國洛杉磯

會議名稱

(中文) 前寒武紀-寒武紀過渡期之古環境與氧分壓研討會

(英文) PALEOENVIRONMENT AND AMBIENT OXYGEN DURING THE PRECAMBRIAN-CAMBRIAN TRANSITION

發表題目

(中文)伊迪亞卡拉期陡山沱與寒武奇蘭頭地層之磷灰石放射性同位素定年研究

(英文) APATITE-BASED GEOCHRONOLOGY: Radiometric dating of fossil-infilling/-encrusting apatite grains from the Ediacarian Doushantuo and Early Cambrian Chulaktau Formations

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一、參加會議經過

本次至美國加州大學洛杉磯分校(UCLA)，主要目的是參加前寒武紀-寒武紀過渡期之古環境與氧分壓研討會。此會議是由微體古生物的泰斗 Williams James Schopf 所主辦，集合了來自台灣、美國、中國、俄羅斯等國的學者一起與會。會議行程如下:

交通行程：

2016/09/11 去程：Tainan, Taipei, Los Angeles International Airport

2016/09/15 回程：Los Angeles International Airport, Taipei, Tainan

會議行程:

MONDAY 12 SEPTEMBER

8:00am -- 9:00am Coffee and pastries/donuts, CSEOL Library UCLA (Room 5681 Geology Building; Map #1)

9:00am -- 9:10am Opening Remarks, Schopf 9:10am -- 10:10amYanan SHEN

University of Science and Technology of China, Hefei. China

GLOBAL OVERVIEW: The Precambrian-Cambrian phosphogenic episode: its geologic/biologic significance and distribution in space and time

10:10am -- 10:30am Coffee Break

10:30am -- 11:30am Volodya SERGEEV

Geological Institute, Russian Academy of Sciences, Moscow. Russia GEOLOGY/PALEONTOLOGY REGIONAL EXAMPLE: Geology,

stratigraphy and microbiotas of the Upper Precambrian through Lower Cambrian succession, Maly Karatau Range, Kazakhstan

11:30am -- 12:00 noon GROUP DISCUSSION

How/Where/Why was this global phosophogenic episode?

12:00 noon -- 1:15pm Lunch (on site)

1:15pm -- 2:00pm UCLA Campus Tour (return to CSEOL ~1:45pm)

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2:00pm – 3:00pm Dadan LI

University of Science and Technology of China, Hefei, China

STABLE ISOTOPE OVERVIEW: Sulfur and carbon isotopes at the Precambrian-Cambrian transition

3:00pm -- 3:30pm Coffee Break

3:30pm – 4:30pm Bear CHUNG

National Cheng Kung University, Tainan City, Taiwan

APATITE-BASED GEOCHRONOLOGY: Radiometric dating of fossil- infilling/-encrusting apatite grains from the Ediacarian Doushantuo and Early Cambrian Chulaktau Formations

4:30pm -- 5:00 pm GROUP DISCUSSION

What can we learn from the stable isotope and geochronometric data?

TUESDAY 13 SEPTEMBER

7:30am -- 8:30 am Coffee and pastries/donuts, CSEOL Library UCLA (Room 5681 Geology Building; see map#1)

8:30am -- 9:30am Dave BOTTJER

University of Southern California, Los Angeles, USA

PALEOBIOLOGY: DOUSHANTUO FM., CHINA Geological setting, paleoecology, and new insights into the apatite-permineralized Ediacarian Doushantuo microfossils

9:30am --10:30am Freemont GAO

California Institute of Technology, Pasadena, California, USA

PALEOBIOLOGY: DOUSHANTUO FM., CHINA A biology-based perspective of the preservation, affinities, and new discoveries of apatite- permineralized Ediacarian Doushantuo microfossils

10:30am -- 11:00am Coffee Break

11:00am -- 12:00 noon Chengguo GUAN

Nanjing Institute of Geology and Palaeontology, CAS, China

PALEOBIOLOGY: LANTIAN FM., CHINA Geological setting and paleoecology of Ediacarian Lantian carbonaceous and pyritized macrofossils

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12:00 noon -- 1:30pm Lunch (on site)

