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东南大学能源与环境学院,能源热转换及其过程测控教育部重点实验室,江苏 南京 210096
Received:01 April 2019,
Revised:2019-06-20,
Online First:24 July 2026,
Published:05 August 2019
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陈潇雪, 宋敏, 孟凡跃, 卫月星. FexMnCe1-AC低温SCR催化剂SO2中毒机理研究[J]. 化工学报, 2019, 70(8): 3000-3010 DOI: 10.11949/0438-1157.20190318.
CHEN Xiaoxue, SONG Min, MENG Fanyue, WEI Yuexing. Mechanism study on SO2 poisoning of FexMnCe1-AC catalyst for low-temperature SCR[J]. CIESC Journal, 2019, 70(8): 3000-3010 DOI: 10.11949/0438-1157.20190318.
陈潇雪, 宋敏, 孟凡跃, 卫月星. FexMnCe1-AC低温SCR催化剂SO2中毒机理研究[J]. 化工学报, 2019, 70(8): 3000-3010 DOI: 10.11949/0438-1157.20190318. DOI:
CHEN Xiaoxue, SONG Min, MENG Fanyue, WEI Yuexing. Mechanism study on SO2 poisoning of FexMnCe1-AC catalyst for low-temperature SCR[J]. CIESC Journal, 2019, 70(8): 3000-3010 DOI: 10.11949/0438-1157.20190318. DOI:
以活性炭为载体,通过超声辅助浸渍法制备了一系列Fe
x
MnCe
1
-AC催化剂,考察了该系列催化剂的低温NH
3
-SCR脱硝活性,确立了活性最佳的催化剂,并探究了SO
2
对其脱硝性能的影响。结果表明,Fe
0.1
MnCe
1
-AC催化剂低温脱硝活性最高,在120~220℃范围内NO的转化率均在90%以上(无SO
2
)。此外,在180℃、SO
2
浓度为429 mg/m
3
时,该催化剂仍能保持77%左右的脱硝率。通过BET、XRD、XPS、H
2
-TPR、NH
3
-TPD、FT-IR、TGA等表征手段对催化剂的SO
2
中毒机理进行了分析。研究发现,SO
2
能与NH
3
及催化剂中金属组分生成硫酸铵盐((NH
4
)
2
SO
4
、(NH
4
)
2
SO
3
)、MnSO
4
等物质,改变了原催化剂孔道结构并减少了催化剂表面Brönsted和Lewis酸性位点,抑制了催化剂吸附NH
3
的能力。更多地,SO
2
促使催化剂中Mn
4+
、Ce
3+
、Fe
3+
和Fe
3+
—OH
-
基团数量下降,表面可还原物质减少,从而降低了催化剂的脱硝活性。
A series of Fe
x
MnCe
1
-AC catalysts were prepared by ultrasonic-assisted impregnation method with activated carbon as carrier. The low-temperature NH
3
-SCR denitrification activity of the catalysts was investigated
and the best activity catalyst was established. The effect of SO
2
on its denitration performance was also explored. The results showed that Fe
0.1
MnCe
1
-AC catalyst exhibited best denitration efficiency at low-temperature among prepared catalysts
th
e conversion rate of NO exceeded 90% with the temperature range from 120℃ to 220℃ (no SO
2
). In addition
the catalyst could maintain NO conversion rate of approximately 77% under the atmosphere of 180℃ and SO
2
concentration of 429 mg/m
3
. The mechanism of SO
2
poisoning on the catalyst was characterized with BET
XRD
XPS
H
2
-TPR NH
3
-TPD
FT-IR and TGA. It was observed that SO
2
could form ammonium sulfate ( (NH
4
)
2
SO
4
(NH
4
)
2
SO
3
)
and MnSO
4
with NH
3
and the metal components in the catalyst
which changed the pore structure of the fresh catalyst and reduced the Brönsted acid sites and Lewis acid sites on the catalyst surface. These variation made the inhibitory effect on the catalytic adsorption capacity of NH
3
. Moreover
SO
2
also promoted a decrease in the number of Mn
4+
Ce
3+
Fe
3+
and Fe
3+
—OH
-
groups in the catalyst
and lessened the surface reducible species
thereby reducing the activity of the catalyst denitration.
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