三<strong>(</strong>氯异丙基<strong>)</strong>磷酸酯在蒙脱石表面吸附机理的模拟计算

doi:10.11901/1005.3093.2020.075

材料研究学报

2020, Vol. 34

Issue (11): 853-860 DOI: 10.11901/1005.3093.2020.075

研究论文

本期目录 | 过刊浏览

三(氯异丙基)磷酸酯在蒙脱石表面吸附机理的模拟计算

刘珊珊¹, 兰艳花³, 杨荣杰²(

), 周智明¹

^1.北京理工大学化学与化工学院北京 100081
^2.北京理工大学材料学院北京 100081
^3.中北大学环境与安全工程学院太原 030051

Simulation Calculation for Adsorption Mechanism of Tris (chloroisopropyl) Phosphate on Surface of Montmorillonite

LIU Shanshan¹, LAN Yanhua³, YANG Rongjie²(

), ZHOU Zhiming¹

^1.School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China
^2.School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
^3.School of Environmental and Safety Engineering, North University of China, Taiyuan 030051, China

引用本文:

刘珊珊, 兰艳花, 杨荣杰, 周智明. 三(氯异丙基)磷酸酯在蒙脱石表面吸附机理的模拟计算[J]. 材料研究学报, 2020, 34(11): 853-860.
Shanshan LIU, Yanhua LAN, Rongjie YANG, Zhiming ZHOU. Simulation Calculation for Adsorption Mechanism of Tris (chloroisopropyl) Phosphate on Surface of Montmorillonite[J]. Chinese Journal of Materials Research, 2020, 34(11): 853-860.

全文: PDF(6490 KB) HTML

摘要:

基于密度泛函理论研究了三(氯异丙基)磷酸酯(TCPP)与钠基蒙脱石(NaMMT)凝胶化的机理，在微观水平上建立TCPP和NaMMT的分子模型并计算了在无水和有水状态下TCPP在NaMMT的001表面以及晶层间的吸附参数。结果表明，TCPP在NaMMT的001表面和晶层间均能通过物理作用稳定吸附，钠离子有利于TCPP在NaMMT表面的吸附。在有水分子状态下TCPP与水分子在NaMMT表面协同吸附，水分子作为“桥梁”将TCPP与NaMMT表面连接起来，增强了它们之间的相互作用。实验结果亦表明，水分能明显提高TCPP与NaMMT的凝胶化速度。NaMMT与TCPP通过强相互作用自发溶胀形成物理交联结构，吸收大量的TCPP液体。水分增强了体系的相互作用，使交联网络更容易形成，从而加速凝胶化过程。

关键词 ：无机非金属材料, 三（氯异丙基）磷酸酯, 蒙脱石, 吸附, 模拟

Abstract：

To explore the gelation mechanism of tris (chloroisopropyl) phosphate (TCPP) and sodium montmorillonite (NaMMT), the molecular models of TCPP and NaMMT at the micro level were established based on the density functional theory method, The adsorption parameters of TCPP on 001 lattice plane and interplanar of NaMMT in anhydrous and hydrous conditions were calculated. The results show that TCPP can stably adsorb on the 001 lattice plane and interplanar of NaMMT through physical force. And sodium ions are beneficial to the adsorption of TCPP on NaMMT surface. In the presence of water molecules TCPP and water molecule on the surface of NaMMT exhibit synergistic adsorption, and water molecules serve as "bridges" to connect TCPP and NaMMT surfaces, enhancing interaction between them. Experimental research also shows that water can significantly accelerate the gelation rate of TCPP and NaMMT. NaMMT and TCPP swell spontaneously through strong interaction to form a physical cross-linked structure, and then the network can absorb a large amount of TCPP liquid, and water molecules enhance the interaction of the system, making the cross-linked network easier to form, which accelerate the gelation process.

Key words： inorganic non-metallic materials tris (chloroisopropyl) phosphate montmorillonite adsorption simulation

收稿日期: 2020-03-11

ZTFLH:

O641

基金资助:国家国际科技合作专项(2014DFA52900)

作者简介: 刘珊珊，女，1994年生，硕士生

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https://www.cjmr.org/CN/10.11901/1005.3093.2020.075 或 https://www.cjmr.org/CN/Y2020/V34/I11/853

图1 NaMMT晶体的球棍模型

图2 TCPP的分子结构和模拟结构

图3 NaMMT的Na-001表面和None-001表面

图4 TCPP在Na-001、None-001表面和晶层间吸附的最优吸附构型

表1 吸附质在Na-001和None-001表面和晶层间的吸附能

表2 不同系统中的成键情况和键长

图5 Na、Cl原子的态密度

图6 Cl、O原子的态密度

图7 H、O原子的态密度

图8 水分对TCPP与NaMMT凝胶化的影响

图9 一个H2O分子在Na-001、None-001和晶层间吸附的最优构型

图10 H2O/TCPP在三个不同表面吸附的最优构型

表3 NaMMT-TCPP-H2O系统中的键长

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