A theoretical study of temperature dependence of cluster formation from sulfuric acid and ammonia

被引：17

作者：

Chon, Nara Lee ^{[1
]}

Lee, Shan-Hu ^{[2
]}

Lin, Hai ^{[1
]}

机构：

[1] Univ Colorado, Dept Chem, Denver, CO 80217 USA

[2] Kent State Univ, Coll Publ Hlth, Kent, OH 44242 USA

来源：

CHEMICAL PHYSICS | 2014年 / 433卷

基金：

美国国家科学基金会;

关键词：

Sulfuric acid; Ammonia; Cluster; Nucleation; Temperature dependence; MOLECULAR-ORBITAL METHODS; DENSITY-FUNCTIONAL THEORY; GAUSSIAN-TYPE BASIS; BASIS-SETS; PARTICLE FORMATION; EARTHS ATMOSPHERE; GAS-PHASE; NUCLEATION; H2SO4; AEROSOL;

D O I：

10.1016/j.chemphys.2014.01.010

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

We have performed density functional theory (BL3YP) and ab initio (MP2) calculations to investigate the energetics of the cluster formation for (NH3)m(H2SO4) and (NH3)(H2SO4)(n) (m, n = 1-6) in the atmospherically-relevant temperature range between 200 and 300 K. For (NH3)(m)(H2SO4) clusters, the binding increases from m = 1 to 6 at 200 K, while the most stable complex at 300 K is the cluster with m = 2. For (NH3)(H2SO4) n clusters, the binding is more stable for those with larger n. There is a strong temperature dependence for the (NH3)(m)(H2SO4) cluster formation; the lowest free energy shifts from m = 6 at T = 200 K to m = 5 around T = 240 K and further to m = 2 at T >= 280 K. The temperature effects on (NH3) (H2SO4)(n) clusters are much less stronger, while there is still a similar trend which favors larger n in the entire temperature range from 200 to 300 K. (C) 2014 Elsevier B.V. All rights reserved.

引用

页码：60 / 66

页数：7

共 72 条

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