Theoretical study on reaction mechanism of sulfuric acid and ammonia and hydration of (NH4)2SO4
Theoretical study on reaction mechanism of sulfuric acid and ammonia and hydration of (NH4)2SO4
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硫酸与氨反应机理及(NH4)2SO4水合的理论研究
DOI：
10.1007/s00214-012-1103-4
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发表时间：
2012-02
影响因子：
1.7
通讯作者：
Ze-Sheng Li
中科院分区：
文献类型：
--
作者：
Wei-Wei Liu;Xiao-Lin Wang;Shi-Lu Chen;Yun-Hong Zhang;Ze-Sheng Li
为了研究（NH 4）2SO 4气溶胶的成核机理，在M06/6-311++G（d，p）水平下，模拟了无水条件下硫酸与氨的反应.结果表明，（NH 4）2SO 4和NH 4 HSO 4单元可能在气相中不含水分子的情况下瞬间存在，这是一个理论预测，需要进一步的实验验证。为了进一步研究初生核的生长，在M06/6-311++G（d，p）和B3 LYP/6- 311 ++ G（d，p）水平上计算了（NH 4）2SO 4·（H2O）n（n= 0-9）的几何构型、能量和谐振频率.理论振动频率的变化趋势与实验结果一致。分析了水分子对（NH_4）_2SO_4性质的影响。我们的结果表明，M06是更准确的比B3 LYP这类系统。此外，还采用第一性原理分子动力学方法模拟了两种能量相近的代表性异构体的结构转变，以了解溶剂共享离子对与接触离子对之间的关系。
In order to understand the mechanism of nucleation of (NH4)2SO4aerosol, the reaction between sulfuric acid and ammonia in the absence of water molecule is performed at M06/6-311++G(d,p) level. The results show that the (NH4)2SO4and NH4HSO4units may exist instantaneously in gas phase without water molecule, which is a theoretical prediction that needs detection by further experiment. To further study the growth of the primary nuclei, the geometries, energies, and harmonic frequencies of (NH4)2SO4· (H2O)n(n= 0–9) are calculated both at M06/6-311++G(d,p) and B3LYP/6-311++G(d,p) levels. The tendency of the theoretical vibration frequencies is in accordance with the experimental results. The influence of the water molecule on the properties of (NH4)2SO4is also analyzed. Our results indicate that M06 is more accurate than B3LYP for this kind of system. Moreover, the first principle molecular dynamics method is used to simulate the structural transformation for two representative isomers whose energies are close, to understand the relationship between solvent-shared ion pairs and contact ion pairs.
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影响因子：
2.2
作者：
Zhao Ya-ying;Y. ZengEddy;Zhang Xi-hui;Ma Lin;Tao Fu-ming
通讯作者：
Zhao Ya-ying;Y. ZengEddy;Zhang Xi-hui;Ma Lin;Tao Fu-ming
DOI：
10.1063/1.2943671
发表时间：
2008-06
期刊：
The Journal of chemical physics
影响因子：
--
作者：
S. Karthikeyan;Jitender Singh;Mina Park;Rajesh Kumar;Kwang Soo Kim
通讯作者：
S. Karthikeyan;Jitender Singh;Mina Park;Rajesh Kumar;Kwang Soo Kim
影响因子：
4.4
作者：
Yi-Siang Wang;Jyh‐Chiang Jiang;Chia‐Liang Cheng;S. Lin;Yungja Lee;H. Chang
通讯作者：
Yi-Siang Wang;Jyh‐Chiang Jiang;Chia‐Liang Cheng;S. Lin;Yungja Lee;H. Chang
影响因子：
3.1
作者：
Hock Lim;Chih-Pei Chang
通讯作者：
Hock Lim;Chih-Pei Chang
影响因子：
4.4
作者：
C. Bauschlicher;S. Langhoff;H. Partridge;J. Rice;A. Komornicki
通讯作者：
C. Bauschlicher;S. Langhoff;H. Partridge;J. Rice;A. Komornicki