A hydrogen preconcentration equipment was developed to separate and enrich the microhydrogen in natural gases with molecular sieve trap at 77 K and 159 K. The enriched hydrogen was carried into GC-isoto ratio mass spectrometric (IRMS) system by carrier gas to analyze the isotope composition. This on-line continuous-flow process can overcome the difficulty for the determination of micro-hydrogen in natural gases. A set of manual standard samples were analyzed by the method. The results show the method is applicable for the 1 ×10-5 (V/V) hydrogen in the sample and has a good reproductivity and linearity, the relative standard deviation is less than 3. 3‰. Using this method, the six gas samples from different oil-gas-bearing basins were analyzed. Further more, the isotope composition origin of hydrogen in natural gas was discussed.%为实现天然气中丰度很低的氢同位素分析,自制氢气富集分离装置,利用在159和77 K温度条件下5A分子筛对不同气体组分的物理吸附性能差异,使天然气样品中微痕量氢与烃类组分分离,并进一步富集后,由载气送入色谱-同位素质谱计系统,分析其同位素组成.分析过程为在线连续流模式,与色谱同位素质谱工作站联动控制,从根本上解决了微痕量氢同位素分析的技术瓶颈.采用本方法分析了已知氢同位素组成的不同浓度人工混合样品,结果表明,本分析方法具有较高的精确度和良好线性,能够满足天然气中氢浓度低至1×10-5(V/V)样品准确分析的要求,标准偏差小于3.3‰.用此方法对不同含油气盆地6个天然气样品进行了分析检测,并对样品中氢同位素组成特征及成因进行了探讨.
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