Photochemistry of reduced sulfur compounds in a landfill environment

This study examines the distribution characteristics of reduced sulfur compounds (RSCs such as DMS, CS2 ,H 2S, DMDS, and CH3SH) and their photochemical reactions in landfill air. The photochemical conversions of RSCs to a further oxidized form, SO2 were evaluated in the landfill site using a photochemical box model. Measurements of RSCs were carried out from landfill areas in Daegu, Korea, during a wintertime period (e.g., 13–16 Jan 2004). This study indicated that H2S was the most dominant RSC in the landfill, with the concentrations of 4.275.8 ppbv. The chemical species of RSCs, which may exert influences on the SO2 production depending on sampling conditions, were found to include DMS, DMDS, and H2S. In general, the RSC contribution to the observed SO2 levels was insignificant in the sampling sites investigated. Overall, the extent of the RSC oxidation to the observed SO2 varied dramatically during the sampling period. The photochemical conversion of the RSCs in the landfill environment can account for about 15% of the observed SO2, on average. There was a strong correlation between DMS and SO2 concentration levels during the study period. r 2005 Elsevier Ltd. All rights reserved.

[1]  Youn-Sang Choi,et al.  Characterization of malodorous sulfur compounds in landfill gas , 2005 .

[2]  Shao-Meng Li,et al.  Seasonal variations of dimethylsulfide emissions and atmospheric sulfur and nitrogen species over the western North Atlantic Ocean , 1991 .

[3]  C. N. Hewitt,et al.  Dimethylsulfide and its oxidation products at two sites in Brittany (France) , 1999 .

[4]  N. Jensen,et al.  Observation of DMSO and CH3S(O)OH from the gas phase reaction between DMS and OH , 1996 .

[5]  Patrick M. Crill,et al.  Natural and anthropogenic methane sources in New England , 1999 .

[6]  Simon F. Watts,et al.  The mass budgets of carbonyl sulfide, dimethyl sulfide, carbon disulfide and hydrogen sulfide , 2000 .

[7]  T. Wallington,et al.  Absolute rate constants for the gas-phase reactions of the nitrogen trioxide radical with methanethiol, dimethyl sulfide, dimethyl disulfide, hydrogen sulfide, sulfur dioxide, and dimethyl ether over the temperature range 280-350 K , 1986 .

[8]  A. Bandy,et al.  Low yields of SO2 from dimethyl sulfide oxidation in the marine boundary layer , 1992 .

[9]  Andreas Wahner,et al.  A study of nighttime nitrogen oxide oxidation in a large reaction chamber : The fate of NO2, N2O5, HNO3, and O3 at different humidities , 1996 .

[10]  Aysen Muezzinoglu,et al.  A study of volatile organic sulfur emissions causing urban odors. , 2003, Chemosphere.

[11]  C. E. Junge Sulfur in the atmosphere , 1960 .

[12]  J. Houghton,et al.  Climate change 2001 : the scientific basis , 2001 .

[13]  H. Haraguchi,et al.  Spatial and temporal characteristics of urban atmospheric methane in Nagoya City, Japan:: an assessment of the contribution from regional landfills , 2001 .

[14]  A. Wahner,et al.  Heterogeneous reaction of N2O5 on sodium nitrate aerosol , 1998 .

[15]  Zang-Ho Shon,et al.  Evaluation of the DMS flux and its conversion to SO2 over the southern ocean , 2001 .

[16]  H. Skov,et al.  Products and mechanisms of the gas phase reactions of NO3 with CH3SCH3, CD3SCD3, CH3SH and CH3SSCH3 , 1992 .

[17]  R. A. Cox,et al.  Evaluated kinetic and photochemical data for atmospheric chemistry: Volume III - gas phase reactions of inorganic halogens , 2006 .

[18]  Alan C. Lloyd,et al.  A chemical mechanism for use in long‐range transport/acid deposition computer modeling , 1986 .

[19]  A. Bandy,et al.  Chemistry of dimethyl sulfide in the equatorial Pacific atmosphere , 1996 .

[20]  P. Wine,et al.  Kinetics and mechanism of hydroxyl reactions with organic sulfides , 1986 .

[21]  J. Seinfeld,et al.  Photooxidation of dimethyl sulfide and dimethyl disulfide. I: Mechanism development , 1990 .

[22]  Jeffrey R. Brook,et al.  Description and evaluation of a model of deposition velocities for routine estimates of dry deposition over North America. Part II: review of past measurements and model results , 1999 .

[23]  M. Molina,et al.  Chemical kinetics and photochemical data for use in stratospheric modeling , 1985 .

[24]  B. R. Gurjar,et al.  Emission Estimates and Trends (1990-2000) for Megacity Delhi and Implications , 2004 .

[25]  A. R. Ravishankara,et al.  Kinetics of hydroxyl radical reactions with the atmospheric sulfur compounds hydrogen sulfide, methanethiol, ethanethiol, and dimethyl disulfide , 1981 .

[26]  J. Douglas Faires,et al.  Numerical Analysis , 1981 .

[27]  D. Lenschow,et al.  Dimethyl sulfide oxidation in the equatorial Pacific: Comparison of model simulations with field observations for DMS, SO2, H2SO4(g), MSA(g), MS and NSS , 1999 .

[28]  U. Platt,et al.  Chemistry and oxidation capacity of the nitrate radical in the continental boundary layer near Berlin , 2001 .

[29]  C. Leck,et al.  Seasonal and short-term variability in dimethyl sulfide, sulfur dioxide and biogenic sulfur and sea salt aerosol particles in the arctic marine boundary layer during summer and autumn , 1996 .

[30]  Ki‐Hyun Kim,et al.  Assessment of the photochemistry of OH and NO3 on Jeju Island during the Asian-dust-storm period in the spring of 2001. , 2003, Chemosphere.

[31]  Ki-Hyun Kim,et al.  Performance characterization of the GC/PFPD for H2S, CH3SH, DMS, and DMDS in air , 2005 .