Ozone production in the atmosphere simulation chamber SAPHIR:
Saved in:
| Main Author: | |
|---|---|
| Format: | Thesis Book |
| Language: | English |
| Published: |
Jülich
Forschungszentrum, Zentralbibliothek
2008
|
| Series: | Schriften des Forschungszentrums Jülich : Reihe Energie & Umwelt
2 |
| Subjects: | |
| Online Access: | Inhaltsverzeichnis |
| Physical Description: | XIV, 147 S. Ill., graph. Darst. 24 cm |
| ISBN: | 9783893365135 3893365133 |
Staff View
MARC
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| 100 | 1 | |a Richter, Cornelia Anna |e Verfasser |4 aut | |
| 245 | 1 | 0 | |a Ozone production in the atmosphere simulation chamber SAPHIR |c Cornelia Anna Richter |
| 264 | 1 | |a Jülich |b Forschungszentrum, Zentralbibliothek |c 2008 | |
| 300 | |a XIV, 147 S. |b Ill., graph. Darst. |c 24 cm | ||
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| 490 | 1 | |a Schriften des Forschungszentrums Jülich : Reihe Energie & Umwelt |v 2 | |
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Record in the Search Index
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| adam_text | Contents
Introduction 1
1.1 Ozone................................ 3
1.2 Ozone Precursor Species...................... 6
1.3 Isoprene............................... 8
1.4 Peroxyacyl Nitrates......................... 8
1.5 Chemical Weather Forecast .................... 9
1.6 Chamber Experiments....................... 10
1.7 Aim of this Thesis ......................... 12
Theory 13
2.1 Gas Phase Chemistry........................ 13
2.1.1 Tropospheric Ozone Production.............. 14
2.1.2 Chemical Regimes ..................... 19
2.2 Chemical Mechanisms ....................... 20
2.3 Numerical Solving.......................... 23
Experimentals 25
3.1 The SAPHIR Chamber....................... 25
3.1.1 Dilution........................... 28
3.1.2 HONO Source........................ 28
3.1.3 HCHO Source........................ 29
3.1.4 Background Reactivity................... 36
3.1.5 Other Sources........................ 36
3.1.6 Deposition at the Walls .................. 37
3.2 Instrumentation........................... 37
3.2.1 Ozone Measurements.................... 39
3.2.2 Reactive Species ...................... 39
3.2.3 Volatile Organic Compounds................ 41
3.2.4 NOy Species......................... 42
3.2.5 Photolysis Frequencies................... 43
3.2.6 Meteorological Conditions................. 44
Ozone Production Due to Isoprene Degradation 47
4.1 Fully Time Dependent MCM Model Runs ............ 49
4.1.1 Results............................ 51
4.1.2 Discussion.......................... 55
4.2 First Degradation Step Approach................. 58
4.2.1 Used Method........................ 59
4.2.2 Results............................ 63
4.2.3 Discussion.......................... 67
4.3 OH Lifetime............................. 69
4.3.1 Idea............................. 70
4.3.2 Used Method........................ 1
4.3.3 Results and Discussion................... 74
4.4 Conclusion.............................. 79
5 Methacrolein Degradation Studies 81
5.1 OH Induced MACR Degradation ................. 81
5.1.1 Used MCM Model ..................... 82
5.1.2 Observations ........................ 85
5.1.3 Results............................ 88
5.2 Photolysis and Ozonolysis of MACR ............... 92
5.2.1 Used Models . ....................... 92
5.2.2 Results............................ 93
5.3 NO3 Induced MACR Degradation................. 95
5.3.1 Used Models......................... 97
5.3.2 Results............................ 98
5.4 Conclusion.............................. 101
6 Resume and Outlook 103
A Used Gas Phase Chemistry Mechanisms 107
A.I Function Definitions ........................107
A.2 Default Settings and MCM Constants...............108
A.3 Inorganic Section..........................109
A.4 MCM Isoprene Subset.......................110
A.4.1 Chamber-Features in the Isoprene MCM Model.....122
B Tables of Analyzed Experiments 127
C Statistics 129
List of Figures
1.1 Picture of ozone injury of a Salix caprca leaf........... -I
