Identification and characterization of aging products in the glyoxal/ammonium sulfate system - implications for light-absorbing material in atmospheric aerosols

被引:143
作者
Kampf, C. J. [1 ]
Jakob, R. [1 ]
Hoffmann, T. [1 ]
机构
[1] Johannes Gutenberg Univ Mainz, Inst Inorgan & Analyt Chem, D-55128 Mainz, Germany
关键词
SECONDARY ORGANIC AEROSOL; HETEROGENEOUS REACTIONS; CHEMICAL-COMPOSITION; PARTICULATE MATTER; OLIGOMER FORMATION; GLYOXAL UPTAKE; METHYLGLYOXAL; SOA; IMIDAZOLE; HYDRATION;
D O I
10.5194/acp-12-6323-2012
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In this study we report the identification of bicyclic imidazoles in aqueous aerosol mimics using HPLC-ESI-MS/MS. 2,2'-Biimidazole was identified to be a major contributor to the 280 nm absorbance band observed in mixtures of glyoxal and ammonium sulfate, despite the fact that its production rate is two orders of magnitude lower than the previously reported production rates of imidazole or imidazole-2-carboxaldehyde. The molar absorptivity of 2,2'-biimidazole was determined to be (36 690 +/- 998) M-1 cm(-1). This demonstrates the necessity of molecular product identification at trace levels to enable a better understanding of relevant absorbing species. Additionally, the formation of lower polarity products including formamides of imidazoles is proposed. The role of imidazoles and other light-absorbing species in the formation of SOA and optical properties of SOA is discussed and potentially interesting fields for future investigations are outlined.
引用
收藏
页码:6323 / 6333
页数:11
相关论文
共 44 条
[21]   Chemical composition and association of size-differentiated aerosols at a suburban site in a semi-arid tract of India [J].
Kulshrestha, UC ;
Saxena, A ;
Kumar, N ;
Kumari, KM ;
Srivastava, SS .
JOURNAL OF ATMOSPHERIC CHEMISTRY, 1998, 29 (02) :109-118
[22]   Reactive uptake of glyoxal by particulate matter [J].
Liggio, J ;
Li, SM ;
McLaren, R .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2005, 110 (D10) :1-13
[23]   Heterogeneous reactions of glyoxal on particulate matter: Identification of acetals and sulfate esters [J].
Liggio, J ;
Li, SM ;
McLaren, R .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2005, 39 (06) :1532-1541
[24]   Aqueous chemistry and its role in secondary organic aerosol (SOA) formation [J].
Lim, Y. B. ;
Tan, Y. ;
Perri, M. J. ;
Seitzinger, S. P. ;
Turpin, B. J. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (21) :10521-10539
[25]   Oligomer formation in evaporating aqueous glyoxal and methyl glyoxal solutions [J].
Loeffler, Kirsten W. ;
Koehler, Charles A. ;
Paul, Nichole M. ;
De Haan, David O. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (20) :6318-6323
[26]   Long tethers binding redox centers to polymer backbones enhance electron transport in enzyme "wiring" hydrogels [J].
Mao, F ;
Mano, N ;
Heller, A .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (16) :4951-4957
[27]   Products and Kinetics of the Liquid-Phase Reaction of Glyoxal Catalyzed by Ammonium Ions (NH4+) [J].
Noziere, Barbara ;
Dziedzic, Pawel ;
Cordova, Armando .
JOURNAL OF PHYSICAL CHEMISTRY A, 2009, 113 (01) :231-237
[28]   Gas/particle partitioning and secondary organic aerosol yields [J].
Odum, JR ;
Hoffmann, T ;
Bowman, F ;
Collins, D ;
Flagan, RC ;
Seinfeld, JH .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1996, 30 (08) :2580-2585
[29]   AN ABSORPTION-MODEL OF THE GAS AEROSOL PARTITIONING INVOLVED IN THE FORMATION OF SECONDARY ORGANIC AEROSOL [J].
PANKOW, JF .
ATMOSPHERIC ENVIRONMENT, 1994, 28 (02) :189-193
[30]   Precipitation and aerosol studies in India [J].
Parashar, DC ;
Kulshrestha, UC ;
Jain, M .
ENVIRONMENTAL MONITORING AND ASSESSMENT, 2001, 66 (01) :47-61