Comprehensive reevaluation of acetaldehyde chemistry - part I: Assessment of important kinetic parameters and the underlying uncertainties
Understanding the combustion chemistry of acetaldehyde is crucial to developing robust and accurate combustion chemistry models for practical fuels, especially for biofuels. This study aims to re-evaluate the important rate and thermodynamic parameters for acetaldehyde combustion chemistry and deter...
Saved in:
| Main Authors: | , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Elsevier
2025-03-01
|
| Series: | Applications in Energy and Combustion Science |
| Subjects: | |
| Online Access: | http://www.sciencedirect.com/science/article/pii/S2666352X25000020 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1849773236720500736 |
|---|---|
| author | Xinrui Ren Hongqing Wu Ruoyue Tang Yanqing Cui Mingrui Wang Song Cheng |
| author_facet | Xinrui Ren Hongqing Wu Ruoyue Tang Yanqing Cui Mingrui Wang Song Cheng |
| author_sort | Xinrui Ren |
| collection | DOAJ |
| description | Understanding the combustion chemistry of acetaldehyde is crucial to developing robust and accurate combustion chemistry models for practical fuels, especially for biofuels. This study aims to re-evaluate the important rate and thermodynamic parameters for acetaldehyde combustion chemistry and determine the physical uncertainties of these parameters. The rate parameters of 79 key reactions are reevaluated using > 100,000 direct experiments and quantum chemistry computations from > 900 studies, and the thermochemistry (Δhf(298 K), s0(298 K) and cp) of 24 key species are reevaluated based on the ATCT database, the NIST Chemistry WebBook, the TMTD database, and 35 published chemistry models. The updated parameters are incorporated into a recent acetaldehyde chemistry model, which is further assessed against available fundamental experiments measurements (10 RCM-IDT, 123 ST-IDT, 633 JSR-species concentrations, and 102 flow reactor-species concentrations) and existing chemistry models, with clearly better performance obtained in the high-temperature regime. Sensitivity and flux analyses further highlight the insufficiencies of previous models in representing the key pathways, particularly the branching ratios of acetaldehyde- and formaldehyde-consuming pathways. Meanwhile, temperature-dependent and temperature-independent uncertainties are statistically evaluated for kinetic and thermochemical parameters, respectively, where the large differences between the updated and the original model parameters reveal the necessity of reassessment of kinetic and thermochemical parameters completely based on direct experiments and theoretical calculations for rate and thermodynamic parameters. The application of the determined uncertainty domains of the key kinetic and thermodynamic parameters is further demonstrated through a case study, with the modelling uncertainty and its reliability highlighted. With the configured uncertainty domain of the updated acetaldehyde chemistry model, further uncertainty quantification and optimization can be conducted to improve the model performance, which is currently under progress in the authors’ group. |
| format | Article |
| id | doaj-art-e964f1b066be429b86d058023e514c1d |
| institution | DOAJ |
| issn | 2666-352X |
| language | English |
| publishDate | 2025-03-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Applications in Energy and Combustion Science |
| spelling | doaj-art-e964f1b066be429b86d058023e514c1d2025-08-20T03:02:06ZengElsevierApplications in Energy and Combustion Science2666-352X2025-03-012110032010.1016/j.jaecs.2025.100320Comprehensive reevaluation of acetaldehyde chemistry - part I: Assessment of important kinetic parameters and the underlying uncertaintiesXinrui Ren0Hongqing Wu1Ruoyue Tang2Yanqing Cui3Mingrui Wang4Song Cheng5Department of Mechanical Engineering, The Hong Kong Polytechnic University, Kowloon 999077, Hong KongDepartment of Mechanical Engineering, The Hong Kong Polytechnic University, Kowloon 999077, Hong KongDepartment of Mechanical Engineering, The Hong Kong Polytechnic University, Kowloon 999077, Hong KongDepartment of Mechanical Engineering, The Hong Kong Polytechnic University, Kowloon 999077, Hong KongDepartment of Mechanical Engineering, The Hong Kong Polytechnic University, Kowloon 999077, Hong KongDepartment of Mechanical Engineering, The Hong Kong Polytechnic University, Kowloon 999077, Hong Kong; Research Institute for Smart Energy, The Hong Kong Polytechnic University, Kowloon 999077, Hong Kong; Corresponding authors at: Department of Mechanical Engineering, The Hong Kong Polytechnic University, Kowloon 999077, Hong