1.2 Graphic formulas of some biogenie VOCs............. 7
1.3 Role of Chamber Experiments in Atmospheric Chemistry .... 11
2.1 Ozone null cycle........................... 11
2.2 Ideal ozone production cycle.................... 18
2.3 Chain terminating reactions.................... 19
2.4 Ozone production isopleths plot.................. 21
3.1 Picture of the SAPHIR chamber.................. 25
3.2 Water dependence of the SAPHIR HCHO source ........ 31
3.3 Changes of the SAPHIR HCHO source over time ........ 34
3.4 Other sources of trace gases found during the standard experi-
ment at the 31st Aug 2006..................... 38
4.1 Ox fitting lines at GC sampling times............... 49
4.2 Fully time dependent isoprene model run............. 53
4.3 Correlations of the net Ox productions between measurements
and fully time dependent model runs............... 54
4.4 Correlations for measured vs. modelled VOC concentrations for
Sep 2005 experiments........................ 5(i
4.5 Variation of amplifying factors over time............. 60
4.6 Decision tree for the determination of amplifying factors ... 62
4.7 Time series of fitted versus first-degradation-step approach de-
rived Ox production on 15th of May 2006............. 65
4.8 Comparison of fitted and FDS calculated Ox production for ex-
periments between Sep 2005 and June 2006............ 66
4.9 Methacrolein degradation induced by OH as proposed by the
MCM ................................ 68
4.10 Time series of defining parameters for the integrated amplifying
factor ................................ 73
4.11 Correlation between the net Ox production and the OH loss rate
for all experiments......................... 71
4.12 Averaged OH loss rate times amplifying factor over mean net
Ox production............................ 75
4.13 Roundoff errors occurring in Foh calculation........... 76
4.14 Dependencies of the integrated amplifying factor Fqh...... 77
5.1 NOX discrepancy at the OH induced MACR degradation .... 83
5.2 Comparison of the NOX time series for different MCM model
parameters and the NOX measurements..............84
5.3 Rate coefficients used by the MCM and recommended by IU-
PAC for the MACR + OH reaction.................87
5.4 Reaction scheme recommended by IUPAC for the MACR + OH
reaction...............................89
5.5 IUPAC model runs for the OH induced MACR degradation . . 91
5.6 PAN and MPAN measurements and model concentrations for
OH induced MACR degradation..................92
5.7 Reaction scheme of the MACR photolysis IUPAC implemen-
tation.................................94
5.8 Reaction scheme of the MACR ozonolysis.............95
5.9 MACR photolysis and ozonolysis experiment on 12th Apr 2007 . 96
5.10 NO3 induced MACR degradation scheme implemented in the
IUPAC model............................98
5.11 Nighttime MACR degradation experiments on 13th Nov 2006
and 13th Apr 2007.........................100
Vlll
List of Tables
1.1 Selected components of the earth s atmosphere.......... 2
1.2 Ozone threshold values for the European Union......... 5
3.1 Technical specification of the SAPHIR chamber.......... 27
3.2 Fitting parameters of the HCHO source s water dependence . . 33
3.3 Overview of the instrumentation at SAPHIR........... 15
4.1 Measurement vs. model correlation parameters of the net Ox
production.............................. 52
4.2 Measurement vs. model correlation parameters for VOC mea-
surements .............................. 57
5.1 MCM model parameters for the OH induced MACR degrada-
tion experiments .......................... 86
5.2 IUPAC model parameters for the OH induced MACR degra-
dation experiments......................... 90
5.3 Changes in the MCM EASY model to represent the IUPAC
recommendation........................... 102
B.I Analyzed Standard Experiments ................. 127
B.2 Experiments concerning VOC — ozone.............. 128
|
| adam_txt |
Contents
Introduction 1
1.1 Ozone. 3
1.2 Ozone Precursor Species. 6
1.3 Isoprene. 8
1.4 Peroxyacyl Nitrates. 8
1.5 Chemical Weather Forecast . 9
1.6 Chamber Experiments. 10
1.7 Aim of this Thesis . 12
Theory 13
2.1 Gas Phase Chemistry. 13
