地球内部熔/流体的分子模拟:进展与展望

Molecular Simulation of Melts and Fluids in the Earth's Interior:An Overview and Outlook

目前对超临界地质流体的形成条件、成分、结构和物理化学性质的认识还不是特别清晰,分子模拟作为一种方兴未艾的理论研究手段,正在被广泛应用于地球科学领域。本文简述了目前采用分子模拟研究硅酸盐熔体、含水硅酸盐熔体、富水流体以及超临界地质流体所取得的主要成果,侧重讨论分子模拟方法在其中的应用,为超临界地质流体的计算模拟研究提供帮助,并展望了超临界地质流体分子模拟可能遇到的挑战和发展趋势。已有研究结果表明,不同分子模拟方法各有优缺点,相对于精度较低的经典分子动力学方法而言,采用一般泛函的第一性原理方法加上色散校正之后,可以满足目前对超临界地质流体研究的精度需要。另外,机器学习和第一性原理方法结合,以及建立相关热力学模型将是推进与超临界地质流体相关研究的有效途径。

The understanding of the formation conditions,compositions,structures,and physicochemical properties of supercritical geofluids is not very clear yet at present.As a growing theoretical method,the molecular simulation has been widely used in the field of geosciences.In this paper,we have briefly summarized main achievements of researches on the silicate melts,hydrous silicate melts,aqueous fluids,and supercritical geofluids obatined by using the molecular simulation method,particularly discussed the application of molecular simulation method to those researches,provided assistance for the computational simulation study of supercritical geofluids,and then proposed an outlook on possible challenges and development trends of the molecular simulation of supercritical geofluids.Previous researches show that different molecular simulation methods have their own advantages and disadvantages.Compared to the classical molecular dynamics methods with relatively low accuracy,the first-principles method using general functionals can meet the need of calculation accuracy for studying supercritical geofluids after adding dispersion correction.In addition,the combination of the machine learning and first-principles method,and the establishment of related thermodynamic models,will be an effective way to promote researches on topics associated with the supercritical geofluids.