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  1. NTU Theses and Dissertations Repository
  2. 理學院
  3. 地質科學系
請用此 Handle URI 來引用此文件: http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/34176
完整後設資料紀錄
DC 欄位值語言
dc.contributor.advisor沈川洲(Chuan-Chou Shen)
dc.contributor.authorYu-Te Hsiehen
dc.contributor.author謝玉德zh_TW
dc.date.accessioned2021-06-13T05:57:00Z-
dc.date.available2007-07-03
dc.date.copyright2006-07-03
dc.date.issued2006
dc.date.submitted2006-06-28
dc.identifier.citationAndersen, M. B., Stirling, C. H., Potter, E.-K., and Halliday, A. N. (2004) Toward epsilon levels of measurement precision on 234U/238U by using MC-ICPMS. International Journal of Mass Spectrometry 237, 107-118.
Banner, J. L., Wasserburg, G. L., Chen, J. H., and Moore, C. H. (1990) 234U-238U-230U-232Th systematics in saline groundwaters from central Missouri. Earth and Planetary Science Letters 101 (2-4), 296-312.
Barnes, J. W., Lang, E. J., and Potratz, H. A. (1956) Ratio of ionium to uranium in coral limestone. Science 124, 175-176.
Bourdon, B., Henderson, G. M., Lundstrom, C. C., Turner, S. P. (2003) Uranium-Series Geochemistry, The Mineralogical Society of America, Washington, DC, USA.
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Chen, J. H., Edwards, R. L., and Wasserburg, G. J. (1986) 238U, 234U and 232Th in seawater. Earth and Planetary Science Letters 80 (3-4), 241-251.
Cheng, H., Edwards, R. L., Hoff, J., Gallup, C. D., Richards, D. A., and Asmerom, Y. (2000) The half-lives of uranium-234 and thorium-230. Chemical Geology 169, 17-33.
Delanghe, D., Bard, E., and Hamelin, B. (2002) New TIMS constraints on the uranium-238 and uranium-234 in seawaters from the main ocean basins and the Mediterranean Sea. Marine Chemistry 80 (1), 79-93.
Deschamps, P., Doucelance, R., Ghaleb, B., and Michelot, J.-L. (2003) Further investigations on optimized tail correction and high-precision measurement of uranium isotopic ratios using multi-collector ICP-MS. Chemical Geology 201,
141-160.
Edwards, R. L., Chen, J. H., and Wasserburg, G. J. (1986/87) 238U-234U-230Th-232Th systematics and the precise measurement of time over the past 500,000 years. Earth and Planetary Science Letters 81, 175-192.
Edwards, R. L. (1988) High precision thorium-230 ages of corals and the timing of sea level fluctuation in the late Quaternary. PhD thesis, California Institute of Technology.
Edwards, R. L., Beck, J. R., Burr, G. S., Donahue, D. J., Chappell, J. M. A., Bloom, A. L., Druffel, E. R. M., and Taylor, F. W. (1993) A large drop in atmospheric 14C/12C and reduced melting in the Younger Dryas, documented with 230Th ages of corals. Science 260, 962-968.
Eisenhauer, A., Wasserburg, G. J., Chen, J. H., Bonani, G., Collins, L. B., Zhu, Z. R., and Wyrwoll, K. H. (1993) Holocene sea-level determination relative to the Australian continent: U/Th (TIMS) and 14C (AMS) dating of coral cores from the Abrolhos Islands. Earth and Planetary Science Letters 114, 529-547.
Goldstein, S. J. and Stirling, C. H. (2003) Techniques for measuring uranium-series nuclides: 1992-2002. Reviews in Mineralogy and Geochemistry 52, 23-57.
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Robinson, L. F., Belshaw, N. S., and Henderson, G. M. (2004) U and Th concentrations and isotope rations in modern carbonates and waters from the Bahamas. Geochimica et Cosmochimica Acta 68, 1777-1789.
