Reaktionen von organischen Schwefelverbindungen in der Atmosphäre:
Gespeichert in:
| Beteiligte Personen: | , |
|---|---|
| Format: | Buch |
| Sprache: | Deutsch |
| Veröffentlicht: |
Wuppertal
Bergische Univ., Gesamthochsch., PC
1996
|
| Schriftenreihe: | Bericht / Bergische Universität, Gesamthochschule Wuppertal, Fachbereich 9, Physikalische Chemie
35 |
| Schlagwörter: | |
| Links: | http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=007288308&sequence=000002&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA |
| Beschreibung: | Literaturverz. S. 143 - 155 |
| Umfang: | IV, 155 S. graph. Darst. |
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| adam_text | Titel: Reaktionen von organischen Schwefelverbindungen in der Atmosphäre
Autor: Becker, Karl H
Jahr: 1996
UMMERBITRT GEBRnTHOCHBCHULE UUPPERTRL FRCHBEREICH 3 PH!d5lk!RLI5CHE CHEMIE Reaktionen von organischen Schwefelverbindungen in der Atmosphäre K. H. Becker J. v. Patroescu Bericht Nr. 35 März 1996
I Contents Introduction.................................................................................................................................1 1. Sulphur compounds of atmospheric importance......................................................................3 1.1 Sources and sinks for sulphur compounds of atmospheric importance................................4 1.2 Atmospheric relevance of sulphur compounds....................................................................7 2. State of knowledge..............................................................................................................•••••9 2.1 Atmospheric chemistry of dimethyl sulphide.......................................................................9 2.2 The OH-initiated oxidation of dimethyl sulphide................................ ...10 3. Aims of the present work.....................................................................................................-12 4. Experimental Section.............................................................................................................13 4.1 Reaction chambers........................ 13 4.2 Analytical tools...............................................................................................................-16 4.3 Sources of radical..............................................................................................................17 5. Product analysis of the OH-initiated oxidation of dimethyl sulphide......................................19 5.1 Product analysis of the OH initiated oxidation of DMS in the absence of NO x ...................19 5.2 Discussion of the results....................................................................................................24 5.3 Formation of dimethyl sulphoxide in the OH-initiated oxidation of DMS in NO x -free
systems..........................................................................................................26 5.3.1 Discussion of the formation yield determined for dimethyl sulphoxide in the OH-initiated oxidation of DMS in the absence of NO x ..........................................26 5.3.2 Discussion of the formation mechanism of DMSO in the OH-initiated oxidation of DMS.......................................................................................29 5.4. Formation of dimethyl sulphone in the OH-initiated oxidation of DMS in NO x -free systems..........................................................................................................31 5.4.1 Discussion regarding the formation yield of DMS0 2 in the OH-initiated oxidation of DMS...........................................................................................................31 5.4.2 The contribution of the OH-initiated oxidation of DMSO to the formation yield of dimethyl sulphone in the OH-initiated oxidation of DMS..................................32 5.4.3 Discussion of the formation mechanism of dimethyl sulphone in the OH-initiated oxidation of DMS................. 33 5.5. Formation of S0 2 in the OH-initiated oxidation of DMS in NO x -free systems...................34
n 5.5.1 Discussion of the formation yield of SO 2 in the OH-initiated oxidation of DMS in the absence of NO x ......................................................................34 5.5.2 The contribution of the OH-initiated oxidation of DMSO to the formation yield of SO 2 in the OH-initiated oxidation of DMS.......................................................35 5.5.3 Discussion of the formation mechanism of SO 2 in the OH-initiated oxidation of DMS...37 5.6. Formation of methane sulphonic acid in the OH-initiated oxidation of DMS in NO x -free systems..........................................................................................................39 5.6.1 Discussion of the formation yield of methane sulphonic acid in the OH-initiated oxidation of DMS in the absence of NO x ....................................................39 5.6.2 The contribution of the OH-initiated oxidation of DMSO to the formation yield of methane sulphonic acid in the OH-initiated oxidation of DMS...........................40 5.6.3 Discussion of the formation mechanism of methane sulphonic acid in the OH-initiated oxidation of DMS.................................................................................40 5.7. Formation of methyl thiolformate in the OH-initiated oxidation of DMS in NO x -free systems..........................................................................................................42 5.7.1 Discussion of the formation yield of methyl thiolformate in the OH-initiated oxidation of DMS...........................................................................................................42 5.7.2 Discussion on the formation mechanism of MTF in the oxidation of DMS.....................45 5.8. Formation of carbonyl sulphide in the OH-initiated oxidation of DMS in the NO x -free systems....................................... 46 5.8.1 Discussion of the formation yield of carbonyl sulphide in the