1:30pm -- 2:30pm Chen YOU

National Cheng Kung University, Tainan City, Taiwan

PALEOBIOLOGY: LANTIAN FM., CHINA Geochemical, including Boron analyses of Ediacarian Lantian carbonates and shales

3:15pm -- 4:15pm Volodya SERGEEV

Geological Institute, Russian Academy of Sciences, Moscow, Russia

PALEOBIOLOGY: CHULAKTAU FM, KAZAKHSTAN Geological setting,

paleoecology and biological affinities of apatite-permineralized microfossils of the Early Cambrian Chulaktau Formation, southern Kazakhstan

4:15pm -- 5:00 pm GROUP DISCUSSION

Paleobiology of the Doushantuo, Lantian & Chulaktau Fms -- unanswered questions

WEDNESDAY 14 SEPTEMBER

7:30am – 8:30 am Coffee and pastries/donuts, CSEOL Library UCLA (Room 5681 Geology Building)

NOVEL ANALYTICAL TECHNIQUES &APPLICATIONS

8:30am -- 9:30am Bill SCHOPF

University of California, Los Angeles, USA

NOVEL TECHNIQUES – CLSM and Raman and Fluorescence

Spectroscopy: Apatitic fossils of the Early Cambrian Kuanchuanpu Fm (China), Proterozoic Fifteenmile Grp (Yukon), and Early Cambrian Chulaktau Fm (Kazakhstan)

9:30am --10:30am Ken WILLIFORD

NASA Jet Propulsion Laboratory, Pasadena, California, USA

NOVEL TECHNIQUES – Secondary Ion Mass Spectroscopic (SIMS):

Analyses of Stable Isotopes: Sulfur and carbon isotopic studies of individual microscopic fossils

10:30am -- 11:00am Coffee Break 11:00am -- 12:00 noon Amanda GARCIA

University of California, Los Angeles, USA

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NOVEL TECHNIQUES: Progress Report on an apatite-based potential barometer of ambient O2 at the Precambrian-Cambrian transition 12:00 noon -- 12:45pm GROUP DISCUSSION

Questions about techniques? Other techniques we should apply?

12:45pm -- 2:00pm Lunch (on site)

2:00pm – 3:30pm SUMMARY GROUP DISCUSSION Yanan SHEN (Discussion Leader)

University of Science and Technology of China, Hefei. China Status of our work - what do we know?

What are the unanswered questions?

4:00pm – 5:00pm CONCLUDNG GROUP DISCUSSION Bill SCHOPF (Discussion Leader)

University of California, Los Angeles, USA How should we proceed?

Future group meeting September 2017?

==========================================================

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二、與會心得

此次會議的重點著重於過去研究結果的發表與未來方向的討論，會中各成員充分溝通、分享其專業經驗，會議雖然只有短短三天，但收穫卻出奇的豐碩。主要心得整理如下:

1. Doushantuo 以及 Chulaktau 地層中的微體古生物在此會議中詳細的探討其產狀和可能成因，有助於前寒武紀和寒武紀早期海洋環境的變化以及生命的演化。並找到了目前最古老的完整海綿化石，此化石以同步輻射詳細測繪其三維型態﹑成果發表於 PNAS。未來此團隊將著重於研究化石埋藏學以及新種的鑑定。

2. 新的研究工具如高精確硫同位素分析、二次離子質譜儀、共軛焦拉曼光譜

儀以及同步輻射等，使微體古生物學進入了一個全新的研究世紀。不僅可以獲取詳細的三維化石形貌，也可以了解化石的微區元素及同位素組成。可獲得了解化石的成因及重建古環境重要資訊。

3. 磷灰石定年結果不如預期，主要原因在於樣品中的磷灰石鈾的含量太低，

僅理想濃度的 1/100~1/10；且初始鉛濃度過高。將另外挑選適合樣品繼續嘗試放射性鈾鉛定年。

4. 磷灰石中釤元素的拉曼吸收峰有希望作為一個氧分壓紀錄器，可用以重建

早期地球(寒武紀以前）大氣組成的改變。

在此特別致謝「科技部」補助筆者出席此次國際會議，除了跟研究團隊分享過去的研究成果外，也和與會者討論未來方向，了解最新的研究趨勢，獲益良多。

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三、發表論文全文或摘要

The purpose of this trip is to attend a science working group meeting-- PALEOENVIRONMENT AND AMBIENT OXYGEN DURING THE

