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Theoretical Studies on Mechanism and Rate Constant of Gas Phase Hydrolysis of Glyoxal Catalyzed by Sulfuric Acid

文献类型：期刊论文

作者Huang, Ming-qiang1,2,3; Cai, Shun-you1,2; Liao, Ying-min3; Zhao, Wei-xiong4; Hu, Chang-jin4; Wang, Zhen-ya4; Zhang, Wei-jun4
刊名CHINESE JOURNAL OF CHEMICAL PHYSICS
出版日期2016-06-01
卷号29期号:3页码:335-343
关键词Glyoxal Hydrolysis Sulfuric Acid Acid-catalyzed Mechanism
DOI10.1063/1674-0068/29/cjcp1509193
文献子类Article
英文摘要The gas phase hydration of glyoxal (HCOCHO) in the presence of sulfuric acid (H2SO4) were studied by the high-level quantum chemical calculations with M06-2X and CCSD(T) theoretical methods and the conventional transition state theory (CTST). The mechanism and rate constant of the five different reaction paths are considered corresponding to HCOCHO+H2O, HCOCHO+H2O. . . H2O, HCOCHO. . . H2O+H2O, HCOCHO+H2O. . . H2SO4 and HCOCHO. . . H2O+H2SO4. Results show that H2SO4 has a strong catalytic ability, which can significantly reduce the energy barrier for the hydration reaction of glyoxal. The energy barrier of hydrolysis of glyoxal in gas phase is lowered to 7.08 kcal/mol from 37.15 kcal/mol relative to pre-reactive complexes at the CCSD(T)/6-311++G(3df, 3pd)//M06-2X/6-311++G(3df, 3pd) level of theory. The rate constant of the H2SO4 catalyzed hydrolysis of glyoxal is 1.34x10(-11) cm(3)/(molecule"s), about 10(13) higher than that involving catalysis by an equal number of water molecules, and is greater than the reaction rate of glyoxal reaction with OH radicals of 1.10x10(-11) cm(3)/(molecule"s) at the room temperature, indicating that the gas phase hydrolysis of glyoxal of H2SO4 catalyst is feasible and could compete with the reaction glyoxal+OH under certain atmospheric conditions. This study may provide useful information on understanding the mechanistic features of inorganic acid-catalyzed hydration of glyoxal for the formation of oligomer.
WOS关键词ORGANIC AEROSOL FORMATION ; OH ; CHEMISTRY ; FORMALDEHYDE ; TOLUENE ; WATER ; SITE ; IDENTIFICATION ; KINETICS ; SULFATE
WOS研究方向Physics
语种英语
WOS记录号WOS:000381313000009
资助机构National Natural Science Foundation of China(41575118 ; National Natural Science Foundation of China(41575118 ; National Natural Science Foundation of China(41575118 ; National Natural Science Foundation of China(41575118 ; Outstanding Youth Science Foundation of Fujian Province of China(2015J06009) ; Outstanding Youth Science Foundation of Fujian Province of China(2015J06009) ; Outstanding Youth Science Foundation of Fujian Province of China(2015J06009) ; Outstanding Youth Science Foundation of Fujian Province of China(2015J06009) ; Natural Science Foundation of Fujian Province of China(2015J05028) ; Natural Science Foundation of Fujian Province of China(2015J05028) ; Natural Science Foundation of Fujian Province of China(2015J05028) ; Natural Science Foundation of Fujian Province of China(2015J05028) ; 41305109 ; 41305109 ; 41305109 ; 41305109 ; 21502086 ; 21502086 ; 21502086 ; 21502086 ; 41575126 ; 41575126 ; 41575126 ; 41575126 ; 41330424 ; 41330424 ; 41330424 ; 41330424 ; 41127001) ; 41127001) ; 41127001) ; 41127001) ; National Natural Science Foundation of China(41575118 ; National Natural Science Foundation of China(41575118 ; National Natural Science Foundation of China(41575118 ; National Natural Science Foundation of China(41575118 ; Outstanding Youth Science Foundation of Fujian Province of China(2015J06009) ; Outstanding Youth Science Foundation of Fujian Province of China(2015J06009) ; Outstanding Youth Science Foundation of Fujian Province of China(2015J06009) ; Outstanding Youth Science Foundation of Fujian Province of China(2015J06009) ; Natural Science Foundation of Fujian Province of China(2015J05028) ; Natural Science Foundation of Fujian Province of China(2015J05028) ; Natural Science Foundation of Fujian Province of China(2015J05028) ; Natural Science Foundation of Fujian Province of China(2015J05028) ; 41305109 ; 41305109 ; 41305109 ; 41305109 ; 21502086 ; 21502086 ; 21502086 ; 21502086 ; 41575126 ; 41575126 ; 41575126 ; 41575126 ; 41330424 ; 41330424 ; 41330424 ; 41330424 ; 41127001) ; 41127001) ; 41127001) ; 41127001)
源URL[http://ir.hfcas.ac.cn:8080/handle/334002/30829]  
专题合肥物质科学研究院_中科院安徽光学精密机械研究所
作者单位1.Minnan Normal Univ, Coll Chem & Environm, Zhangzhou 363000, Peoples R China
2.Fujian Prov Key Lab Modern Analyt Sci & Separat T, Zhangzhou 363000, Peoples R China
3.Xiamen Univ, Coll Tan Kah Kee, Dept Environm Sci & Engn, Zhangzhou 363105, Peoples R China
4.Chinese Acad Sci, Lab Atmospher Physicochem, Anhui Inst Opt & Fine Mech, Hefei 230031, Peoples R China
推荐引用方式
GB/T 7714		 Huang, Ming-qiang,Cai, Shun-you,Liao, Ying-min,et al. Theoretical Studies on Mechanism and Rate Constant of Gas Phase Hydrolysis of Glyoxal Catalyzed by Sulfuric Acid[J]. CHINESE JOURNAL OF CHEMICAL PHYSICS,2016,29(3):335-343.
APA Huang, Ming-qiang.,Cai, Shun-you.,Liao, Ying-min.,Zhao, Wei-xiong.,Hu, Chang-jin.,...&Zhang, Wei-jun.(2016).Theoretical Studies on Mechanism and Rate Constant of Gas Phase Hydrolysis of Glyoxal Catalyzed by Sulfuric Acid.CHINESE JOURNAL OF CHEMICAL PHYSICS,29(3),335-343.
MLA Huang, Ming-qiang,et al."Theoretical Studies on Mechanism and Rate Constant of Gas Phase Hydrolysis of Glyoxal Catalyzed by Sulfuric Acid".CHINESE JOURNAL OF CHEMICAL PHYSICS 29.3(2016):335-343.

入库方式： OAI收割

来源：合肥物质科学研究院

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