Modeling Nitric Oxide and its dimer: force field development and thermodynamics of dimerization

IF 2.9 3区化学 Q3 CHEMISTRY, PHYSICAL

Physical Chemistry Chemical Physics Pub Date : 2025-06-10 DOI:10.1039/d5cp00784d

Tijin Saji, Thijs JH Vlugt, Sofia Calero, Behnaz Bagheri

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Abstract

Nitric Oxide, NO, is a free radical that forms dimers, (NO)₂, at its vapor-liquid coexisting temperatures. In this work, we developed an all-atom force field for NO and (NO)₂. To assess the performance of this force field, we computed the vapor-liquid equilibrium (VLE) properties of the reactive NO-(NO)₂ system, as well as those of pure NO and pure (NO)₂, using Continuous Fractional Component Monte Carlo (CFCMC) simulations. We then compared the results with the available experimental data and predictions from two previously developed force fields. For the reactive NO-(NO)₂ system, we performed CFCMC simulations in the reactive Gibbs ensemble in which the formation of NO dimers, 2NO↔(NO)₂, is considered. The predicted coexistence vapor-liquid densities, dimer mole fractions in the liquid phase, saturated vapor pressures, and heats of vaporization using our force field in the temperature range 120 K to 170 K are in excellent agreement with experimental values. In addition, we conducted a systematic parameter study to analyze the sensitivity of the new force field parameters and the isolated molecule partition functions of (NO)₂ on the VLE properties of the reactive NO-(NO)₂ system. The results indicate that the VLE properties of the reactive NO-(NO)₂ system are affected by both the force field parameters of the involved species as well as the isolated molecule partition functions of (NO)₂.

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一氧化氮及其二聚体的建模：力场发展和二聚热力学

一氧化氮（NO）是一种自由基，在其汽液共存温度下形成二聚体（NO）2。在这项工作中，我们建立了NO和（NO）2的全原子力场。为了评估该力场的性能，我们使用连续分数分量蒙特卡罗（CFCMC）模拟计算了反应性NO-(NO)2体系以及纯NO和纯（NO）2体系的气液平衡（VLE）特性。然后，我们将结果与现有的实验数据和先前开发的两个力场的预测进行了比较。对于反应性NO-(NO)2系统，我们在考虑NO二聚体2NO↔（NO）2的反应性Gibbs综中进行了CFCMC模拟。在120 ~ 170 K的温度范围内，利用我们的力场预测的汽液共存密度、液相二聚体摩尔分数、饱和蒸汽压和汽化热与实验值非常吻合。此外，我们还进行了系统的参数研究，分析了新的力场参数和（NO）2的分离分子配分函数对反应性NO-(NO)2体系VLE特性的敏感性。结果表明，反应性NO-(NO)2体系的VLE特性受参与物质的力场参数和（NO）2的分离分子配分函数的影响。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Physical Chemistry Chemical Physics 化学-物理：原子、分子和化学物理

CiteScore

5.50

自引率

9.10%

发文量

2675

审稿时长

2.0 months

期刊介绍： Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.