H2 + N2O反应的理论分析

IF 5.8 2区工程技术 Q2 ENERGY & FUELS

Combustion and Flame Pub Date : 2025-07-04 DOI:10.1016/j.combustflame.2025.114330

Clayton R. Mulvihill

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引用次数: 0

摘要

H2和N2O直接生成H2O和N2的反应一直是一个有争议的问题，报道的速率常数在1500 K时跨越了近五个数量级。本研究首次对标题反应进行了理论分析。通过耦合ANL1-QZF势能面和主方程处理，在400 ~ 3000 K范围内确定了与压力无关的热速率常数k1。最合适的k1以cm3·mol-1·s-1表示，k1=5.23×104T2.272exp (- 21745/T)， T以k表示。这个速率常数比最近动力学机制中使用的值小几个数量级。

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A theoretical analysis of the reaction H2 + N2O ⇆ H2O + N2

The reaction of H₂ and N₂O to directly form H₂O and N₂ has been a matter of some controversy, with reported rate constants spanning nearly five orders of magnitude at 1500 K. This study presents the first theoretical analysis of the title reaction. By coupling an ANL1-QZF potential energy surface with a master equation treatment, the pressure-independent thermal rate constant

k_{1}

was determined between 400 and 3000 K. The best-fit

k_{1}

is given in cm³·mol^–1·s^–1 as

k_{1} = 5.23 \times 10^{4} T^{2.272} exp (- 21745 / T)

, with

T

in K. This rate constant is several orders of magnitude smaller than values utilized in recent kinetics mechanisms.

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来源期刊

Combustion and Flame 工程技术-工程：化工

CiteScore

9.50

自引率

20.50%

发文量

631

审稿时长

3.8 months

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.