OH-initiated oxidation of DMS...........................................................................................................46 5.8.2 Formation yield determined for carbonyl sulphide in the photolysis of dimethyl disulphide (DMDS).....................................................................................49 5.8.3 Discussion on the formation mechanism of carbonyl sulphide in the OH-initiated oxidation of DMS.......................................................................................50 5.9. Product analysis of the OH initiated oxidation of DMS in the presence of NO x .................53 5.10 The influence of NO x presence on the distribution of the products of the addition channel in the OH-initiated oxidation of DMS.....................................................55 5.10.1 Discussion of the formation yield of dimethyl sulphoxide in the OH-initiated oxidation of DMS in the presence of NO x ......................................................................55 5.10.2 Discussion of the formation yield of dimethyl sulphone in the OH-initiated oxidation of DMS in the presence of NO x ......................................................................57 5.10.3 Discussion on the influence of reactants other than O 2 on the chemical fate of the DMS-OH adduct...................................................................................................58 5.11 The formation of methylsulphonyl peroxynitrate in the OH-initiated oxidation of DMS in the presence of NO x .........................................................................61
ni 5.11.1 Discussion of the formation yield of methylsulphonyl peroxynitrate in the OH-initiated oxidation of DMS in the presence of NO x ................................................61 5.11.2 Discussion of the formation mechanism of the methylsulphonyl peroxynitrate in the OH-initiated oxidation of DMS.............................................................................63 5.12 The influence of NO x on the formation yield of S0 2 in the OH-initiated oxidation of DMS.............................................................................................................65 5.12.1 Discussion of the formation yield of S0 2 in the OH-initiated oxidation of DMS in the presence of NO x .....................................................................................65 5.12.2 Discussion of the influence of NO x on the formation mechanism of S0 2 in the OH-initiated oxidation of DMS......................................................................67 5.13 The influence of NO x presence on the formation yield of methane sulphonic acid in the OH-initiated oxidation of DMS........................................................69 5.13.1 Discussion of the formation yield of methane sulphonic acid in the OH-initiated oxidation of DMS in the presence of NO x ..................................................69 5.13.2 Discussion of the influence of NO x on the formation mechanism of methane sulphonic acid in the OH-initiated oxidation of DMS........................................70 5.14 The influence of NO x presence on the formation yield of methyl thiol-formate in the OH-initiated oxidation of DMS..........................................................71 5.14.1 Discussion of the formation yield of methyl thiolformate in the OH-initiated oxidation of DMS in the presence of NO x ..................................................71 5.14.2 Discussion of the influence of NO x on the formation mechanism of
methyl thiolformate in the OH-initiated oxidation of DMS.........................................73 5.15 The influence of NO x on the formation yield of carbonyl sulphide in the OH-initiated oxidation of DMS................................................................................74 5.15.1 Discussion of the formation yield of carbonyl sulphide in the OH-initiated oxidation of DMS in the presence of NO x ..................................................74 5.15.2 Discussion of the influence of NO x on the formation mechanism of carbonyl sulphide in the OH-initiated oxidation of DMS............................................75 6. Kinetic and product analysis of the OH-initiated oxidation of DMSO...................................77 6.1 Kinetic of the reaction DMSO+OH — products.................................................................77 6.2. Product analysis of the OH-initiated oxidation of dimethyl sulphoxide in the absence of NO x ...........................................................................................................79 6.3 Discussion of the mechanism of the OH-initiated oxidation of DMSO in the absence of NO x ...................................................:.......................................................81 6.4 Product analysis of the OH-initiated oxidation of dimethyl sulphoxide in the presence of NO x ......................................................................................................84
