基于ReaxFF力场的对硝基苯酚臭氧氧化分子动力学模拟

引用本文: 王子民, 郑默, 谢勇冰, 李晓霞, 曾鸣, 曹宏斌, 郭力. 基于ReaxFF力场的对硝基苯酚臭氧氧化分子动力学模拟[J]. 物理化学学报, 2017, 33(7): 1399-1410. doi: 10.3866/PKU.WHXB201704132 shu

Citation: WANG Zi-Min, ZHENG Mo, XIE Yong-Bing, LI Xiao-Xia, ZENG Ming, CAO Hong-Bin, GUO Li. Molecular Dynamics Simulation of Ozonation of p-Nitrophenol at Room Temperature with ReaxFF Force Field[J]. Acta Physico-Chimica Sinica, 2017, 33(7): 1399-1410. doi: 10.3866/PKU.WHXB201704132 shu

基于ReaxFF力场的对硝基苯酚臭氧氧化分子动力学模拟

王子民 ^1,2, ,
郑默 ^2, ,
谢勇冰 ^3, ,
李晓霞 ^2,4, ,
曾鸣 ^1, ,
曹宏斌 ^3, ,
郭力 ^2,4,

1.
中国矿业大学(北京)化学与环境工程学院, 北京 100083;
2.
中国科学院过程工程研究所复杂系统国家重点实验室, 北京 100190;
3.
中国科学院过程工程研究所环境技术与工程研究部, 北京 100190;
4.
中国科学院大学化学与化工学院, 北京 100049
基金项目:
国家自然科学基金（21373227），国家杰出青年科学基金（51425405）和多相复杂系统国家重点实验室基金（COM2015A004）资助项目

摘要: 本文采用基于ReaxFF反应力场的分子动力学方法（ReaxFF MD），利用自主研发的国际首个基于GPU加速的ReaxFF MD程序系统GMD-Reax和独特的化学反应分析工具VARxMD，探索臭氧氧化对硝基苯酚的反应机理。通过模拟考察了300 K恒温条件下臭氧氧化水中对硝基苯酚的行为，获得了酚结构开环、CO₂生成、主要自由基（·OH、·O₂、·O）及团簇型自由基的数量演变趋势，并可定性描述六元环开环和CO₂生成均遵循伪一级反应动力学规律。反应机理分析表明酚类分子在水溶液中被臭氧氧化的路径主要经过攫氢、六元环开环、碳链的氧化分解三个阶段，也揭示了自由基和团簇型自由基在臭氧降解对硝基苯酚时所发挥的重要作用。本工作是应用ReaxFF MD分子模拟方法对常温水环境下臭氧降解酚类污染物反应机理研究的一个尝试，可为深入认识该机理及相关的实验、理论研究提供一定的参考。

关键词:

English

Molecular Dynamics Simulation of Ozonation of p-Nitrophenol at Room Temperature with ReaxFF Force Field

1.
School of Chemical and Environmental Engineering, China University of Mining and Technology, Beijing, Beijing 100083, P. R. China;
2.
State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Science, Beijing 100190, P. R. China;
3.
Research Center for Process Pollution Control, National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Institute of Process Engineering, Chinese Academy of Science, Beijing 100190, P. R. China;
4.
School of Chemistry and Chemical Engineering, University of Chinese Academy of Science, Beijing 100049, P. R. China
Received Date: 26 January 2017
Revised Date: 06 April 2017
Available Online: 11 April 2017
Fund Project:
The project was supported by the National Natural Science Foundation of China (21373227), the National Science Fund for Distinguished Young Scholars, China (51425405), and China's State Key Laboratory of Multiphase Complex Systems, China (COM2015A004).

Abstract: Understanding the reaction mechanism of phenol ozonation in coking wastewater is very important for industrial applications of the ozonation process. Ozonation of p-nitrophenol in water at 300 K was simulated by ReaxFF force field molecular dynamics (ReaxFF MD) employing the GPU-enabled high-performance code of GMD-Reax and a unique code of VARxMD developed in authors' group. Evolution trends of aromatic ring opening, CO₂ generation, dominant radicals (·OH, ·O₂, ·O), and H₂O clusters were obtained. The simulated CO₂ generation and reduction of aromatic ring could be described with pseudo-first-order kinetics. Moreover, the reaction pathways for the ozonation of p-nitrophenol can be divided into three stages:hydrogen abstraction, opening of the six-membered-ring structure, and the breaking of C-C bonds. The simulations revealed the important role of radicals and water clusters in the ozonation of p-nitrophenol. This work is an attempt to investigate the ozonation mechanism of phenols in aqueous solutions at room temperature using ReaxFF MD, which should be helpful for further experimental or theoretical investigation of the mechanism.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

基于ReaxFF力场的对硝基苯酚臭氧氧化分子动力学模拟

English

Molecular Dynamics Simulation of Ozonation of p-Nitrophenol at Room Temperature with ReaxFF Force Field

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

基于ReaxFF力场的对硝基苯酚臭氧氧化分子动力学模拟

English

Molecular Dynamics Simulation of Ozonation of p-Nitrophenol at Room Temperature with ReaxFF Force Field

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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