超临界水中碳酸钠团簇成核与生长分子动力学模拟

引用本文: 张金利, 何正华, 韩优, 李韡, 武江洁星, 甘中学, 谷俊杰. 超临界水中碳酸钠团簇成核与生长分子动力学模拟[J]. 物理化学学报, 2012, 28(07): 1691-1700. doi: 10.3866/PKU.WHXB201205032 shu

Citation: ZHANG Jin-Li, HE Zheng-Hua, HAN You, LI Wei, WU Jiang-Jie-Xing, GAN Zhong-Xue, GU Jun-Jie. Nucleation and Growth of Na₂CO₃ Clusters in Supercritical Water Using Molecular Dynamics Simulation[J]. Acta Physico-Chimica Sinica, 2012, 28(07): 1691-1700. doi: 10.3866/PKU.WHXB201205032 shu

超临界水中碳酸钠团簇成核与生长分子动力学模拟

基金项目:
国家高技术研究发展计划项目(863) (2011AA05A201) (863) (2011AA05A201)

国家自然科学基金(21106094, 20836005) (21106094, 20836005)

国家重点基础研究发展规划项目(973) (2010CB736202)资助 (973) (2010CB736202)

摘要:

应用分子动力学方法研究了碳酸钠颗粒在超临界水中的成核与生长过程. 计算了温度为700-1100 K、压力在23-30 MPa下碳酸钠的团聚过程, 计算时间为1 ns. 对体系结合能与径向分布函数的分析表明, 碳酸钠成核过程主要受静电作用的影响. 在超临界态下, 水分子与Na⁺和CO₃^2- 之间的静电作用降低, Na⁺与CO₃^2- 能够很容易碰撞形成Na₂CO₃小团簇. 在Na₂CO₃整个成核过程中, 单个离子的碰撞在前50 ps 内完成, 同时离子碰撞速率达到10³⁰ cm^-3·s^-1. 另外, 在成核阶段温度的影响比压力更加明显, 温度越高, 离子碰撞速率越快, 形成的初始团簇越多. 而压力对Na₂CO₃团簇的进一步生长影响较大.

关键词:

English

Nucleation and Growth of Na₂CO₃ Clusters in Supercritical Water Using Molecular Dynamics Simulation

1.
1. School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, P. R. China;
2. Tianjin Key Laboratory of Membrane Science and Desalination Technology, Tianjin University, Tianjin 300072, P. R. China;
3. State Key Laboratory of Coal-Based Low Carbon Energy, ENN Group, Langfang 065001, Hebei Province, P. R. China
Received Date: 28 March 2012
Available Online: 07 June 2012
Fund Project:
国家高技术研究发展计划项目(863) (2011AA05A201)

国家自然科学基金(21106094, 20836005)

国家重点基础研究发展规划项目(973) (2010CB736202)资助

Abstract:

The nucleation and growth of Na₂CO₃ particles in supercritical water were investigated using molecular dynamics simulation. The clustering process of Na₂CO₃ was studied for 1 ns at a series of state points, across temperature and pressure ranges of 700 to 1100 K and 23 to 30 MPa, respectively. The binding energy and radial distribution function analysis showed that the electrostatic interaction was the main factor affecting the whole Na₂CO₃ nucleation process. Under supercritical conditions, the electrostatic interaction of water molecules with Na⁺ and CO₃^2- ions rapidly decreased, allowing Na⁺ and CO₃^2- ions to readily collide with each other to form small Na₂CO₃ clusters. During the initial Na₂CO₃ nucleation process, all the single-ion collisions were complete within 50 ps and the ionic collision rates appeared to be of the order of 1030 cm^-3·s^-1. Furthermore, the effect of temperature was found to be more important than that of the pressure at the nucleation stage and a higher temperature led to an enhanced collision rate and the formation of more initial Na₂CO₃ particles. The further growth of the Na₂CO₃ particles was more dependent on the pressure.

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

超临界水中碳酸钠团簇成核与生长分子动力学模拟

English

Nucleation and Growth of Na₂CO₃ Clusters in Supercritical Water Using Molecular Dynamics Simulation

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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

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