高压下多组分体系的演化：VI。氢-碳体系的热力学稳定性：烃类的成因和石油的成因
The Evolution of Multicomponent Systems at High Pressures: VI. The Thermodynamic Stability of the Hydrogen-Carbon System: The Genesis of Hydrocarbons and the Origin of Petroleum
摘要：
用化学热力学稳定性理论分析了天然石油中烃类的自发成因。简要回顾了热力学第二定律对化学演化的限制;确认了在地球近地表地壳的温度和压力特征范围内，生物分子转化为比甲烷重的碳氢化合物分子的有效禁止。通过扩展标度粒子理论（SPT）和利用简化扰动硬链理论（SPHCT）的因子化配分函数技术，建立了一个通用的第一性原理状态方程。化学势，和相应的热力学亲和力，已计算的氢-碳（H-C）系统的典型组件在1-100 kbar之间的压力范围内，并在与地球的深度在这样的压力下的温度一致。理论分析表明，正构烷烃是化学势最低的同系碳氢化合物，只有在压力大于30千巴时才会形成，只有最轻的甲烷除外。30千巴的压力相当于大约100公里的深度。特殊的高压装置已被设计，它允许在50千巴的压力和2000 K的温度下进行研究，并且还允许在保持高压的同时快速冷却。石油碳氢化合物的高压成因已被证明只使用固体试剂氧化铁，FeO，和大理石，碳酸钙，99.9%的纯度和湿与三蒸馏水。
英文摘要：
The spontaneous genesis of hydrocarbons which comprise natural petroleum have been analyzed by chemical thermodynamic stability theory. The constraints imposed upon chemical evolution by the second law of thermodynamics are briefly reviewed; and the effective prohibition of transformation, in the regime of temperatures and pressures characteristic of the near-surface crust of the Earth, of biological molecules into hydrocarbon molecules heavier than methane is recognized. A general, first-principles equation of state has been developed by extending scaled particle theory (SPT) and by using the technique of the factored partition function of the Simplified Perturbed Hard Chain Theory (SPHCT). The chemical potentials, and the respective thermodynamic Affinity, have been calculated for typical components of the hydrogen-carbon (H-C) system over a range pressures between 1-100 kbar, and at temperatures consistent with those of the depths of the Earth at such pressures. The theoretical analyses establish that the normal alkanes, the homologous hydrocarbon group of lowest chemical potential, evolve only at pressures greater than approximately thirty kbar, excepting only the lightest, methane. The pressure of thirty kbar corresponds to depths of approximately 100 km. Special high-pressure apparatus has been designed which permits investigations at pressures to 50 kbar and temperatures to 2000 K, and which also allows rapid cooling while maintaining high pressures. The high-pressure genesis of petroleum hydrocarbons has been demonstrated using only the solid reagents iron oxide, FeO, and marble, CaCO3, 99.9% pure and wet with triple-distilled water.
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