Development of a ReaxFF Force Field for Aqueous Phosphoenolpyruvate as a Novel Biomimetic Carbon Capture Absorbent
Development of a ReaxFF Force Field for Aqueous Phosphoenolpyruvate as a Novel Biomimetic Carbon Capture Absorbent
复制标题
水性磷酸烯醇丙酮酸盐 ReaxFF 力场的开发作为新型仿生碳捕获吸收剂
DOI：
10.1021/acs.jpcc.2c01841
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Faller, Roland
中科院分区：
文献类型：
--
作者：
Huang, Yihan;Wexler, Anthony S.;Bein, Keith J.;Faller, Roland
C4植物中的磷酸烯醇式丙酮酸（PEP）通过其景天酸代谢（CAM）机制，有望成为一种新型的绿色仿生碳捕集吸收剂，并有望取代目前最常用的一乙醇胺吸收剂应用于未来的后燃烧碳捕集系统。在这项研究中，一个新的ReaxFF模型已被开发来描述CAM反应涉及PEP和原子之间的相互作用在P/C/O/H系统。ReaxFF力场参数与部分电荷、分子结构、键离解能、反应能和活化能的量子力学（QM）训练数据拟合。第二代水参数与P/C参数相结合，以更准确地描述水，P的静电参数进行了特别处理，以纠正P/O相互作用。所开发的P/C/O/H ReaxFF模型能够再现CAM过程中涉及的分子和反应的结构和能量学的训练集，并准确地描述碳酸氢盐水溶液和PEP系统。使用该ReaxFF模型的分子动力学模拟描绘了碳酸氢盐如何与PEP和在溶液中反应，并确定了局部结构对通过使用PEP进行碳捕获所需的反应的影响，这使得PEP变体的潜在设计成为最佳的碳捕获吸收剂。
Phosphoenolpyruvate (PEP) found in C4plants could be a novel green absorbent in biomimetic carbon capture through its crassulacean acid metabolism (CAM) mechanism and could potentially substitute the most commonly used absorbent monoethanolamine in future postcombustion capture systems. In this study, a new ReaxFF model has been developed to describe the CAM reactions involving PEP and the atomic interactions in the P/C/O/H system. The ReaxFF force field parameters were fitted against quantum mechanical (QM) training data for partial charges, molecular structures, bond dissociation energies, reaction energies, and activation energies. Second-generation water parameters were combined with P/C parameters for more accurate water description, and P’s electrostatic parameters were specially treated to correct P/O interactions. The developed P/C/O/H ReaxFF model was able to reproduce the training set for structures and energetics of the molecules and reactions involved in the CAM process and accurately describe the aqueous bicarbonate and PEP systems. Molecular dynamics simulations using this ReaxFF model depict how bicarbonate reacts with PEP and in solution and determine the impact of local structure on reactions necessary to perform carbon capture by using PEP, which enables the potential design of PEP variant as the optimal carbon capture absorbent.
影响因子：
4.4
作者：
NOSE, S
通讯作者：
NOSE, S