Long Qin, Qiang Cheng, John Mantzaras, Chung K. Law, Ran Sui
{"title":"催化微通道中氢/空气燃烧的表面-气体化学耦合和稳定性极限","authors":"Long Qin, Qiang Cheng, John Mantzaras, Chung K. Law, Ran Sui","doi":"10.1016/j.proci.2024.105229","DOIUrl":null,"url":null,"abstract":"The catalytic (heterogeneous) and coupled catalytic-gaseous (hetero-/homogeneous) combustion of fuel-lean hydrogen/air mixtures (equivalence ratio = 0.4) in palladium- and rhodium-coated catalytic microchannels was numerically investigated in planar microchannels having a canonical geometry of 10 mm length and 1 mm height. Steady, extinction-induced combustion stability limits were demarcated as a function of inlet velocity and external heat loss at pressures of 1 and 5 bar, with wall thermal conductivities of 1 and 16 W/mK. In each case, interplays between the catalytic and gas-phase chemical reaction pathways, and their impact on the stability limits were identified. The stability results were further compared with literature data for platinum. The simulations indicated that Pd was more resilient against extinction than Rh and had a stronger surface reactivity when competing with gas-phase chemistry in the channel. Similar to Pt, the strong H surface reactivity on Pd resulted in wide stability limits purely determined by surface reactions and independent of gas-phase chemistry. In stark contrast, the presence of gas-phase combustion significantly expanded the stability limits of the Rh channel. The stability limits of Rh at 5 bar were consistently broader than those at 1 bar under all investigated conditions, which was also a behavior different to that of Pd and Pt channels, whose stability limit curves had crossover points between the two pressures. Additional simulations were performed in a Surface Perfectly Stirred Reactor (SPSR), providing comprehensive chemistry information, including sensitivity analyses of key reactions and surface coverages. When approaching extinction, OH(s) was a major surface species on Pd, while the Rh surface was primarily blocked by O(s).","PeriodicalId":408,"journal":{"name":"Proceedings of the Combustion Institute","volume":null,"pages":null},"PeriodicalIF":5.3000,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Surface-gas chemistry coupling and stability limits of hydrogen/air combustion in catalytic microchannels\",\"authors\":\"Long Qin, Qiang Cheng, John Mantzaras, Chung K. Law, Ran Sui\",\"doi\":\"10.1016/j.proci.2024.105229\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The catalytic (heterogeneous) and coupled catalytic-gaseous (hetero-/homogeneous) combustion of fuel-lean hydrogen/air mixtures (equivalence ratio = 0.4) in palladium- and rhodium-coated catalytic microchannels was numerically investigated in planar microchannels having a canonical geometry of 10 mm length and 1 mm height. Steady, extinction-induced combustion stability limits were demarcated as a function of inlet velocity and external heat loss at pressures of 1 and 5 bar, with wall thermal conductivities of 1 and 16 W/mK. In each case, interplays between the catalytic and gas-phase chemical reaction pathways, and their impact on the stability limits were identified. The stability results were further compared with literature data for platinum. The simulations indicated that Pd was more resilient against extinction than Rh and had a stronger surface reactivity when competing with gas-phase chemistry in the channel. Similar to Pt, the strong H surface reactivity on Pd resulted in wide stability limits purely determined by surface reactions and independent of gas-phase chemistry. In stark contrast, the presence of gas-phase combustion significantly expanded the stability limits of the Rh channel. The stability limits of Rh at 5 bar were consistently broader than those at 1 bar under all investigated conditions, which was also a behavior different to that of Pd and Pt channels, whose stability limit curves had crossover points between the two pressures. Additional simulations were performed in a Surface Perfectly Stirred Reactor (SPSR), providing comprehensive chemistry information, including sensitivity analyses of key reactions and surface coverages. When approaching extinction, OH(s) was a major surface species on Pd, while the Rh surface was primarily blocked by O(s).\",\"PeriodicalId\":408,\"journal\":{\"name\":\"Proceedings of the Combustion Institute\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.3000,\"publicationDate\":\"2024-06-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Proceedings of the Combustion Institute\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.proci.2024.105229\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Proceedings of the Combustion Institute","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.proci.2024.105229","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
Surface-gas chemistry coupling and stability limits of hydrogen/air combustion in catalytic microchannels
The catalytic (heterogeneous) and coupled catalytic-gaseous (hetero-/homogeneous) combustion of fuel-lean hydrogen/air mixtures (equivalence ratio = 0.4) in palladium- and rhodium-coated catalytic microchannels was numerically investigated in planar microchannels having a canonical geometry of 10 mm length and 1 mm height. Steady, extinction-induced combustion stability limits were demarcated as a function of inlet velocity and external heat loss at pressures of 1 and 5 bar, with wall thermal conductivities of 1 and 16 W/mK. In each case, interplays between the catalytic and gas-phase chemical reaction pathways, and their impact on the stability limits were identified. The stability results were further compared with literature data for platinum. The simulations indicated that Pd was more resilient against extinction than Rh and had a stronger surface reactivity when competing with gas-phase chemistry in the channel. Similar to Pt, the strong H surface reactivity on Pd resulted in wide stability limits purely determined by surface reactions and independent of gas-phase chemistry. In stark contrast, the presence of gas-phase combustion significantly expanded the stability limits of the Rh channel. The stability limits of Rh at 5 bar were consistently broader than those at 1 bar under all investigated conditions, which was also a behavior different to that of Pd and Pt channels, whose stability limit curves had crossover points between the two pressures. Additional simulations were performed in a Surface Perfectly Stirred Reactor (SPSR), providing comprehensive chemistry information, including sensitivity analyses of key reactions and surface coverages. When approaching extinction, OH(s) was a major surface species on Pd, while the Rh surface was primarily blocked by O(s).
期刊介绍:
The Proceedings of the Combustion Institute contains forefront contributions in fundamentals and applications of combustion science. For more than 50 years, the Combustion Institute has served as the peak international society for dissemination of scientific and technical research in the combustion field. In addition to author submissions, the Proceedings of the Combustion Institute includes the Institute''s prestigious invited strategic and topical reviews that represent indispensable resources for emergent research in the field. All papers are subjected to rigorous peer review.
Research papers and invited topical reviews; Reaction Kinetics; Soot, PAH, and other large molecules; Diagnostics; Laminar Flames; Turbulent Flames; Heterogeneous Combustion; Spray and Droplet Combustion; Detonations, Explosions & Supersonic Combustion; Fire Research; Stationary Combustion Systems; IC Engine and Gas Turbine Combustion; New Technology Concepts
The electronic version of Proceedings of the Combustion Institute contains supplemental material such as reaction mechanisms, illustrating movies, and other data.