Adsorption and catalytic oxidation of residual NH3 on coal ash after selective non-catalytic reduction in coal-fired boilers

被引:7
作者
Zheng, Jingfan [1 ]
Wang, Jing [1 ]
Yang, Fengling [1 ]
Du, Zhiping [1 ]
Cheng, Fangqin [1 ]
机构
[1] Shanxi Univ, Inst Resources & Environm Engn, State Environm Protect Key Lab Efficient Utilizat, Taiyuan 030006, Peoples R China
基金
中国国家自然科学基金;
关键词
SNCR; Coal ash; NH3; oxidation; Adsorption; Catalytic oxidation; IN-SITU; WASTE INCINERATION; NOX; OXIDE; PERFORMANCE; COMBUSTION; SURFACE; CAO;
D O I
10.1016/j.chemosphere.2023.137765
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Selective non-catalytic reduction (SNCR) with NH3 as the reducing agent is widely used for the denitrification of flue gas in coal-fired boilers, where fly ash significantly influences the conversion of the residual NH3 that does not participate in denitrification. However, there have been few studies on the exact nature of this influence, particularly the adsorption and reaction mechanisms of NH3 on fly ash. In this study, temperature-programmed desorption (TPD) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) were used to study the mechanisms of NH3 adsorption and reactions over coal ash. In the absence of oxygen, in the temperature range of 50-450 degrees C, NH3 was adsorbed on the surface of the coal ash. The adsorption capacity of lignite ash was higher than that of anthracite ash. This difference was attributed to the large specific surface area and surface acidity of the lignite ash. However, between 450-850 degrees C, coal ash had a catalytic effect on NH3 decomposition and oxidation. Due to the high surface lattice oxygen content of lignite ash, its catalytic oxidative ability was superior to anthracite ash. Moreover, NH3 was first adsorbed over Lewis and Bronsted acid sites on the surface of coal ash and later underwent hydrogen abstraction to produce either the NH2 or the NH intermediate. The intermediates further reacted with the surface lattice oxygen of coal ash to produce NO and N2O. These results might be helpful for the management of NH3 residues from SNCR processes and the utilization of amino reducing agents in coal-fired boilers.
引用
收藏
页数:9
相关论文
共 38 条
[1]  
[Anonymous], 2005, ANN BOOK ASTM STAND, DOI [10.1520/C0618-05,04.02, DOI 10.1520/C0618-05,04.02]
[2]   The influence of carbon particle type in fly ashes on mercury adsorption [J].
Antonia Lopez-Anton, M. ;
Abad-Valle, Patricia ;
Diaz-Somoano, Mercedes ;
Suarez-Ruiz, Isabel ;
Rosa Martinez-Tarazona, M. .
FUEL, 2009, 88 (07) :1194-1200
[3]   Comparison of the performance for oxidation of formaldehyde on nano-Co3O4, 2D-Co3O4, and 3D-Co3O4 catalysts [J].
Bai, Bingyang ;
Arandiyan, Hamidreza ;
Li, Junhua .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2013, 142 :677-683
[4]   Synthesis and characterisation of La1-xCaxFeO3 perovskite-type oxide catalysts for total oxidation of volatile organic compounds [J].
Barbero, Bibiana P. ;
Gamboa, Julio Andrade ;
Cadus, Luis E. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2006, 65 (1-2) :21-30
[5]   In-situ DRIFTS investigation on the selective catalytic reduction of NO with NH3 over the sintered ore catalyst [J].
Chen, Wangsheng ;
Li, Ze ;
Hu, Fali ;
Qin, Linbo ;
Han, Jun ;
Wu, Gaoming .
APPLIED SURFACE SCIENCE, 2018, 439 :75-81
[6]   NOx control in coal combustion by combining biomass co-firing, oxygen enrichment and SNCR [J].
Daood, S. S. ;
Javed, M. T. ;
Gibbs, B. M. ;
Nimmo, W. .
FUEL, 2013, 105 :283-292
[7]   Selective non-catalytic reduction - Fe-based additive hybrid technology [J].
Daood, Syed Sheraz ;
Yelland, Thomas S. ;
Nimmo, William .
FUEL, 2017, 208 :353-362
[8]   Mechanism study on the adsorption and reactions of NH3, NO, and O2 on the CaO surface in the SNCR deNOx process [J].
Fu, Shi-long ;
Song, Qiang ;
Yao, Qiang .
CHEMICAL ENGINEERING JOURNAL, 2016, 285 :137-143
[9]   Effect of CaO on the selective non-catalytic reduction deNOx process: Experimental and kinetic study [J].
Fu, Shi-long ;
Song, Qiang ;
Tang, Jun-shi ;
Yao, Qiang .
CHEMICAL ENGINEERING JOURNAL, 2014, 249 :252-259
[10]   Experimental and Kinetic Study on the Influence of Iron Oxide on the Selective Noncatalytic Reduction DeNOx Process [J].
Fu, Shi-Long ;
Song, Qiang ;
Yao, Qiang .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2014, 53 (14) :5801-5809