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用于模拟地质层中有机物氧化降解的反应力场。

Reactive force fields for modeling oxidative degradation of organic matter in geological formations.

作者信息

Hur Jaewoong, Abousleiman Younane N, Hull Katherine L, Abdolhosseini Qomi Mohammad Javad

机构信息

Department of Civil and Environmental Engineering, Henry Samueli School of Engineering, University of California E4130 Engineering Gateway Irvine CA 92697-2175 USA

Integrated PoroMechanics Institute, School of Geosciences, The University of Oklahoma Norman Oklahoma 73019 USA.

出版信息

RSC Adv. 2021 Sep 1;11(47):29298-29307. doi: 10.1039/d1ra04397h.

Abstract

In an attempt to better explore organic matter reaction and properties, at depth, to oxidative fluid additives, we have developed a new ReaxFF potential to model and describe the oxidative decompositions of aliphatic and aromatic hydrocarbons in the presence of the oxychlorine ClO oxidizers. By carefully adjusting the new H/C/O/Cl parameters, we show that the potential energies in both training and validation sets correlate well with calculated density functional theory (DFT) energies. Our parametrization yields a reliable empirical reactive force field with an RMS error of ∼1.57 eV, corresponding to a 1.70% average error. At this accuracy level, the reactive force field provides a reliable atomic-level picture of thermodynamically favorable reaction pathways governing oxidative degradation of H/C/O/Cl compounds. We demonstrate this capability by studying the structural degradation of small aromatic and aliphatic hydrocarbons in the presence of oxychlorine oxidizers in aqueous environments. We envision that such reactive force fields will be critical in understanding the oxidation processes of organic matter in geological reservoirs and the design of the next generation of reactive fluids for enhanced shale gas recovery and improved carbon dioxide adsorption and sequestration.

摘要

为了更深入地探究有机物质与氧化流体添加剂的反应及性质,我们开发了一种新的ReaxFF势,用于模拟和描述在氯氧化物ClO氧化剂存在下脂肪族和芳香族烃的氧化分解。通过仔细调整新的H/C/O/Cl参数,我们表明训练集和验证集中的势能与计算得到的密度泛函理论(DFT)能量具有良好的相关性。我们的参数化产生了一个可靠的经验反应力场,均方根误差约为1.57 eV,对应平均误差为1.70%。在这个精度水平下,反应力场提供了关于控制H/C/O/Cl化合物氧化降解的热力学有利反应途径的可靠原子级图景。我们通过研究在水环境中氯氧化物氧化剂存在下小芳香族和脂肪族烃的结构降解来证明这种能力。我们设想,这种反应力场对于理解地质储层中有机物质的氧化过程以及设计用于提高页岩气采收率和改善二氧化碳吸附与封存的下一代反应流体至关重要。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/fc44/9040638/7e5988cc5e2f/d1ra04397h-f1.jpg

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