IV 6.5 Discussion of the mechanism of the OH-initiated oxidation of DMSO in the presence of NO x ......................................................................................................87 6.6 Discussion regarding the unidentified spectral features in the spectra recorded during experiments on the oxidation of DMSO..................................................88 7. Oxidation processes of methyl thiolformate..........................................................................90 7.1 Photolysis frequencies of methyl thiolformate...................................................................90 7.2 Product analysis of the UV-photolysis of methyl thiolformate...........................................91 7.2.1 Discussion of the chemical mechanism of the photolytic decomposition of MTF...........94 7.3 Kinetic and product analysis of the reaction of MTF with OH radicals.............................101 7.3.1 Discussion of the mechanism of the OH-initiated oxidation of MTF.............................102 7.4 Reactivity of MTF towards N0 3 radicals..........................................................................107 7.5 Kinetic and product analysis of the reaction of MTF with Cl atoms..................................107 7.5.1 Discussion of the chemical mechanism of the Cl-initiated oxidation of MTF.................110 8. Conclusions..........................................................................................................................114 Appendix I. Synthesis of methyl thiolformate....................................................................117 Appendix II. Determination of rate constants using the relative kinetic method...................119 Appendix III. Loss processes influencing the quantification of dimethyl sulphoxide, dimethyl sulphone and methyl thiolformate...................................................121 Appendix IV. Correction of the formation yields
of dimethyl sulphoxide and MTF in the OH-initiated oxidation of DMS to account for OH-losses and other loss processes.................................................................125 Appendix V. Gas phase IR-spectrum of methylsulphonyl peroxinitrate (CH 3 S(0)200N02) and estimation of its absorption cross-section..................127 Appendix VI. Synthesis of the methyl sulphenyl chloride (CH3SCI) and methyl sulphinyl chloride (CH 3 S(0)C1). Calibration of the IR-gas phase spectra of methyl sulphenyl chloride and methyl sulphinyl chloride...............129 Appendix VII. Origin and purity of the chemicals and gases used..........................................133 Appendix VIII. Concentration units used................................................................................134 Appendix IX. Reference spectra used...................................................................................134 References 143
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| illustrated | Illustrated |
| indexdate | 2024-12-20T10:02:47Z |
| institution | BVB |
| language | German |
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| physical | IV, 155 S. graph. Darst. |
| publishDate | 1996 |
| publishDateSearch | 1996 |
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| publisher | Bergische Univ., Gesamthochsch., PC |
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| series2 | Bericht / Bergische Universität, Gesamthochschule Wuppertal, Fachbereich 9, Physikalische Chemie |
| spellingShingle | Becker, Karl H. 1935-2021 Patroescu, J. von Reaktionen von organischen Schwefelverbindungen in der Atmosphäre Schwefelorganische Verbindungen (DE-588)4180419-3 gnd Atmosphäre (DE-588)4003397-1 gnd Chemische Reaktion (DE-588)4009853-9 gnd |
| subject_GND | (DE-588)4180419-3 (DE-588)4003397-1 (DE-588)4009853-9 |
| title | Reaktionen von organischen Schwefelverbindungen in der Atmosphäre |
| title_auth | Reaktionen von organischen Schwefelverbindungen in der Atmosphäre |
| title_exact_search | Reaktionen von organischen Schwefelverbindungen in der Atmosphäre |
| title_full | Reaktionen von organischen Schwefelverbindungen in der Atmosphäre K. H. Becker ; J. v. Patroescu. Bergische Universität, Gesamthochschule Wuppertal, Fachbereich 9, Physikalische Chemie |
| title_fullStr | Reaktionen von organischen Schwefelverbindungen in der Atmosphäre K. H. Becker ; J. v. Patroescu. Bergische Universität, Gesamthochschule Wuppertal, Fachbereich 9, Physikalische Chemie |
| title_full_unstemmed | Reaktionen von organischen Schwefelverbindungen in der Atmosphäre K. H. Becker ; J. v. Patroescu. Bergische Universität, Gesamthochschule Wuppertal, Fachbereich 9, Physikalische Chemie |
| title_short | Reaktionen von organischen Schwefelverbindungen in der Atmosphäre |
| title_sort | reaktionen von organischen schwefelverbindungen in der atmosphare |
| topic | Schwefelorganische Verbindungen (DE-588)4180419-3 gnd Atmosphäre (DE-588)4003397-1 gnd Chemische Reaktion (DE-588)4009853-9 gnd |
| topic_facet | Schwefelorganische Verbindungen Atmosphäre Chemische Reaktion |
| url | http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=007288308&sequence=000002&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA |
| volume_link | (DE-604)BV001823295 |
| work_keys_str_mv | AT beckerkarlh reaktionenvonorganischenschwefelverbindungeninderatmosphare AT patroescujvon reaktionenvonorganischenschwefelverbindungeninderatmosphare |
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