合成气/氮氧化物的氧化特性实验与反应动力学研究  

Experimental and Kinetic Modeling on the Oxidation Characteristics of Syngas/Nitrogen Oxides

作　　者：刘昀洋 赵韵 尤佳俊 殷阁媛 胡二江[1] 黄佐华[1] 包炀阳 LIU Yunyang;ZHAO Yun;YOU Jiajun;YIN Geyuan;HU Erjiang;HUANG Zuohua;BAO Yangyang(State Key Laboratory of Multiphase Flow in Power Engineering,Xi’an Jiaotong University,Xi’an 710049,China;China United Gas Turbine Technology Co.,Ltd.,Beijing 100016,China)

机构地区：[1]西安交通大学动力工程多相流国家重点实验室,西安710049 [2]中国联合重型燃气轮机技术有限公司,北京100016

出　　处：《西安交通大学学报》2025年第2期73-83,共11页Journal of Xi'an Jiaotong University

基　　金：国家科技重大专项资助项目(J2019-Ⅲ-0018-0062)。

摘　　要：为明晰合成气与氮氧化物(NO_(x))之间的相互作用机制,采用高压流动反应器,在623~1273 K温度下,实验分析了不同压力(0.19,1.80 MPa)、不同NO_(x)初始摩尔分数(0,0.0925%,0.185%)工况下,典型煤制合成气掺混NO_(x)的氧化特性。基于6种已有的反应动力学模型开展模拟计算,并结合实验结果和计算得到的反应速率常数,更新了CRECK-2019模型。采用更新后的模型进一步开展反应动力学分析,揭示了合成气/NO_(x)氧化过程的关键反应。研究结果表明:升高压力对合成气的低温氧化存在促进作用,且促进作用随NO_(x)掺混量的增大而增强;掺混NO_(x)对0.19 MPa下合成气的低温氧化无明显影响,而对1.80 MPa下的低温氧化存在促进作用,且对不同压力下的中、高温氧化均存在抑制作用;反应H_(2)+NO_(2)=H+HONO对高压下合成气/NO_(x)的氧化有显著贡献,反应HNO+NO_(2)=HONO+NO、HNO+H=NO+H_(2)和HNO+OH=NO+H_(2)O严重影响着中高温下OH的生成。研究结果可为合成气燃气轮机开发与污染物排放控制提供理论支撑。To clarify the interaction mechanism between syngas and nitrogen oxides(NO_(x)),the oxidation characteristics of typical coalderived syngas doped with NO_(x)at different pressures(0.19,1.80MPa)and initial mole fractions of NO_(x)(0,0.0925%,0.185%)were measured and analyzed in a highpressure flow reactor over a temperature range of 623 to 1273K.Simulations were conducted using six previously published kinetic models,and the CRECK2019 model was updated based on experimental results and the latest calculated reaction rate constants.This updated model was used for a detailed kinetic analysis,revealing key reactions in the oxidation process of syngas/NO_(x).The experimental results show that increased pressure enhanced the lowtemperature oxidation of syngas as NO_(x)doping increased.NO_(x)doping had no significant effect on the lowtemperature oxidation of syngas at 0.19MPa,whereas it promoted low-temperature oxidation at 1.80MPa and inhibited oxidation at medium and high temperatures across different pressures.The reaction H_(2)+NO_(2)=H+HONO contributed significantly to the oxidation of syngas/NO_(x)at high pressure.Additionally,the reactions HNO+NO_(2)=HONO+NO,HNO+H=NO+H_(2),and HNO+OH=NO+H_(2)O strongly influenced the generation of OH at medium and high temperatures.This study can provide a theoretical foundation for the design and pollutant emission control of syngas turbine.

关 键 词：合成气 氮氧化物 高压流动反应器 氧化特性 反应动力学模型 

分 类 号：TK407.9[动力工程及工程热物理—动力机械及工程]