化工学报 ›› 2022, Vol. 73 ›› Issue (7): 3174-3181.DOI: 10.11949/0438-1157.20220097
赵继昊1(),唐伟强1,徐小飞1(),赵双良1,2,贺炅皓3
收稿日期:
2022-01-18
修回日期:
2022-04-12
出版日期:
2022-07-05
发布日期:
2022-08-01
通讯作者:
徐小飞
作者简介:
赵继昊(1996—),男,硕士研究生,基金资助:
Jihao ZHAO1(),Weiqiang TANG1,Xiaofei XU1(),Shuangliang ZHAO1,2,Jionghao HE3
Received:
2022-01-18
Revised:
2022-04-12
Online:
2022-07-05
Published:
2022-08-01
Contact:
Xiaofei XU
摘要:
由高分子、填料、键合剂及各种功能助剂组成的高分子复合材料广泛应用于轮胎、含能材料、医疗、环保、建筑、交通等行业。键合剂在填料表面的吸附特性对高分子复合材料的性能有重要影响。分别以未改性的高氯酸铵、炭黑和二氧化硅填料为对象,利用第一性原理计算评估了五种键合剂分子,即三乙醇胺(TEA)、三氟化硼三乙醇胺络合物(T313)、N,N'-二邻甲苯胍(DOTG)、N,N'-二苯基硫脲(DPTU)和二苯胍(DPG),在填料表面的吸附能。计算结果表明,随着填料基底层数的增加,吸附能逐渐增加,最后趋于一个稳定值。其中TEA和T313键合剂在高氯酸铵表面的吸附能为-0.84~-1.37 eV;DOTG、DPTU和DPG在炭黑表面的吸附能为-1.01~-1.29 eV;在二氧化硅表面的吸附能为-0.87~-0.94 eV;在接枝羟基的二氧化硅上的吸附能为-1.16~-1.36 eV。依次考察了单层炭黑点缺陷(单空位缺陷、双空位缺陷、Stone-Wales缺陷)和二氧化硅表面接枝羟基对吸附能的影响,发现单空位和双空位缺陷对吸附能影响不大,而Stone-Wales缺陷和二氧化硅接枝羟基显著增加吸附能。
中图分类号:
赵继昊, 唐伟强, 徐小飞, 赵双良, 贺炅皓. 高分子复合材料中键合剂在不同纳米填料表面的吸附能计算[J]. 化工学报, 2022, 73(7): 3174-3181.
Jihao ZHAO, Weiqiang TANG, Xiaofei XU, Shuangliang ZHAO, Jionghao HE. Adsorption energy of bonding agent on nano-filler in polymer composites[J]. CIESC Journal, 2022, 73(7): 3174-3181.
图2 五种键合剂分子的分子结构与静电势分布: (a) TEA; (b) T313; (c) DPG; (d) DPTU; (e) DOTG(1 cal=4.184 J)
Fig.2 Molecular structure and electrostatic potential distribution of five bond agents: (a) TEA; (b) T313; (c) DPG; (d) DPTU; (e) DOTG
图7 炭黑表面缺陷模型: (a) 单空位缺陷;(b) 双空位缺陷;(c) Stone-Wales缺陷
Fig.7 Carbon black surface defect model: (a) single vacancy defect; (b) divacancy defect; (c) Stone-Wales defect
缺陷类型 | 吸附能/eV | ||
---|---|---|---|
DPG | DPTU | DOTG | |
无缺陷 | -0.99 | -1.12 | -1.28 |
单空位 | -0.99 | -1.12 | -1.27 |
双空位 | -0.97 | -1.09 | -1.26 |
Stone-Wales | -1.01 | -1.14 | -1.30 |
表1 有机分子与不同缺陷类型炭黑的吸附能
Table 1 Adsorption energy of organic molecules with different defect types of carbon black
缺陷类型 | 吸附能/eV | ||
---|---|---|---|
DPG | DPTU | DOTG | |
无缺陷 | -0.99 | -1.12 | -1.28 |
单空位 | -0.99 | -1.12 | -1.27 |
双空位 | -0.97 | -1.09 | -1.26 |
Stone-Wales | -1.01 | -1.14 | -1.30 |
图8 DPTU在不同缺陷类型炭黑上的吸附: (a)无缺陷;(b)单空位缺陷;(c)双空位缺陷;(d)Stone-Wales缺陷
Fig.8 Adsorption of DPTU on carbon black with different defect types: (a) normal;(b) single vacancy defect;(c) divacancy defect;(d) Stone-Wales defect
基底类型 | 吸附能/eV | ||
---|---|---|---|
DPG | DPTU | DOTG | |
双层炭黑 | -1.01 | -1.14 | -1.29 |
双层SiO2 | -0.87 | -0.89 | -0.94 |
双层SiO2@OH | -1.16 | -1.20 | -1.35 |
表2 有机分子与不同基底的吸附能
Table 2 Adsorption energy of organic molecules with different substrates
基底类型 | 吸附能/eV | ||
---|---|---|---|
DPG | DPTU | DOTG | |
双层炭黑 | -1.01 | -1.14 | -1.29 |
双层SiO2 | -0.87 | -0.89 | -0.94 |
双层SiO2@OH | -1.16 | -1.20 | -1.35 |
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