In situ Raman spectroscopic measurement of the 13C/12C ratio in CO2: Experimental calibrations on the effects of fluid pressure, temperature and composition
Wenwen Lu3; Xiaolin Wang1,3,4; Qian Wan3; Wenxuan Hu1,3,4; I-Ming Chou2; Ye Wan2
刊名Chemical Geology
2023-01-05
卷号615期号:2023页码:121201
关键词Raman spectroscopy 13C 12C ratio CO2 Experimental calibration T-P-x influences
ISSN号0009-2541
DOI10.1016/j.chemgeo.2022.121201
英文摘要

The carbon isotope (delta 13C) signature of CO2 within fluid inclusions is of significance to investigate because it can be used to decipher the carbon source of geological fluids. Raman spectroscopy has been applied to determine the delta 13C of pure CO2. However, whether this approach can be applied to natural inclusions with complex compo-sitions remains unknown. Here we present Raman spectra of CO2 +/- N2 +/- CH4 systems with known 13C/12C ratio (0.01-1.12) at temperatures (T) of 21 degrees C and 40 degrees C and at pressures (P) ranging from 0.5 to 50 MPa. Peak areas and peak heights of the 13CO2 (-1370 cm -1) and 12CO2 (-1285 cm-1) bands were determined to calculate the Raman spectroscopic quantification factors (F-and G-factor ratio). The results show that the quantification factors vary significantly with rising pressure in the low pressure range (e.g., <10 MPa), especially for pure CO2 system. Different fluid systems are characterized by pressure dependences. Specifically, both F-and G-factor ratios for CO2 fluid with a low 13C/12C ratio (e.g., 0.01) are different from that with a high 13C/12C ratio (e.g., 0.13) under the same T -P conditions. Fluid temperature does not result in significant variation in F-or G-factor ratios at the investigated temperatures. Based on these calibrations, we suggest that fluid pressure and compo-sition (x) are prerequisites for Raman spectroscopic measurements of the 13C/12C ratio of CO2. However, the 13CO2 (-1370 cm-1) band for CO2 from natural fluid inclusions is characterized by low Raman intensity, resulting in large errors in calculated peak area and peak height. Thus, accurate determination of the 13C/12C ratio of fluid inclusion CO2 is not feasible for inclusions with low CO2 density. Nevertheless, this method can be applied to investigate the carbon isotope fractionation in 13C labelled hydrothermal experiments, where CO2 with high a 13C/12C ratio is produced.

资助项目National Key Research and Development Program of China[2022YFF0800403] ; National Natural Science Foundation of China[41830425] ; National Natural Science Foundation of China[41922023] ; National Natural Science Foundation of China[42173038] ; Research Funds for the Frontiers Science Center for Critical Earth Material Cycling (Nanjing University) ; Fundamental Research Funds for the Central Universities[2022300192]
WOS关键词THERMOCHEMICAL SULFATE REDUCTION ; CARBON-ISOTOPE FRACTIONATION ; FUSED-SILICA CAPILLARIES ; O-H-N ; GAS-MIXTURES ; QUANTITATIVE COMPOSITION ; DETECTION LIMITS ; AQUEOUS FLUIDS ; SICHUAN BASIN ; QUARTZ VEINS
WOS研究方向Geochemistry & Geophysics
语种英语
出版者ELSEVIER
WOS记录号WOS:000895506800004
资助机构National Key Research and Development Program of China ; National Natural Science Foundation of China ; Research Funds for the Frontiers Science Center for Critical Earth Material Cycling (Nanjing University) ; Fundamental Research Funds for the Central Universities
内容类型期刊论文
源URL[http://ir.idsse.ac.cn/handle/183446/9982]  
专题深海科学研究部_深海极端环境模拟研究实验室
作者单位1.State Key Laboratory for Mineral Deposits Research, Nanjing University
2.Institute of Deep-sea Science and Engineering, Chinese Academy of Sciences
3.School of Earth Sciences and Engineering, Nanjing University
4.Frontiers Science Center for Critical Earth Material Cycling, Nanjing University
推荐引用方式
GB/T 7714
Wenwen Lu,Xiaolin Wang,Qian Wan,et al. In situ Raman spectroscopic measurement of the 13C/12C ratio in CO2: Experimental calibrations on the effects of fluid pressure, temperature and composition[J]. Chemical Geology,2023,615(2023):121201.
APA Wenwen Lu,Xiaolin Wang,Qian Wan,Wenxuan Hu,I-Ming Chou,&Ye Wan.(2023).In situ Raman spectroscopic measurement of the 13C/12C ratio in CO2: Experimental calibrations on the effects of fluid pressure, temperature and composition.Chemical Geology,615(2023),121201.
MLA Wenwen Lu,et al."In situ Raman spectroscopic measurement of the 13C/12C ratio in CO2: Experimental calibrations on the effects of fluid pressure, temperature and composition".Chemical Geology 615.2023(2023):121201.
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