1.西安交通大学动力工程多相流国家重点实验室, 710049,西安
2.中国联合重型燃气轮机技术有限公司, 100016,北京
刘昀洋(2000—),女,博士生;
殷阁媛(通信作者),女,副教授,博士生导师。
收稿:2024-07-01,
网络首发:2024-10-25,
纸质出版:2025-02-10
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刘昀洋, 赵韵, 尤佳俊, 等. 合成气/氮氧化物的氧化特性实验与反应动力学研究[J]. 西安交通大学学报, 2025,59(2):73-83.
LIU Yunyang, ZHAO Yun, YOU Jiajun, et al. Experimental and Kinetic Modeling on the Oxidation Characteristics of Syngas/Nitrogen Oxides[J]. Journal of Xi’an Jiaotong University, 2025, 59(2): 73-83.
刘昀洋, 赵韵, 尤佳俊, 等. 合成气/氮氧化物的氧化特性实验与反应动力学研究[J]. 西安交通大学学报, 2025,59(2):73-83. DOI: 10.7652/xjtuxb202502008.
LIU Yunyang, ZHAO Yun, YOU Jiajun, et al. Experimental and Kinetic Modeling on the Oxidation Characteristics of Syngas/Nitrogen Oxides[J]. Journal of Xi’an Jiaotong University, 2025, 59(2): 73-83. DOI: 10.7652/xjtuxb202502008.
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623~1 273 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(0,0.092 5%,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 coal-derived syngas doped with NO
x
at different pressures (0.19
1.80 MPa) and initial mole fractions of NO
x
(0
0.092 5%
0.185%) were measured and analyzed in a high-pressure flow reactor over a temperature range of 623 to 1 273 K. Simulations were conducted using six previously published kinetic models
and the CRECK-2019 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 low-temperature oxidation of syngas as NO
x
doping increased. NO
x
doping had no significant effect on the low-temperature oxidation of syngas at 0.19 MPa
whereas it promoted low-temperature oxidation at 1.80 MPa 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.
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