ROOOH: a missing piece of the puzzle for OH measurements in low-NO environments?

作者: Christa Fittschen , Mohamad Al Ajami , Sebastien Batut , Valerio Ferracci , Scott Archer-Nicholls

DOI: 10.5194/ACP-19-349-2019

关键词:

摘要: Abstract. Field campaigns have been carried out with the FAGE (fluorescence assay by gas expansion) technique in remote biogenic environments last decade to quantify situ concentrations of OH, main oxidant the atmosphere. These data revealed OH radicals up to a factor 10 higher than predicted by models, whereby disagreement increases decreasing NO concentration. This was interpreted as a major lack our understanding chemistry VOCs (volatile organic compounds), particularly isoprene, which are dominant pristine conditions. But interferences these measurements unknown origin have also discovered for some instruments: using pre-injector, all ambient is removed fast reaction before entering cell, and any remaining signal can be attributed an interference. is now systematically used measurements, allowing reliable quantification ambient along due to interference OH. However, disagreement between modelled measured high OH earlier field well the now-quantifiable background still not understood. We present this paper compelling idea that this interference, thus disagreement between model measurement campaigns, might at least partially unexpected decomposition new class molecule, ROOOH, within instruments. based on experiments, obtained set-up University Lille, supported a modelling study. Even though occurrence interference will be highly dependent design conditions different FAGE instruments, including ROOOH atmospheric models reflect a missing piece puzzle clean atmospheres.

参考文章(47)
Anna Novelli, Korbinian Hens, Cheryl Tatum Ernest, Monica Martinez, Anke C. Nölscher, Vinayak Sinha, Pauli Paasonen, Tuukka Petäjä, Mikko Sipilä, Thomas Elste, Christian Plass-Dülmer, Gavin J. Phillips, Dagmar Kubistin, Jonathan Williams, Luc Vereecken, Jos Lelieveld, Hartwig Harder, Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument Atmospheric Chemistry and Physics. ,vol. 17, pp. 7807- 7826 ,(2017) , 10.5194/ACP-17-7807-2017
Yanli Liu, Long Chen, Dongping Chen, Weina Wang, Fengyi Liu, Wenliang Wang, Computational Study on Mechanisms of C 2 H 5 O 2 +OH Reaction and Properties of C 2 H 5 O 3 H Complex Chemical Research in Chinese Universities. ,vol. 33, pp. 623- 630 ,(2017) , 10.1007/S40242-017-7055-4
Hendrik Fuchs, Anna Novelli, Michael Rolletter, Andreas Hofzumahaus, Eva Y. Pfannerstill, Stephan Kessel, Achim Edtbauer, Jonathan Williams, Vincent Michoud, Sebastien Dusanter, Nadine Locoge, Nora Zannoni, Valerie Gros, Francois Truong, Roland Sarda-Esteve, Danny R. Cryer, Charlotte A. Brumby, Lisa K. Whalley, Daniel Stone, Paul W. Seakins, Dwayne E. Heard, Coralie Schoemaecker, Marion Blocquet, Sebastien Coudert, Sebastien Batut, Christa Fittschen, Alexander B. Thames, William H. Brune, Cheryl Ernest, Hartwig Harder, Jennifer B. A. Muller, Thomas Elste, Dagmar Kubistin, Stefanie Andres, Birger Bohn, Thorsten Hohaus, Frank Holland, Xin Li, Franz Rohrer, Astrid Kiendler-Scharr, Ralf Tillmann, Robert Wegener, Zhujun Yu, Qi Zou, Andreas Wahner, Comparison of OH reactivity measurements in the atmospheric simulation chamber SAPHIR Atmospheric Measurement Techniques. ,vol. 10, pp. 4023- 4053 ,(2017) , 10.5194/AMT-10-4023-2017
Emmanuel Assaf, Coralie Schoemaecker, Luc Vereecken, Christa Fittschen, The reaction of fluorine atoms with methanol: yield of CH3O/CH2OH and rate constant of the reactions CH3O + CH3O and CH3O + HO2 Physical Chemistry Chemical Physics. ,vol. 20, pp. 10660- 10670 ,(2018) , 10.1039/C7CP05770A
Valerio Ferracci, Ines Heimann, N. Luke Abraham, John A. Pyle, Alexander T. Archibald, Global modelling of the total OH reactivity: investigations on the “missing” OH sink and its atmospheric implications Atmospheric Chemistry and Physics. ,vol. 18, pp. 7109- 7129 ,(2018) , 10.5194/ACP-18-7109-2018
Paul O. Wennberg, Kelvin H. Bates, John D. Crounse, Leah G. Dodson, Renee C. McVay, Laura A. Mertens, Tran B. Nguyen, Eric Praske, Rebecca H. Schwantes, Matthew D. Smarte, Jason M. St Clair, Alexander P. Teng, Xuan Zhang, John H. Seinfeld, Gas-Phase Reactions of Isoprene and Its Major Oxidation Products. Chemical Reviews. ,vol. 118, pp. 3337- 3390 ,(2018) , 10.1021/ACS.CHEMREV.7B00439
Emmanuel Assaf, Coralie Schoemaecker, Luc Vereecken, Christa Fittschen, Experimental and theoretical investigation of the reaction of RO2 radicals with OH radicals: Dependence of the HO2 yield on the size of the alkyl group International Journal of Chemical Kinetics. ,vol. 50, pp. 670- 680 ,(2018) , 10.1002/KIN.21191
Rebecca L. Caravan, M. Anwar H. Khan, Judit Zádor, Leonid Sheps, Ivan O. Antonov, Brandon Rotavera, Krupa Ramasesha, Kendrew Au, Ming-Wei Chen, Daniel Rösch, David L. Osborn, Christa Fittschen, Coralie Schoemaecker, Marius Duncianu, Asma Grira, Sebastien Dusanter, Alexandre Tomas, Carl J. Percival, Dudley E. Shallcross, Craig A. Taatjes, The reaction of hydroxyl and methylperoxy radicals is not a major source of atmospheric methanol Nature Communications. ,vol. 9, pp. 4343- ,(2018) , 10.1038/S41467-018-06716-X
Xinrong Ren, Hartwig Harder, Monica Martinez, Ian C. Faloona, David Tan, Robert L. Lesher, Piero Di Carlo, James B. Simpas, William H. Brune, Interference Testing for Atmospheric HOx Measurements by Laser-induced Fluorescence Journal of Atmospheric Chemistry. ,vol. 47, pp. 169- 190 ,(2004) , 10.1023/B:JOCH.0000021037.46866.81