2.1.1 Tropospheric Ozone Production. 14
2.1.2 Chemical Regimes . 19
2.2 Chemical Mechanisms . 20
2.3 Numerical Solving. 23
Experimentals 25
3.1 The SAPHIR Chamber. 25
3.1.1 Dilution. 28
3.1.2 HONO Source. 28
3.1.3 HCHO Source. 29
3.1.4 Background Reactivity. 36
3.1.5 Other Sources. 36
3.1.6 Deposition at the Walls . 37
3.2 Instrumentation. 37
3.2.1 Ozone Measurements. 39
3.2.2 Reactive Species . 39
3.2.3 Volatile Organic Compounds. 41
3.2.4 NOy Species. 42
3.2.5 Photolysis Frequencies. 43
3.2.6 Meteorological Conditions. 44
Ozone Production Due to Isoprene Degradation 47
4.1 Fully Time Dependent MCM Model Runs . 49
4.1.1 Results. 51
4.1.2 Discussion. 55
4.2 First Degradation Step Approach. 58
4.2.1 Used Method. 59
4.2.2 Results. 63
4.2.3 Discussion. 67
4.3 OH Lifetime. 69
4.3.1 Idea. 70
4.3.2 Used Method. "1
4.3.3 Results and Discussion. 74
4.4 Conclusion. 79
5 Methacrolein Degradation Studies 81
5.1 OH Induced MACR Degradation . 81
5.1.1 Used MCM Model . 82
5.1.2 Observations . 85
5.1.3 Results. 88
5.2 Photolysis and Ozonolysis of MACR . 92
5.2.1 Used Models . ". 92
5.2.2 Results. 93
5.3 NO3 Induced MACR Degradation. 95
5.3.1 Used Models. 97
5.3.2 Results. 98
5.4 Conclusion. 101
6 Resume and Outlook 103
A Used Gas Phase Chemistry Mechanisms 107
A.I Function Definitions .107
A.2 Default Settings and MCM Constants.108
A.3 Inorganic Section.109
A.4 MCM Isoprene Subset.110
A.4.1 Chamber-Features in the Isoprene MCM Model.122
B Tables of Analyzed Experiments 127
C Statistics 129
List of Figures
1.1 Picture of ozone injury of a Salix caprca leaf. -I
1.2 Graphic formulas of some biogenie VOCs. 7
1.3 Role of Chamber Experiments in Atmospheric Chemistry . 11
2.1 Ozone null cycle. 11
2.2 Ideal ozone production cycle. 18
2.3 Chain terminating reactions. 19
2.4 Ozone production isopleths plot. 21
3.1 Picture of the SAPHIR chamber. 25
3.2 Water dependence of the SAPHIR HCHO source . 31
3.3 Changes of the SAPHIR HCHO source over time . 34
3.4 Other sources of trace gases found during the standard experi-
ment at the 31st Aug 2006. 38
4.1 Ox fitting lines at GC sampling times. 49
4.2 Fully time dependent isoprene model run. 53
4.3 Correlations of the net Ox productions between measurements
and fully time dependent model runs. 54
4.4 Correlations for measured vs. modelled VOC concentrations for
Sep 2005 experiments. 5(i
4.5 Variation of amplifying factors over time. 60
4.6 "Decision tree" for the determination of amplifying factors . 62
4.7 Time series of fitted versus first-degradation-step approach de-
rived Ox production on 15th of May 2006. 65
4.8 Comparison of fitted and FDS calculated Ox production for ex-
periments between Sep 2005 and June 2006. 66
4.9 Methacrolein degradation induced by OH as proposed by the
MCM . 68
4.10 Time series of defining parameters for the integrated amplifying
factor . 73
4.11 Correlation between the net Ox production and the OH loss rate
for all experiments. 71
4.12 Averaged OH loss rate times amplifying factor over mean net
Ox production. 75
4.13 Roundoff errors occurring in Foh calculation. 76
4.14 Dependencies of the integrated amplifying factor Fqh. 77
5.1 NOX discrepancy at the OH induced MACR degradation . 83
5.2 Comparison of the NOX time series for different MCM model
parameters and the NOX measurements.84
5.3 Rate coefficients used by the MCM and recommended by IU-
PAC for the MACR + OH reaction.87
5.4 Reaction scheme recommended by IUPAC for the MACR + OH
reaction.89
5.5 'IUPAC model runs for the OH induced MACR degradation . . 91
5.6 PAN and MPAN measurements and model concentrations for
OH induced MACR degradation.92
5.7 Reaction scheme of the MACR photolysis 'IUPAC implemen-
tation.94
5.8 Reaction scheme of the MACR ozonolysis.95
5.9 MACR photolysis and ozonolysis experiment on 12th Apr 2007 . 96
5.10 NO3 induced MACR degradation scheme implemented in the
'IUPAC model.98
5.11 Nighttime MACR degradation experiments on 13th Nov 2006
and 13th Apr 2007.100
Vlll
List of Tables
1.1 Selected components of the earth's atmosphere. 2
1.2 Ozone threshold values for the European Union. 5
3.1 Technical specification of the SAPHIR chamber. 27