Kong.Understanding the combustion chemistry of acetaldehyde is crucial to developing robust and accurate combustion chemistry models for practical fuels, especially for biofuels. This study aims to re-evaluate the important rate and thermodynamic parameters for acetaldehyde combustion chemistry and determine the physical uncertainties of these parameters. The rate parameters of 79 key reactions are reevaluated using > 100,000 direct experiments and quantum chemistry computations from > 900 studies, and the thermochemistry (Δhf(298 K), s0(298 K) and cp) of 24 key species are reevaluated based on the ATCT database, the NIST Chemistry WebBook, the TMTD database, and 35 published chemistry models. The updated parameters are incorporated into a recent acetaldehyde chemistry model, which is further assessed against available fundamental experiments measurements (10 RCM-IDT, 123 ST-IDT, 633 JSR-species concentrations, and 102 flow reactor-species concentrations) and existing chemistry models, with clearly better performance obtained in the high-temperature regime. Sensitivity and flux analyses further highlight the insufficiencies of previous models in representing the key pathways, particularly the branching ratios of acetaldehyde- and formaldehyde-consuming pathways. Meanwhile, temperature-dependent and temperature-independent uncertainties are statistically evaluated for kinetic and thermochemical parameters, respectively, where the large differences between the updated and the original model parameters reveal the necessity of reassessment of kinetic and thermochemical parameters completely based on direct experiments and theoretical calculations for rate and thermodynamic parameters. The application of the determined uncertainty domains of the key kinetic and thermodynamic parameters is further demonstrated through a case study, with the modelling uncertainty and its reliability highlighted. With the configured uncertainty domain of the updated acetaldehyde chemistry model, further uncertainty quantification and optimization can be conducted to improve the model performance, which is currently under progress in the authors’ group.http://www.sciencedirect.com/science/article/pii/S2666352X25000020Acetaldehyde chemistryPhysics-based model reevaluationModel validation and comparisonUncertainty analysis |
| spellingShingle | Xinrui Ren Hongqing Wu Ruoyue Tang Yanqing Cui Mingrui Wang Song Cheng Comprehensive reevaluation of acetaldehyde chemistry - part I: Assessment of important kinetic parameters and the underlying uncertainties Applications in Energy and Combustion Science Acetaldehyde chemistry Physics-based model reevaluation Model validation and comparison Uncertainty analysis |
| title | Comprehensive reevaluation of acetaldehyde chemistry - part I: Assessment of important kinetic parameters and the underlying uncertainties |
| title_full | Comprehensive reevaluation of acetaldehyde chemistry - part I: Assessment of important kinetic parameters and the underlying uncertainties |
| title_fullStr | Comprehensive reevaluation of acetaldehyde chemistry - part I: Assessment of important kinetic parameters and the underlying uncertainties |
| title_full_unstemmed | Comprehensive reevaluation of acetaldehyde chemistry - part I: Assessment of important kinetic parameters and the underlying uncertainties |
| title_short | Comprehensive reevaluation of acetaldehyde chemistry - part I: Assessment of important kinetic parameters and the underlying uncertainties |
| title_sort | comprehensive reevaluation of acetaldehyde chemistry part i assessment of important kinetic parameters and the underlying uncertainties |
| topic | Acetaldehyde chemistry Physics-based model reevaluation Model validation and comparison Uncertainty analysis |
| url | http://www.sciencedirect.com/science/article/pii/S2666352X25000020 |
| work_keys_str_mv | AT xinruiren comprehensivereevaluationofacetaldehydechemistrypartiassessmentofimportantkineticparametersandtheunderlyinguncertainties AT hongqingwu comprehensivereevaluationofacetaldehydechemistrypartiassessmentofimportantkineticparametersandtheunderlyinguncertainties AT ruoyuetang comprehensivereevaluationofacetaldehydechemistrypartiassessmentofimportantkineticparametersandtheunderlyinguncertainties AT yanqingcui comprehensivereevaluationofacetaldehydechemistrypartiassessmentofimportantkineticparametersandtheunderlyinguncertainties AT mingruiwang comprehensivereevaluationofacetaldehydechemistrypartiassessmentofimportantkineticparametersandtheunderlyinguncertainties AT songcheng comprehensivereevaluationofacetaldehydechemistrypartiassessmentofimportantkineticparametersandtheunderlyinguncertainties |