In situ Raman spectroscopic measurement of the 13 C/12 C ratio of dissolved CO2 at high temperatures and pressures: Method and implications
文献类型：期刊论文
| 作者 | Ge, Yuzhou1,2,3,4; Luan, Zhendong1,2,3,4; Li, Lianfu2,3,4; Xi, Shichuan2,3,4; Du, Zengfeng1,2,4; Zhang, Xin1,2,3,4 |
| 刊名 | GEOSCIENCE FRONTIERS
 |
| 出版日期 | 2026 |
| 卷号 | 17期号:1页码:15 |
| 关键词 | Raman spectroscopy C-13/C-12 ratio Dissolved CO2 In situ Quantitative analysis High temperature and pressure experiment |
| ISSN号 | 1674-9871 |
| DOI | 10.1016/j.gsf.2025.102180 |
| 通讯作者 | Zhang, Xin(xzhang@qdio.ac.cn) |
| 英文摘要 | Submarine hydrothermal activities release a large amount of greenhouse gases such as CO2 and CH4 into the ocean, influencing the global carbon cycle. Carrying out high-temperature and high-pressure hydrothermal experiments to simulate these geochemical processes is a prerequisite for clarifying the source of carbon-containing substances in the hydrothermal fluid. In situ monitoring of the change in carbon isotope composition of CO2 is essential for high-temperature and high-pressure simulation experiments, but it is also a great technical challenge. In recent years, laser Raman spectroscopy has attracted wide attention as a supplementary means to mass spectrometry for measuring the 13C/12C value of CO2. However, the existing research is limited to the Raman spectroscopy study of the carbon isotope composition of supercritical/liquid CO2, and there is little research on dissolved CO2 in solution. In this study, we systematically studied the Raman spectral characteristics of dissolved 13CO2 and 12CO2 in the H2O +/- 13CO2 +/- 12CO2 system at 25-300 degrees C and 10-350 bar. The results show that the peak position of the Raman characteristic band of 13CO2 (aq) is 1367-1370 cm-1, which is 14-17 cm-1 lower than that of 12CO2 (aq), and the full width at half maximum is 2-3 cm-1 smaller than that of 12CO2, which indicate the 13CO2 (aq) and 12CO2 (aq) can be identified by Raman spectroscopy. On this basis, we proposed the optimal likelihood curve fitting method (OLCF) for the first time to decompose the overlapping bands and accurately obtain the peak height ratio (H13/H12) of dissolved 13CO2 and 12CO2. It has been shown that the G-factor ratios (G13/G12) are significantly affected by temperature and the relative content of 13CO2 and 12CO2. Obtaining an appropriate G-factor ratio is a prerequisite for accurately determining the 13C/12C of dissolved CO2. Based on the functional relationship between the H13/H12 and the 13C/12C, we established an empirical equation to quickly estimate the 13C/12C value, thereby assisting in selecting an appropriate G-factor ratio. The calibrated G-factor can be well used to determine the 13C/12C of dissolved CO2 in the hydrothermal experiments with 13C labelled. In-situ monitoring experiments show that the phase separation of the hydrothermal fluid hardly causes changes in the carbon isotope composition of dissolved CO2. However, the contamination of organic matter, such as oxalic acid, will result in a higher content and amore negative d13C of CO2 in the hydrothermal fluids. (c) 2025 China University of Geosciences (Beijing) and Peking University. Published by Elsevier B.V. on behalf of China University of Geosciences (Beijing). This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/). |
| WOS关键词 | CARBON-ISOTOPE FRACTIONATION ; HOSTED HYDROTHERMAL SYSTEMS ; ABIOTIC ORGANIC-SYNTHESIS ; O-H-N ; QUANTITATIVE-ANALYSIS ; FLUID INCLUSIONS ; PHASE-SEPARATION ; VENT FLUIDS ; OXALIC-ACID ; EXPERIMENTAL CALIBRATION |
| 资助项目 | National Natural Science Foundation of China[42327805] ; National Natural Science Foundation of China[92358301] ; National Natural Science Foundation of China[42221005] ; National Natural Science Foundation of China[42206190] ; Natural Science Foundation of Shandong Province[ZR2024MD012] |
| WOS研究方向 | Geology |
| 语种 | 英语 |
| WOS记录号 | WOS:001604874700001 |
| 出版者 | CHINA UNIV GEOSCIENCES, BEIJING |
| 源URL | [http://ir.qdio.ac.cn/handle/337002/203722]  |
| 专题 | 海洋研究所_深海极端环境与生命过程研究中心 |
| 通讯作者 | Zhang, Xin |
| 作者单位 | 1.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 2.Chinese Acad Sci, Inst Oceanol, Ctr Deep Sea Res, Ctr Ocean Mega Sci, Qingdao 266071, Peoples R China 3.LaoShan Lab, 168 Wanhai Middle Rd, Qingdao 266237, Shandong, Peoples R China 4.Chinese Acad Sci, Inst Oceanol, Ctr Ocean Mega Sci, CAS Key Lab Marine Geol & Environm, Qingdao 266071, Peoples R China |
| 推荐引用方式 GB/T 7714 | Ge, Yuzhou,Luan, Zhendong,Li, Lianfu,et al. In situ Raman spectroscopic measurement of the 13 C/12 C ratio of dissolved CO2 at high temperatures and pressures: Method and implications[J]. GEOSCIENCE FRONTIERS,2026,17(1):15. |
| APA | Ge, Yuzhou,Luan, Zhendong,Li, Lianfu,Xi, Shichuan,Du, Zengfeng,&Zhang, Xin.(2026).In situ Raman spectroscopic measurement of the 13 C/12 C ratio of dissolved CO2 at high temperatures and pressures: Method and implications.GEOSCIENCE FRONTIERS,17(1),15. |
| MLA | Ge, Yuzhou,et al."In situ Raman spectroscopic measurement of the 13 C/12 C ratio of dissolved CO2 at high temperatures and pressures: Method and implications".GEOSCIENCE FRONTIERS 17.1(2026):15. |
入库方式： OAI收割
来源：海洋研究所
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