{"title":"Rush-to-equilibrium concept for minimizing reactive nitrogen emissions in ammonia combustion","authors":"Hernando Maldonado Colmán, Michael E. Mueller","doi":"10.1016/j.combustflame.2025.114049","DOIUrl":null,"url":null,"abstract":"<div><div>Ammonia is a zero-carbon fuel that has been receiving increasing attention for power generation and even transportation. Compared to hydrogen, ammonia’s volumetric energy density is higher, is not as explosive, and has well established transport and storage technologies. However, ammonia has poor flammability and flame stability characteristics and more reactive nitrogen emissions (nitrogen oxides, nitrous oxide) than hydrocarbon fuels, at least with traditional combustion processes. Partially cracking ammonia addresses its flammability and stability issues, through on-board catalysts or autothermal crackers, into a mixture of ammonia, hydrogen, and nitrogen. However, reactive nitrogen emissions remain a challenge, and mechanisms of their emissions are fundamentally different in ammonia and hydrocarbon combustion. While rich-quench-lean ammonia combustion strategies have shown promise, the largest contributions to reactive nitrogen emissions are the unrelaxed emissions in the fuel-rich first stage due to overshoot of thermodynamic equilibrium within the reaction zone of premixed flames coupled with finite residence times available for relaxation to equilibrium. This work introduces a rush-to-equilibrium concept for partially cracked ammonia combustion, which aims to reduce the unrelaxed reactive nitrogen emissions in finite residence times by accelerating the approach to equilibrium. In the concept, a flow particle is subjected to a decaying mixing rate as it transits the premixed flame. This plays an important role in mitigating the mixing effects that prevents the flow particle approach to equilibrium, and promoting the chemistry effects to push the particle toward equilibrium, all while considering residence times typical of gas turbines for power generation. Evaluated with a state-of-the-art combustion model at gas turbine conditions, the concept shows the potential for a reduction in reactive nitrogen emissions by an order of magnitude at even modest mixing rate decay rates. It is also shown that the concept works irrespective of cracking extent, pressure, temperature, etc. A brief discussion of practical feasibility reveals reasonable geometric and flow parameters characteristic of modern gas turbine combustors for power generation.</div><div><strong>Novelty and Significance Statement</strong></div><div>A novel rush-to-equilibrium combustion concept is proposed with the aim of reducing reactive nitrogen emissions, which include nitrogen oxides and nitrous oxide, from partially cracked ammonia combustion at gas turbine conditions. Reactive nitrogen emissions are elevated in partially cracked ammonia combustion systems because insufficient residence time is available to reach thermodynamic equilibrium. A concept is proposed to address this issue, leveraging decaying mixing rates, without modifying typical gas turbine for power generation residence times by accelerating the approach to thermodynamic equilibrium. The new concept is demonstrated of being capable of significantly reducing reactive nitrogen emissions (by a factor of an order of magnitude). Finally, implementation of the new concept is showed to be practically feasible.</div></div>","PeriodicalId":280,"journal":{"name":"Combustion and Flame","volume":"275 ","pages":"Article 114049"},"PeriodicalIF":5.8000,"publicationDate":"2025-02-19","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/S0010218025000872","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
Ammonia is a zero-carbon fuel that has been receiving increasing attention for power generation and even transportation. Compared to hydrogen, ammonia’s volumetric energy density is higher, is not as explosive, and has well established transport and storage technologies. However, ammonia has poor flammability and flame stability characteristics and more reactive nitrogen emissions (nitrogen oxides, nitrous oxide) than hydrocarbon fuels, at least with traditional combustion processes. Partially cracking ammonia addresses its flammability and stability issues, through on-board catalysts or autothermal crackers, into a mixture of ammonia, hydrogen, and nitrogen. However, reactive nitrogen emissions remain a challenge, and mechanisms of their emissions are fundamentally different in ammonia and hydrocarbon combustion. While rich-quench-lean ammonia combustion strategies have shown promise, the largest contributions to reactive nitrogen emissions are the unrelaxed emissions in the fuel-rich first stage due to overshoot of thermodynamic equilibrium within the reaction zone of premixed flames coupled with finite residence times available for relaxation to equilibrium. This work introduces a rush-to-equilibrium concept for partially cracked ammonia combustion, which aims to reduce the unrelaxed reactive nitrogen emissions in finite residence times by accelerating the approach to equilibrium. In the concept, a flow particle is subjected to a decaying mixing rate as it transits the premixed flame. This plays an important role in mitigating the mixing effects that prevents the flow particle approach to equilibrium, and promoting the chemistry effects to push the particle toward equilibrium, all while considering residence times typical of gas turbines for power generation. Evaluated with a state-of-the-art combustion model at gas turbine conditions, the concept shows the potential for a reduction in reactive nitrogen emissions by an order of magnitude at even modest mixing rate decay rates. It is also shown that the concept works irrespective of cracking extent, pressure, temperature, etc. A brief discussion of practical feasibility reveals reasonable geometric and flow parameters characteristic of modern gas turbine combustors for power generation.
Novelty and Significance Statement
A novel rush-to-equilibrium combustion concept is proposed with the aim of reducing reactive nitrogen emissions, which include nitrogen oxides and nitrous oxide, from partially cracked ammonia combustion at gas turbine conditions. Reactive nitrogen emissions are elevated in partially cracked ammonia combustion systems because insufficient residence time is available to reach thermodynamic equilibrium. A concept is proposed to address this issue, leveraging decaying mixing rates, without modifying typical gas turbine for power generation residence times by accelerating the approach to thermodynamic equilibrium. The new concept is demonstrated of being capable of significantly reducing reactive nitrogen emissions (by a factor of an order of magnitude). Finally, implementation of the new concept is showed to be practically feasible.
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.