3.2 Fitting parameters of the HCHO source's water dependence . . 33
3.3 Overview of the instrumentation at SAPHIR. 15
4.1 Measurement vs. model correlation parameters of the net Ox
production. 52
4.2 Measurement vs. model correlation parameters for VOC mea-
surements . 57
5.1 MCM model parameters for the OH induced MACR degrada-
tion experiments . 86
5.2 'IUPAC model parameters for the OH induced MACR degra-
dation experiments. 90
5.3 Changes in the MCM EASY model to represent the IUPAC
recommendation. 102
B.I Analyzed "'Standard Experiments". 127
B.2 Experiments concerning VOC — ozone. 128 |
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| dewey-search | 551.511011 |
| dewey-sort | 3551.511011 |
| dewey-tens | 550 - Earth sciences |
| discipline | Geologie / Paläontologie |
| discipline_str_mv | Geologie / Paläontologie |
| format | Thesis Book |
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| index_date | 2024-07-02T21:59:13Z |
| indexdate | 2024-07-09T21:21:14Z |
| institution | BVB |
| isbn | 9783893365135 3893365133 |
| language | English |
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| physical | XIV, 147 S. Ill., graph. Darst. 24 cm |
| publishDate | 2008 |
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| record_format | marc |
| series2 | Schriften des Forschungszentrums Jülich : Reihe Energie & Umwelt |
| spelling | Richter, Cornelia Anna Verfasser aut Ozone production in the atmosphere simulation chamber SAPHIR Cornelia Anna Richter Jülich Forschungszentrum, Zentralbibliothek 2008 XIV, 147 S. Ill., graph. Darst. 24 cm txt rdacontent n rdamedia nc rdacarrier Schriften des Forschungszentrums Jülich : Reihe Energie & Umwelt 2 Zugl.: Köln, Univ., Diss., 2007 SAPHIR Simulationskammer (DE-588)4819070-6 gnd rswk-swf Simulation (DE-588)4055072-2 gnd rswk-swf Ozonisierungsreaktion (DE-588)4336828-1 gnd rswk-swf Troposphäre (DE-588)4061018-4 gnd rswk-swf (DE-588)4113937-9 Hochschulschrift gnd-content Troposphäre (DE-588)4061018-4 s Ozonisierungsreaktion (DE-588)4336828-1 s Simulation (DE-588)4055072-2 s SAPHIR Simulationskammer (DE-588)4819070-6 s DE-604 Forschungszentrum <Jülich> Schriften des Forschungszentrums Jülich Reihe Energie & Umwelt 2 (DE-604)BV023393979 2 HBZ Datenaustausch application/pdf http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=016726280&sequence=000002&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA Inhaltsverzeichnis |
| spellingShingle | Richter, Cornelia Anna Ozone production in the atmosphere simulation chamber SAPHIR SAPHIR Simulationskammer (DE-588)4819070-6 gnd Simulation (DE-588)4055072-2 gnd Ozonisierungsreaktion (DE-588)4336828-1 gnd Troposphäre (DE-588)4061018-4 gnd |
| subject_GND | (DE-588)4819070-6 (DE-588)4055072-2 (DE-588)4336828-1 (DE-588)4061018-4 (DE-588)4113937-9 |
| title | Ozone production in the atmosphere simulation chamber SAPHIR |
| title_auth | Ozone production in the atmosphere simulation chamber SAPHIR |
| title_exact_search | Ozone production in the atmosphere simulation chamber SAPHIR |
| title_exact_search_txtP | Ozone production in the atmosphere simulation chamber SAPHIR |
| title_full | Ozone production in the atmosphere simulation chamber SAPHIR Cornelia Anna Richter |
| title_fullStr | Ozone production in the atmosphere simulation chamber SAPHIR Cornelia Anna Richter |
| title_full_unstemmed | Ozone production in the atmosphere simulation chamber SAPHIR Cornelia Anna Richter |
| title_short | Ozone production in the atmosphere simulation chamber SAPHIR |
| title_sort | ozone production in the atmosphere simulation chamber saphir |
| topic | SAPHIR Simulationskammer (DE-588)4819070-6 gnd Simulation (DE-588)4055072-2 gnd Ozonisierungsreaktion (DE-588)4336828-1 gnd Troposphäre (DE-588)4061018-4 gnd |
| topic_facet | SAPHIR Simulationskammer Simulation Ozonisierungsreaktion Troposphäre Hochschulschrift |
| url | http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=016726280&sequence=000002&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA |
| volume_link | (DE-604)BV023393979 |
| work_keys_str_mv | AT richtercorneliaanna ozoneproductionintheatmospheresimulationchambersaphir |