Oxidative removal of NO in DTPMPA/Fenton system

doi:10.16085/j.issn.1000-6613.2022-1970

Abstract

Abstract:

In view of the current Fenton oxidation method to remove NO in coal-fired flue gas, a large amount of H₂O₂ ineffectively decomposes to generate oxygen, the DTPMPA (diethylenetriamine pentamethylphosphonic acid) /Fenton system was used to oxidize and remove NO. The results showed that when NO removal efficiency of the system was 95.1%, the proportion of H₂O₂ ineffective decomposition decreased to 15.5%. The increase of DTPMPA concentration inhibited H₂O₂ineffective decomposition, and it promoted NO removal when the concentration was low but inhibited NO removal when the concentration was high. The increase of H₂O₂ and Fe²⁺ concentrations had a certain promoting effect on NO removal and H₂O₂ ineffective decomposition, but when the concentration of both was too high, it also had a certain inhibitory effect on NO removal. Lower reaction temperature had little effect on NO removal, but weakened H₂O₂ ineffective decomposition. SO₂ had little effect on NO removal and H₂O₂ ineffective decomposition. Electron spin resonance technology and quenching addition experiments showed that the addition of DTPMPA increased the content of ·OH radicals and ·O₂^- radicals in the Fenton system, ·O $2 -$ radicals were the main active species for NO removal, and the main pathway of oxygen generation was ·O $2 -$ + HO· $→$ O₂ + HO^-. Ion chromatography of the reaction products showed that NO was oxidized to NO $2 -$ and NO $3 -$ during the reaction.

Key words: Fenton, diethylenetriamine pentamethylphosphonic acid, radical, denitration, ineffective decomposition

摘要：

针对当前Fenton氧化法脱除燃煤烟气中 NO的过程中H₂O₂大量无效分解生成氧气的缺点，本文采用二乙烯三胺五亚甲基膦酸（DTPMPA）/Fenton系统进行氧化脱除NO的实验研究。结果表明：该系统在NO脱除效率为95.1%的情况下，H₂O₂无效分解占比降低至15.5%。DTPMPA浓度的增加抑制了H₂O₂无效分解，其浓度较低时促进NO脱除而浓度较高时抑制NO脱除；H₂O₂及Fe²⁺浓度的增加均对NO脱除及H₂O₂无效分解有一定的促进作用，但二者浓度过高时亦均对脱除NO有一定抑制作用；降低反应温度对NO脱除影响较小，但会削弱H₂O₂无效分解；SO₂对NO的脱除及H₂O₂无效分解影响甚小。电子自旋共振技术和淬灭剂添加实验结果表明：DTPMPA的添加提高了Fenton系统中·OH自由基和·O $2 -$ 自由基的含量，且·O $2 -$ 自由基为脱除NO的主要活性物质，·O $2 -$ + HO· $→$ O₂ + HO^-为氧气生成的主要途径。反应产物离子色谱表明：NO在反应过程中被氧化为NO $2 -$ 和NO $3 -$ 。

关键词: 芬顿法, 二乙烯三胺五亚甲基膦酸, 自由基, 脱硝, 无效分解

CLC Number:

X701

BAI Zhihua, ZHANG Jun. Oxidative removal of NO in DTPMPA/Fenton system[J]. Chemical Industry and Engineering Progress, 2023, 42(9): 4967-4973.

白志华, 张军. 二乙烯三胺五亚甲基膦酸/Fenton体系氧化脱除NO[J]. 化工进展, 2023, 42(9): 4967-4973.

Figures/Tables 12

序号	峰名称	样品量/mg·L^-1
1	NO $2 -$	1.1351
2	NO $3 -$	4.7087

序号	峰名称	样品量/mg·L^-1
1	NO $2 -$	1.1351
2	NO $3 -$	4.7087

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