磷酸酯类单体与氧化锆间化学反应模型的建立及作用机制

doi:10.7518/hxkq.2017.02.007

华西口腔医学杂志 ›› 2017, Vol. 35 ›› Issue (2): 145-149.doi: 10.7518/hxkq.2017.02.007

磷酸酯类单体与氧化锆间化学反应模型的建立及作用机制

卢枳岑^1,²(), 谢海峰^1,², 章非敏^1,², 张怀勤^1,², 陈晨^2,³()

1.南京医科大学口腔医院修复科
2.南京医科大学口腔疾病研究江苏省重点实验室
3.南京医科大学口腔医院牙体牙髓科,南京 210029

收稿日期:2016-07-16 修回日期:2016-10-08 出版日期:2017-04-01 发布日期:2017-04-01
作者简介:
卢枳岑,硕士,E-mail：fjlzc92@163.com
基金资助:
国家自然科学基金（81400539）;江苏高校优势学科建设工程资助项目（2014-37）;江苏省自然科学基金（BK20150998,BK20140913）;江苏省高校自然科学基金（15KJB320003）

Establishment and mechanisms of chemical interaction between phosphate monomer and zirconia model

Zhicen Lu^1,²(), Haifeng Xie^1,², Feimin Zhang^1,², Huaiqin Zhang^1,², Chen Chen^2,³()

1. Dept. of Prosthetics, Affiliated Hospital of Stomatology, Nanjing Medical University, Nanjing 210029, China
2. Jiangsu Key Laboratory of Oral Diseases, Nanjing Medical University, Nanjing 210029, China
3. Dept. of Conservative Dentistry and Endodontics, Affiliated Hospital of Stomatology, Nanjing Medical University, Nanjing 210029, China

Received:2016-07-16 Revised:2016-10-08 Online:2017-04-01 Published:2017-04-01
Supported by:
The National Natural Science Foundation of China (81400539);Priority Academic Program Development of Jiangsu Higher Education Institutions (2014-37);Natural Science Foundation of Jiangsu Province (BK20150998, BK20140913);Natural Science Foundation for Jiangsu Higher Education Institutions (15KJB320003)

摘要/Abstract

摘要：

目的对磷酸酯单体10-甲基丙烯酰氧癸二氢磷酸酯（MDP）提高四方相氧化锆与树脂间化学粘接的作用机制进行解释。方法分别构建MDP、四方相氧化锆陶瓷晶体以及两者反应的数字模型,采用热力学方法对MDP分子与四方相氧化锆晶体簇相互作用的吉布斯自由能和平衡常数进行计算。结果MDP与四方相氧化锆晶体簇可能发生单配位形式和双配位形式的结合,其吉布斯自由能分别为-147.761和-158.073 kJ·mol^-1,说明MDP能够与四方相氧化锆晶体发生化学结合,平衡常数较高（4.95×10²⁷）的双配位结合形式较平衡常数较低（7.72×10²⁵）的单配位结合形式更为稳定。结论 MDP能够通过与四方相氧化锆陶瓷以双配位形式发生化学结合来提高其与树脂的粘接强度。

关键词: 量子化学, 反应机制, 氧化锆, 粘接, 磷酸酯单体, 底涂剂

Abstract:

Objective To analyze chemical mechanism of bonding improvement of zirconia via 10-methacryloyloxydecyl dihydrogen phosphate (MDP) conditioning. Methods Various models were created for tetragonal zirconia crystals, molecular MDP, and MDP complex, and tetragonal zirconia crystal. Thermodynamic methods were used to analyze configuration between MDP and tetragonal zirconia crystal through calculation of their Gibbs free energy values and equilibrium constants. Results Two potential configurations (double- and single-coordinate) may occur between MDP and ZrO₂crystal clusters. Thermodynamic calculations showed that -147.761 and -158.073 kJ·mol^-1 Gibbs free energy were required to form single- and double-coordinate configurations; their negative signs indicate that reactions for both configurations can occur. Equilibrium constant for single-coordinate configuration was 7.72×10²⁵, which was less than that of double-coordinate configuration (4.95×10²⁷), suggesting that the latter was more stable. Conclusion MDP can spontaneously establish a double-coordinate configuration with zirconia.

Key words: quantum chemistry, reaction mechanism, zirconia, bonding, phosphate monomer, primer

中图分类号:

R783.1

卢枳岑, 谢海峰, 章非敏, 张怀勤, 陈晨. 磷酸酯类单体与氧化锆间化学反应模型的建立及作用机制[J]. 华西口腔医学杂志, 2017, 35(2): 145-149.

Zhicen Lu, Haifeng Xie, Feimin Zhang, Huaiqin Zhang, Chen Chen. Establishment and mechanisms of chemical interaction between phosphate monomer and zirconia model[J]. West China Journal of Stomatology, 2017, 35(2): 145-149.

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参考文献 11

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项目	R-OP(OH)₂	H₂O	R-OPO₂^2-	H₃O⁺
ν	-1	-2	1	2
ε₀+H_corr/Ha	-643.8	-76.0	-642.9	-76.4
S_electron/[Cal·(Mol-K)^-1]	0	0	0	0
S_rot/[Cal·(Mol-K)^-1]	36.4	10.3	36.3	9.7
S_vib/[Cal·(Mol-K)^-1]	92.9	0.0	86.3	1.2
S_tot/[Cal·(Mol-K)^-1]	129.3	10.3	122.6	10.9
G_final/Ha	-643.9	-76.0	-643.0	-76.4
ΔG1/(kJ·mol^-1)	308.137
K	/

项目	R-OPO₂^2-	Zr₄O₈	R-OPO₂-Zr₄O₈^2-
ν	-1	-1	1
ε₀+H_corr/Ha	-642.6	-788.8	-1 431.6
S_electron/[Cal·(Mol-K)^-1]	0	0	0
S_rot/[Cal·(Mol-K)^-1]	36.3	30.7	40.6
S_vib/[Cal·(Mol-K)^-1]	91.9	40.3	139.4
S_tot/[Cal·(Mol-K)^-1]	128.2	71.0	180.0
G_final/Ha	-642.6	-788.9	-1 431.7
ΔG2(kJ·mol^-1)	-466.210
K	4.95×10²⁷

项目	R-OPO₂^2-	Zr₄O₈	R-OPO₂-Zr₄O₈^2-
ν	-1	-1	1
ε₀+H_corr/Ha	-642.6	-788.8	-1 431.6
S_electron/[Cal·(Mol-K)^-1]	0	0	0
S_rot/[Cal·(Mol-K)^-1]	36.3	30.7	40.6
S_vib/[Cal·(Mol-K)^-1]	91.9	40.3	139.6
S_tot/[Cal·(Mol-K)^-1]	128.2	71.0	180.2
G_final	-642.6	-788.9	-1 431.7
ΔG3(kJ·mol^-1)	-455.897
K	7.72×10²⁵

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磷酸酯类单体与氧化锆间化学反应模型的建立及作用机制

Establishment and mechanisms of chemical interaction between phosphate monomer and zirconia model

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