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Shen, C.-C., Edwards, R. L., Cheng, H., Dorale, J. A., Thomas, R. B., Moran, S. B., Weinstein, S. E., and Edmonds, H. N. (2002) Uranium and thorium isotopic and concentration measurements by magnetic sector inductively coupled plasma mass spectrometry. Chemical Geology 185, 165-178.
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Stein, M., Wasserburg, G. L., Lajoie, K. R., and Chen, J. H. (1991) U-series ages of solitary corals from the California coast by mass spectrometry. Geochimica et Cosmochimica Acta 55, 3709-3722.
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the timing and duration of the Last Interglacial. Earth and Planetary Science Letters 135, 115-130.
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Walder, A. J., Koller, D., Reed, N. M., Hutton, R. C., and Freedman, P. A. (1993) Isotope ratio measurement by inductively coupled plasma multiple collector mass spectrometry incorporating a high efficiency nebulization system. Journal of Analytical Atomic Spectrometry 8, 1037-1041.
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dc.identifier.urihttp://tdr.lib.ntu.edu.tw/jspui/handle/123456789/34176-
dc.description.abstract本研究利用多偵測器感應耦合電漿質譜儀發展了一套精準的鈾同位素比值及含量測量技術,精確度可達萬分比等級。我們使用四個法拉第杯同時測量鈾同位素, 233U, 234U, 235U, 及236U。利用233U-236U 雙示蹤劑有效校正質量分化效應以及計算鈾濃度。複雜之背景干擾,主要因不同238U 訊號、真空狀況及基質而改變外,亦235U 拖尾所影響,故同位素之背景值必須個別校正。若以簡單的指數行為描述背景頻譜,對233U, 234U 及236U的訊號強度,將造成萬分比至千分比的錯估。以進樣速率為每分鐘50 ml,測量鈾濃度2 ppm 約2-6 分鐘,僅需200-600 ng U 的標本量,δ234U 和鈾含量的測量精準度可達± 0.1-0.5‰ (2σ)。分析國際及實驗室之標準品,長時間之δ234U 及鈾含量測定重現性分別可達0.12‰及0.47‰,且與其他質譜術量測數值相吻合。重複分析國際標準品NBL-112A 和HU-1 的δ234U 平均結果分別為-37.10 ± 0.03‰ (2σm, n = 17) 和-0.17 ± 0.05‰ (2σm, n = 5)。自然界具有不同基質之各種珊瑚及洞穴石筍碳酸鹽樣品的δ234U 及鈾濃度測量值與其他千分比準度之質譜術所得數值一致。此分析技術將可應用至鈾系定年法,古氣候學,及岩石地球化學之相關研究。zh_TW
dc.description.abstractTechniques used for precise and accurate determination of natural uranium isotopic ratios and concentration with sub-permil precision have been developed on a multi-collector inductively coupled plasma mass spectrometer (MC-ICP-MS), Thermo Electron NEPTUNE. Uranium isotopes, 233U, 234U, 235U, and 236U, were statically measured in 4 Faraday collectors. A 233U-236U double spike method was employed to correct mass bias and determine uranium concentration. The behavior of complicated spectral background is attributed to tailing characteristics of 235U and 238U ion beams as well as vacuum condition and matrix effect. Individual background correction should be applied to the measured isotopes, 233U, 234U, and 236U, or a bias of sub-permil to permil level could be caused by using a simple exponential function correction. By introducing 2 ppm uranium with a uptake rate of 50 ml/min for 2-6 minutes, a sample size of 200-600 ng U is needed to offer a within-run precision of 0.1-0.5‰ for d234U and uranium concentration. Measurements made on reference materials and in-house standards demonstrate that an external reproducibility of 0.12‰ can be achieved for d234U and 0.47‰ for uranium concentration. Repeated measurements of NBL-112A and HU-1 give averaged d234U values of -37.10 ± 0.03‰ (2σm, n = 17) and -0.17 ± 0.05‰ (2σm, n =5), respectively, within error of accepted values. MC-ICP-MS data of d234U and uranium concentration for different carbonates, including corals and speleothems with various matrices, are in agreement with those measured by other mass spectrometric methods with a permil-level precision. This technique can be applied to the exploration of the frontiers in diverse fields of Earth Sciences, such as U series chronology, paleoclimatology, and geochemistry.en
dc.description.provenanceMade available in DSpace on 2021-06-13T05:57:00Z (GMT). No. of bitstreams: 1
ntu-95-R93224102-1.pdf: 606184 bytes, checksum: bab6ce70e21bdbd2ed263452bc5d4b90 (MD5)
Previous issue date: 2006
en
dc.description.tableofcontentsList of Figures ...III
List of Tables ...V
摘要(Abstract in Chinese) ...1
Abstract ...2
Chapter 1 Introduction ...3
Chapter 2 Experimental Methods ...6
2.1 Materials and chemistry ...6
2.1.1 Standards and samples ...6
2.1.2 Chemistry ...6
2.2 Instrumentation ...7
2.2.1 MC-ICP-MS ...7
2.2.2 Introduction system ...8
2.3 Detector calibration ...9
2.3.1 Faraday cup: gain and baseline ...9
2.3.2 SEM: yield and dead time ...9
2.4 Spectral interference ...10
2.4.1 Instrumental memory blank ...10
2.4.2 Scattering of reflected 238U ions ...11
2.4.3 238U and 235U tailing ...13
2.5 Analytical procedure ...14
2.5.1 Analysis protocols ...14
2.5.2 Measurement sequence ...15
2.5.3 Data acquisition ...16
2.5.4 Off-line data reduction ...17
Chapter 3 Results and Discussion ...18
3.1 Background correction for U tailing ...18
3.1.1 Behaviors of 235U and 238U tailing ...18
3.1.2 Correction of tailing background ...19
3.1.3 Mixtures of standard and 233U-236U tracer ...23
3.2 Precision and accuracy ...24
3.2.1 Protocol-1 with 6S-jumping mode ...24
3.2.2 Protocol-1 with 2S-jumping mode ...24
3.2.3 Comparison between the 6-step and the 2-step jumping modes ...26
3.2.4 Protocol-2 ...28
3.3 Natural carbonate standards and samples ...29
3.4 Comparison with other mass spectrometric techniques ...34
Chapter 4 Conclusions ...37
References ...38
Acknowledgments ...42
dc.language.isoen
dc.subject多偵測器感應耦合電漿質譜儀zh_TW
dc.subject同位素zh_TW
dc.subject鈾zh_TW
dc.subject雙示蹤劑法zh_TW
dc.subject拖尾效應校正zh_TW
dc.subject法拉第杯zh_TW
dc.subject濃度zh_TW
dc.subjectMC-ICP-MSen
dc.subjectUraniumen
dc.subjectIsotopeen
dc.subjectConcentrationen
dc.subjectDouble spike methoden
dc.subjectTail correctionen
dc.subjectFaraday cupen
dc.title多偵測器感應耦合電漿質譜儀之精準鈾含量及同位素比值測量技術zh_TW
dc.titleAccurate and precise determination of uranium concentration and isotopic composition by multi-collector inductively coupled plasma mass spectrometryen
dc.typeThesis
dc.date.schoolyear94-2
dc.description.degree碩士
dc.contributor.oralexamcommittee羅尚德(Shangde Luo),扈治安(Chin-An Huh),沈君山(Jiun-San Shen)
dc.subject.keyword鈾,同位素,濃度,雙示蹤劑法,拖尾效應校正,法拉第杯,多偵測器感應耦合電漿質譜儀,zh_TW
dc.subject.keywordUranium,Isotope,Concentration,Double spike method,Tail correction,Faraday cup,MC-ICP-MS,en
dc.relation.page42
dc.rights.note有償授權
dc.date.accepted2006-06-29
dc.contributor.author-college理學院zh_TW
dc.contributor.author-dept地質科學研究所zh_TW
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