Study on Oxidation Rate and Isotope Fractionation of Methane in Bohai Sea Sediments
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摘要: 渤海蕴藏着大量的油气资源，其主要成分是温室气体甲烷，自然环境下或人为因素的影响会引起其泄露与迁移，对环境造成负面的影响。但是，泄露与迁移过程中微生物会氧化绝大部分甲烷，而不同的环境条件会影响氧化过程中的速率及碳同位素分馏过程。为了更好地认识渤海沉积物中甲烷氧化规律和同位素分馏规律以及为进一步研究此区域的甲烷氧化提供参考，本文选取渤海沉积物作为进行实验室模拟降解实验原料，借助气相色谱和气相色谱-同位素比值质谱仪测定渤海沉积物中的甲烷氧化速率，确定了甲烷氧化碳同位素分馏系数ε。结果表明：渤海沉积物中甲烷氧化作用以好氧氧化占主导，氧化温度和气体流速是影响甲烷氧化速率的主要因素。在连续培养的模式下，当温度由28℃降至15℃时，甲烷的平均氧化速率降低60%±10%，即温度越低越不利于甲烷氧化作用的发生。而气体流速由50 μL/min增加至150 μL/min时，甲烷的平均氧化速率增加90%±10%，即增加气体流速有利于氧化反应速率的提高。实验还发现，甲烷碳、氢同位素的分馏效应主要受氧化温度制约，分馏程度与温度呈正相关。实验结论认为温度是影响甲烷氧化速率和同位素分馏规律的重要因素。Abstract:
BACKGROUND The Bohai Sea contains a large amount of oil and gas, the main component of which is methane. The influence of natural or human factors will cause its leakage and migration and then have a negative impact on the environment. However, most of the methane would be oxidized by microorganisms during the leakage and migration processes. Meanwhile, the different environmental conditions will affect oxidation rate and carbon isotope fractionation of methane. OBJECTIVE In order to better understand the law of isotope fractionation and methane oxidization in the sediments and to provide reference for further related research in this area, the Bohai Sea sediments were selected as laboratory raw materials for the degradation of laboratory experiments and are described in this paper. METHODS Gas Chromatography and Gas Chromatography-Isotope Ratio Mass Spectrometry were used to determine the methane oxidation rate, and the carbon isotope fractionation coefficient ε of methane was determined. RESULTS The results show that the aerobic oxidation of methane is dominant. Oxidation temperature and gas flow rate are the main factors affecting the rate of methane oxidation. In the mode of continuous incubation, when the temperature reduced from 28℃ to 15℃, the average oxidation rate reduced by 60%±10%, indicating that the lower temperature is not helpful for methane oxidation. When the gas flow rate increases from 50 to 150 μL/min, the average oxidation rate of methane increases by 90%±10%. This indicates that the higher gas flow rate is favorable to the increase of oxidation rate. It is also found that the fractionation effect of carbon and hydrogen isotopes are mainly affected by temperature where the fractionation degree is positively correlated with temperature. CONCLUSIONS Temperature is an important factor affecting methane oxidation rate and isotopic fractionation. -
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表 1 不同实验条件CH4实验时间及氧化速率
Table 1. Experiment time and oxidation rate of CH4 in different experimental conditions
培养方式 摇床转速或气体流速 实验温度(℃) 实验时间(天) 氧化速率(μmol/g·d-1) 适应期 对数期 平均值 分批氧化 50 r/min 28 27 0.18 (0~10天) 1.48 (10~27天) 1.14 连续氧化 50 μL/min 28 24 0.42 (0~7天) 1.31 (7~24天) 1.05 连续氧化 50 μL/min 15 74 0.25 (0~46天) 0.40 (46~74天) 0.34 连续氧化 150 μL/min 28 14 0.52 (0~5天) 2.29 (3~15天) 1.90 
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