含酰胺和尿嘧啶的氢键复合物的三体效应

doi:10.7503/cjcu20140477

摘要/Abstract

摘要：

采用包含BSSE校正的MP2/aug-cc-pVTZ方法对酰胺、二肽、尿嘧啶和水分子形成的氢键复合物的三体效应进行了研究, 分析了三体作用能对体系总作用能的贡献. 结果表明, 在这些氢键复合物中, 三体作用能占体系总作用能的10%~20%, 三体作用属于近程作用, 因此在分子模拟中至少应考虑近处的三体效应.

关键词: 三体效应, 氢键复合物, 作用能, 酰胺, 尿嘧啶, 团簇体系, 凝聚相体系

Abstract:

Many-body effect plays a critical role on the structures and properties of clusters and condensed phases. Therefore the quantitative evaluation of the strength of many-body effects is important. In this paper, the three-body interactions and their contributions to the total interaction energy for hydrogen-bonded complexes composed of amide, dipeptide, uracil and water were evaluated at the second-order perturbation MP2 level of theory. It is found that the three-body interactions contribute as high as 10%—20% to the total interaction energy of the hydrogen-bonded complexes. It is also found that the three-body interaction is a short-range interaction, suggesting that the neighboring three-body effect should be taken into account in molecular simulation at least.

Key words: Three-body effect, Hydrogen-bonded complex, Interaction energy, Amide, Uracil, Clusters system, Condensed phases system

中图分类号:

O641

TrendMD:

李书实, 姜笑楠, 王长生. 含酰胺和尿嘧啶的氢键复合物的三体效应. 高等学校化学学报, 2014, 35(11): 2403.

LI Shushi, JIANG Xiaonan, WANG Changsheng. Three-body Effect in Hydrogen-bonded Complexes Containing Amides and Uracil^†. Chem. J. Chinese Universities, 2014, 35(11): 2403.

图/表 7

参考文献 33

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Complex	E_2B/(kJ·mol^-1)	E_3B/(kJ·mol^-1)	E_4B/(kJ·mol^-1)	E_total/(kJ·mol^-1)
1	-55.5(85.5%)	-9.4(14.5%)		-64.9
2	-72.6(83.2%)	-14.6(16.8%)		-87.2
3	-72.4(85.1%)	-12.6(14.9%)		-85.0
4	-83.2(85.3%)	-14.4(14.7%)		-97.6
5	-84.9(85.8%)	-14.1(14.2%)		-99.0
6	-104.7(96.3%)	-4.1(3.7%)		-108.8
7	-73.2(98.0%)	-1.5(2.0%)		-74.7
8	-82.5(84.2%)	-15.4(15.8%)		-97.9
9	-89.2(77.5%)	-23.9(20.7%)	-2.1(1.8%)	-115.2
10	-96.0(77.7%)	-22.7(18.4%)	-4.8(3.9%)	-123.5
11	-100.2(81.3%)	-21.0(17.0%)	-2.1(1.7%)	-123.3
12	-114.6(87.3%)	-17.5(13.4%)	-0.9(0.7%)	-131.2
13	-108.5(80.1%)	-24.7(18.2%)	-2.3(1.7%)	-135.5
14	-108.5(79.7%)	-25.4(18.7%)	-2.2(1.6%)	-136.1
15	-126.0(86.4%)	-19.5(13.3%)	-0.5(0.3%)	-146.0
16	-131.3(86.8%)	-19.4(12.8%)	-0.5(0.4%)	-151.2

Complex	E_2B/(kJ·mol^-1)	E_3B/(kJ·mol^-1)	E_4B/(kJ·mol^-1)	E_total/(kJ·mol^-1)
1	-55.5(85.5%)	-9.4(14.5%)		-64.9
2	-72.6(83.2%)	-14.6(16.8%)		-87.2
3	-72.4(85.1%)	-12.6(14.9%)		-85.0
4	-83.2(85.3%)	-14.4(14.7%)		-97.6
5	-84.9(85.8%)	-14.1(14.2%)		-99.0
6	-104.7(96.3%)	-4.1(3.7%)		-108.8
7	-73.2(98.0%)	-1.5(2.0%)		-74.7
8	-82.5(84.2%)	-15.4(15.8%)		-97.9
9	-89.2(77.5%)	-23.9(20.7%)	-2.1(1.8%)	-115.2
10	-96.0(77.7%)	-22.7(18.4%)	-4.8(3.9%)	-123.5
11	-100.2(81.3%)	-21.0(17.0%)	-2.1(1.7%)	-123.3
12	-114.6(87.3%)	-17.5(13.4%)	-0.9(0.7%)	-131.2
13	-108.5(80.1%)	-24.7(18.2%)	-2.3(1.7%)	-135.5
14	-108.5(79.7%)	-25.4(18.7%)	-2.2(1.6%)	-136.1
15	-126.0(86.4%)	-19.5(13.3%)	-0.5(0.3%)	-146.0
16	-131.3(86.8%)	-19.4(12.8%)	-0.5(0.4%)	-151.2

