Hao Zhao , Chao Yan , Guohui Song , Ziyu Wang , Ahren W. Jasper , Stephen J. Klippenstein , Yiguang Ju
{"title":"High-pressure oxidation of hydrogen diluted in N2 with added H2O or CO2 at 100 atm in a supercritical-pressure jet-stirred reactor","authors":"Hao Zhao , Chao Yan , Guohui Song , Ziyu Wang , Ahren W. Jasper , Stephen J. Klippenstein , Yiguang Ju","doi":"10.1016/j.combustflame.2024.113543","DOIUrl":null,"url":null,"abstract":"<div><p>The oxidation of H<sub>2</sub> diluted in N<sub>2</sub> with and without 10 % H<sub>2</sub>O or 20 % CO<sub>2</sub> additions are studied at fuel-lean conditions at 100 atm and 500–1000 K in a supercritical-pressure jet-stirred reactor. The mole fractions of H<sub>2</sub> and O<sub>2</sub> are quantified by using micro-gas chromatography (µ-GC). Experiment shows that H<sub>2</sub> oxidation is inhibited at lower temperatures (850–950 K) while it is promoted at higher temperatures (950–1050 K) with 10 % H<sub>2</sub>O additions or 20 % CO<sub>2</sub> additions. In addition, the effect of H<sub>2</sub>O is more significant than that of CO<sub>2</sub>. Five models are employed in simulations of the observables. Unfortunately, all of these models fail to capture the effect of H<sub>2</sub>O and CO<sub>2</sub> additions on H<sub>2</sub> oxidation. Pathway and sensitivity analyses of H<sub>2</sub> show that the reactions of H + O<sub>2</sub> + (M) = HO<sub>2</sub> + (M) and H<sub>2</sub>O<sub>2</sub> + (M) = 2OH + (M) dominate the radical production (HO<sub>2</sub> and OH) and H<sub>2</sub> oxidation at 100 atm. A further perturbation of pre-exponential coefficients and collisional factors of these reactions indicates that collisional factors of H<sub>2</sub>O and CO<sub>2</sub> have small effect under the experimental conditions, while a smaller reaction rate for H<sub>2</sub>O<sub>2</sub> + (M) = 2OH + (M) may explain the inhibiting effect of H<sub>2</sub>O and CO<sub>2</sub> additions at lower temperatures. Real-fluid corrections on intermolecular interactions and mixing rules should be further investigated to explain the effect of H<sub>2</sub>O and CO<sub>2</sub> additions.</p></div>","PeriodicalId":280,"journal":{"name":"Combustion and Flame","volume":null,"pages":null},"PeriodicalIF":5.8000,"publicationDate":"2024-06-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Combustion and Flame","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0010218024002529","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}
引用次数: 0
Abstract
The oxidation of H2 diluted in N2 with and without 10 % H2O or 20 % CO2 additions are studied at fuel-lean conditions at 100 atm and 500–1000 K in a supercritical-pressure jet-stirred reactor. The mole fractions of H2 and O2 are quantified by using micro-gas chromatography (µ-GC). Experiment shows that H2 oxidation is inhibited at lower temperatures (850–950 K) while it is promoted at higher temperatures (950–1050 K) with 10 % H2O additions or 20 % CO2 additions. In addition, the effect of H2O is more significant than that of CO2. Five models are employed in simulations of the observables. Unfortunately, all of these models fail to capture the effect of H2O and CO2 additions on H2 oxidation. Pathway and sensitivity analyses of H2 show that the reactions of H + O2 + (M) = HO2 + (M) and H2O2 + (M) = 2OH + (M) dominate the radical production (HO2 and OH) and H2 oxidation at 100 atm. A further perturbation of pre-exponential coefficients and collisional factors of these reactions indicates that collisional factors of H2O and CO2 have small effect under the experimental conditions, while a smaller reaction rate for H2O2 + (M) = 2OH + (M) may explain the inhibiting effect of H2O and CO2 additions at lower temperatures. Real-fluid corrections on intermolecular interactions and mixing rules should be further investigated to explain the effect of H2O and CO2 additions.
期刊介绍:
The mission of the journal is to publish high quality work from experimental, theoretical, and computational investigations on the fundamentals of combustion phenomena and closely allied matters. While submissions in all pertinent areas are welcomed, past and recent focus of the journal has been on:
Development and validation of reaction kinetics, reduction of reaction mechanisms and modeling of combustion systems, including:
Conventional, alternative and surrogate fuels;
Pollutants;
Particulate and aerosol formation and abatement;
Heterogeneous processes.
Experimental, theoretical, and computational studies of laminar and turbulent combustion phenomena, including:
Premixed and non-premixed flames;
Ignition and extinction phenomena;
Flame propagation;
Flame structure;
Instabilities and swirl;
Flame spread;
Multi-phase reactants.
Advances in diagnostic and computational methods in combustion, including:
Measurement and simulation of scalar and vector properties;
Novel techniques;
State-of-the art applications.
Fundamental investigations of combustion technologies and systems, including:
Internal combustion engines;
Gas turbines;
Small- and large-scale stationary combustion and power generation;
Catalytic combustion;
Combustion synthesis;
Combustion under extreme conditions;
New concepts.