PRECAMBRIAN-CAMBRIAN TRANSITION held at the Department Earth and Space Sciences, UCLA. The aims of the meeting are: (1) to become acquainted with one another and each other’s expertise;(2) to identify the problems that we need to address; (3) to see where we stand on trying to solve those problems; and (4) to define a path for our ongoing studies. The meeting included numerous group discussions and is intended to be an informal and highly interactive get-together with lots of

interruptions/questions/ replies, give-and-take and active discussion. The participants are diverse (including expertise in geology, geochronology, isotopic and organic geochemistry, paleoecology, paleontology and biology) and is notably international (China, Taiwan, Russia, USA), all involved helping others to solve the pressing problems.

四、建議

應多多鼓勵、補助學者參與類似研討會。

五、攜回資料名稱及內容

會議演講題目及 Chulaktau 地層論文集六、其他

無

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105年度專題研究計畫成果彙整表

計畫主持人：游鎮烽計畫編號：105-2116-M-006-011- 計畫名稱：非傳統穩定鍶同位素在陸地風化過程中所產生的同位素分化作用(5/5)

成果項目量化單位

質化

（說明：各成果項目請附佐證資料或細項說明，如期刊名稱、年份、卷期、起訖頁數、證號...等）　　　　　　　

國

內學術性論文期刊論文 7 篇

H.C. Liu, C.F. You, H. Zhou, K.F.

Huang, C.H. Chung, W.J. Huang and J. Tang (2017) Effect of calcite precipitation on stable strontium isotopic compositions: Insights from riverine and pool waters in a karst cave". Chemical Geology 456 (2017) 85–97.

HC Liu, CH Chung, CF You* and YH Chiang (2015) Determination of 87Sr/86Sr and δ88/86Sr ratios in plant materials using MC-ICP-MS Anal Bioanal Chem DOI

10.1007/s00216-015-9070-y (IF 3.44, 13/74 in Chemistry: analytical) Ju-Lien Pi, Chen-Feng You and Kuo- Lung Wang (2016) The influence of Ryukyu subduction on magma genesis in the Northern Taiwan Volcanic Zone and Middle Okinawa

Trough—Evidence from boron

isotopes, Lithos 260 242–252 (SCI, IF 4.482, 6/79 in Geophysical &

Geochemical)

Gaojun Li, Jens Hartmann, Louis A.

Derry, A. Joshua West , Chen-Feng You, Xiaoyong Long, Tao Zhan, Laifeng Li, Gen Li, Wenhong Qiu , Tao Li, Lianwen Liu, Yang Chen, Junfeng Ji, Liang Zhao, Jun Chen (2016) Temperature dependence of basalt weathering. Earth and

Planetary Science Letters 443, 59- 69 (SCI, IF 4.72, 5/79 in

Geophysical & Geochemical)

S. K. Aggarwal and C.F.You (2017) A review on the determination of isotope ratios of boron with mass spectrometry (2016) Mass

Spectrometry Review 2017, 36, 499- 519 (IF 9.373, 1/41 in

SPECTROSCOPY)

K. J. Meyer, A. E. Carey, C.F. You (2017) Typhoon impacts on chemical

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weathering source provenance of a high standing island watershed, Taiwan, Geochimica et Cosmochimica Acta 215, 404-420. (SCI, IF 4.61, 5/83) in GEOCHEMISTRY &

GEOPHYSICS).

SF Wu, CF You, Yen-Po Lin, Eugenia Valsami-Jones and Emmanuel

Baltatzis (2016) New Boron Isotopic Evidence for Sedimentary and

Magmatic Fluid Influence in the Shallow Hydrothermal Vent System of Milos Island (Aegean Sea, Greece) Journal of Volcanology and

Geothermal Research, 310, 58–71 (IF 2.54, 47/175 in GEOSCIENCES, MULTIDISCIPLINARY)

Yao-Jen Tu, Ting-Shan Chan, Hao-Wei Tu, Shan-Li Wang, Chen-Feng You, Chien-Kuei Chang (2016) Rapid and Efficient Removal/Recovery of Mo

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