Complex	E_total/ (kJ·mol^-1)	E_2B/(kJ·mol^-1)	E_3B/(kJ·mol^-1)	E_other/ (kJ·mol^-1)	(E_total/n)/ (kJ·mol^-1)	(E_2B/n)/ (kJ·mol^-1)
1	-64.9	-55.5(85.5%)	-9.4(14.5%)		-21.6	-18.5
9	-115.2	-89.2(77.5%)	-23.9(20.7%)	-2.1(1.8%)	-28.8	-22.3
17	-20.0	-20.0(100%)			-20.0	-20.0
18	-151.7	-110.6(72.9%)	-36.2(23.9%)	-4.9(3.2%)	-30.3	-22.1
19	-187.2	-133.1(71.1%)	-46.7(24.9%)	-7.4(4.0%)	-31.2	-22.2
20	-105.0	-87.8(83.6%)	-16.2(15.4%)	-1.0(1.0%)	-26.3	-21.9
21	-135.4	-110.3(81.5%)	-23.4(17.3%)	-1.7(1.2%)	-27.1	-22.1
22	-31.1	-31.1(100%)			-31.1	-31.1
23	-163.1	-143.2(87.8%)	-18.5(11.3%)	-1.4(0.9%)	-40.8	-35.8
24	-210.9	-182.1(86.3%)	-25.8(12.3%)	-3.0(1.4%)	-42.2	-36.4

Complex	E_total/ (kJ·mol^-1)	E_2B/(kJ·mol^-1)	E_3B/(kJ·mol^-1)	E_other/ (kJ·mol^-1)	(E_total/n)/ (kJ·mol^-1)	(E_2B/n)/ (kJ·mol^-1)
1	-64.9	-55.5(85.5%)	-9.4(14.5%)		-21.6	-18.5
9	-115.2	-89.2(77.5%)	-23.9(20.7%)	-2.1(1.8%)	-28.8	-22.3
17	-20.0	-20.0(100%)			-20.0	-20.0
18	-151.7	-110.6(72.9%)	-36.2(23.9%)	-4.9(3.2%)	-30.3	-22.1
19	-187.2	-133.1(71.1%)	-46.7(24.9%)	-7.4(4.0%)	-31.2	-22.2
20	-105.0	-87.8(83.6%)	-16.2(15.4%)	-1.0(1.0%)	-26.3	-21.9
21	-135.4	-110.3(81.5%)	-23.4(17.3%)	-1.7(1.2%)	-27.1	-22.1
22	-31.1	-31.1(100%)			-31.1	-31.1
23	-163.1	-143.2(87.8%)	-18.5(11.3%)	-1.4(0.9%)	-40.8	-35.8
24	-210.9	-182.1(86.3%)	-25.8(12.3%)	-3.0(1.4%)	-42.2	-36.4

Complex	20	23	Complex	20	23
V^3B(1,2,3)/(kJ·mol^-1)	-4.8	-5.1	V^3B(2,3,4)/(kJ·mol^-1)	-5.2	-5.3
V^3B(1,2,4)/(kJ·mol^-1)	-0.4	-0.6	V^3B(2,3,5)/(kJ·mol^-1)	-0.4	-0.7
V^3B(1,3,4)/(kJ·mol^-1)	-0.2	-0.5	V^3B(2,4,5)/(kJ·mol^-1)	-0.3	-0.6
V^3B(1,2,5)/(kJ·mol^-1)	-0.1	-0.2	V^3B(3,4,5)/(kJ·mol^-1)	-4.7	-5.2
V^3B(1,3,5)/(kJ·mol^-1)	0.0	-0.1	E_3B/(kJ·mol^-1)	-16.2	-18.5
V^3B(1,4,5)/(kJ·mol^-1)	-0.1	-0.2