Potential Risk of NH<sub>3</sub> Slip Arisen from Catalytic Inactive Site in Selective Catalytic Reduction of NO<sub><i>x</i></sub> with Metal-Free Carbon Catalysts

催化作用 吸附 选择性催化还原 化学 氮氧化物 打滑(空气动力学) 烟气 金属 无机化学 有机化学 热力学 燃烧 物理
作者
Jin Yuan,Zhen Wang,Jun Liu,Junhua Li,Jianjun Chen
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:57 (1): 606-614 被引量:1
标识
DOI:10.1021/acs.est.2c06289
摘要

Ammonia emissions from industrial processes have rapidly increased in the past years. Recent advances have used carbon-based selective catalytic reduction (SCR) technology combined with a reaction-regeneration process to reduce NOx from sintering flue gas, while NH3 slip is seldom accounted for in this process. This study demonstrates that although the electrophilic carboxyl groups (-COOH) on metal-free carbon catalysts exhibit strong adsorption toward NH3, they do not participate in the SCR reaction. As a result of the competitive adsorption of NH3 in the reaction step, these catalytic inactive carboxyl groups not only prolong the time to the SCR steady state, but also result in the potential risk of NH3 slip. A linear relationship with the equimolar ratio between carboxyl groups and slipped NH3 was established in the regeneration steps. The slip of NH3 could be alleviated by the decomposition of carboxyl groups, and special attention should be paid to the presence of inactive sites with strong NH3 adsorption on industrial-employed carbon catalysts. In addition to advancing the understanding of the NH3-SCR mechanism, this work also provides valuable opportunities for the control of ammonia emissions from industrial processes.
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