An improved method for mobile characterisation of δ13CH4 source signatures and its application in Germany

An improved method for mobile characterisation of δ13CH4 source signatures and its application in Germany
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δ13​​CH4源特征移动表征的改进方法及其在德国的应用

DOI:
10.5194/amt-12-1123-2019
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发表时间:
2019
影响因子:
3.8
通讯作者:
M. Schmidt
M. Schmidt
中科院分区:
地球科学3区
文献类型:
--
作者:
A. Hoheisel;C. Yeman;F. Dinger;Henrik Eckhardt;M. Schmidt

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抽象的。几种甲烷的碳同位素特征(δ~(13)CH_4) 德国(海德堡周围和北莱茵-威斯特伐利亚)的消息来源是 有特点的。对甲烷源的羽流进行了流动测量 使用基于腔衰荡光谱(CRDS)的分析器。为了达到精确的结果 CRDS分析仪,用于测量甲烷(CH4)、二氧化碳(CO2)和 他们的13C与12C的比率,特别是关于 气体基质在空气中组成差异的交叉敏感性 样品或校准罐。两种最重要的气体会影响 δ13CH4是水蒸气(H2O)和乙烷(C2H6)。至 避免与水的交叉敏感,空气用Nafion烘干机烘干 在移动测量期间。C2H6通常富含天然气。 因此,在甲烷羽流或源自天然气的样本中也是如此。一个 C2H6的校正和校准是获得准确的 δ13CH4结果,偏差最高可达3 ‰ 取决于是否应用了C2H6校正。同位素特征是用Miller-Tans方法确定的, 约克拟合法。在21场野战中,平均数 三个奶牛场的δ13CH4签名 (-63.9±0.9‰),沼气厂 (-62·4±1·2‰),垃圾填埋场 (-58·7±3·3‰),污水处理厂 (-52.5±1.4‰),一个活跃的深部煤矿 (-56.0±2.3‰)和两个天然气储存和天然气压缩机 记录站数(-46.1±0.8‰)。此外,2016年12月至2018年11月期间,来自 海德堡天然气配气网络的平均测定值 δ13CH4值为-43.3±0.8‰。与…相反 Levin等人在1991至1996年间的先前测量。(1999),编号 表现出较强的季节性循环。
Abstract. The carbon isotopic signature (δ13CH4) of several methane sources in Germany (around Heidelberg and in North Rhine-Westphalia) were characterised. Mobile measurements of the plume of CH4 sources are carried out using an analyser based on cavity ring-down spectroscopy (CRDS). To achieve precise results a CRDS analyser, which measures methane (CH4), carbon dioxide (CO2) and their 13C-to-12C ratios, was characterised especially with regard to cross sensitivities of composition differences of the gas matrix in air samples or calibration tanks. The two most important gases which affect δ13CH4 are water vapour (H2O) and ethane (C2H6). To avoid the cross sensitivity with H2O, the air is dried with a Nafion dryer during mobile measurements. C2H6 is typically abundant in natural gases and thus in methane plumes or samples originating from natural gas. A C2H6 correction and calibration are essential to obtain accurate δ13CH4 results, which can deviate by up to 3 ‰ depending on whether a C2H6 correction is applied. The isotopic signature is determined with the Miller–Tans approach and the York fitting method. During 21 field campaigns the mean δ13CH4 signatures of three dairy farms (-63.9±0.9‰), a biogas plant (-62.4±1.2‰), a landfill (-58.7±3.3‰), a wastewater treatment plant (-52.5±1.4‰), an active deep coal mine (-56.0±2.3‰) and two natural gas storage and gas compressor stations (-46.1±0.8‰) were recorded. In addition, between December 2016 and November 2018 gas samples from the Heidelberg natural gas distribution network were measured with a mean δ13CH4 value of -43.3±0.8‰. Contrary to previous measurements between 1991 and 1996 by Levin et al. (1999), no strong seasonal cycle is shown.
DOI: 10.3390/s16101638
发表时间: 2016-10-03
期刊: Sensors (Basel, Switzerland)
影响因子: --
作者:
Schmithausen AJ;Trimborn M;Büscher W
通讯作者: Büscher W