Fe-PILC在贫燃条件下催化丙烯选择性还原NO

李前程; 苏亚欣; 董士林; 袁旻昊; 周皞; 邓文义

Fe-PILC在贫燃条件下催化丙烯选择性还原NO

1.
东华大学环境科学与工程学院, 上海 201620
2.
常州工程技术学院, 江苏常州 213164

基金项目:

国家自然科学基金 51278095

江苏省前瞻性联合研究项目 BY2015032-02

详细信息

中图分类号: X511
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- 被引次数: 0
出版历程
- 收稿日期: 2018-06-22
- 修回日期: 2018-08-22
- 网络出版日期: 2021-01-23
- 刊出日期: 2018-10-10

Fe-PILC for selective catalytic reduction of NO by propene under lean-burn conditions

1.
School of Environmental Science and Engineering, Donghua University, Shanghai 201620, China
2.
Changzhou Vocational Institude of Engineering, Changzhou 213164, China

Funds:

the National Natural Science Foundation of China 51278095

Jiangsu Province Prospective Joint Research Projects BY2015032-02

More Information

Corresponding author: SU Ya-xin, Tel:021-67792552, E-mail:suyx@dhu.edu.cn

摘要

摘要: 采用羟基铁离子柱撑Na-Mont制备了铁柱撑黏土催化剂（Fe-PILC），铁物种作为柱撑成分，同时充当活性组分，研究其在贫燃条件下催化丙烯选择性还原NO的特性。通过XRD、N₂吸附-脱附、H₂-TPR、UV-vis、Py-FTIR等方法对催化剂进行物理化学性质表征，进一步研究其反应机理。研究表明，1.0Fe-PILC在450-600 ℃时NO的转化率超过98%，N₂的选择性可达97%以上，且抗水蒸气和SO₂的能力较强。XRD和N₂吸附-脱附研究表明，Fe-PILC中铁物种柱撑进入Na-Mont层间，使催化剂的比表面积和孔容增大。H₂-TPR研究表明，Fe-PILC在400 ℃左右还原能力较强，主要体现为Fe³⁺→Fe²⁺的还原。UV-vis研究表明，Fe-PILC的脱硝活性与铁氧低聚物种Fe_xO_y呈正相关。Py-FTIR研究表明，Fe-PILC表面同时含有Lewis酸和Brønsted酸性位，Lewis酸性位是C₃H₆与NO进行催化反应的主要活性中心。
- 贫燃条件 /
- 铁柱撑黏土 /
- 丙烯 /
- 选择性催化还原 /
- NO
Abstract: Iron-pillared clays (Fe-PILC) were prepared by ion-exchange method and the iron species act as the pillaring components and active components and their performances for selective catalytic reduction of NO by propene were investigated under lean-burn conditions. XRD, N₂ adsorption/desorption, H₂-TPR, UV-vis, Py-FTIR, etc were used to characterize the catalysts. The results showed that 1.0Fe-PILC reduced more than 98% of NO at 450-600℃ and the selectivity for N₂ reached 97%. The catalytic activity of the 1.0Fe-PILC was slightly influenced by water vapor and SO₂. XRD and N₂ adsorption/desorption characterization results showed that the iron species entered the Na-Mont interlayer and formed much larger specific surface area and pore volume. H₂-TPR results indicated that Fe-PILC had a strong reduction ability at about 400 ℃, which represented the reduction of Fe³⁺→Fe²⁺. UV-vis results showed that the denitrification activity of Fe-PILC was positively correlated with the iron oxide oligomer Fe_xO_y. Py-FTIR results revealed that Lewis acid and Brønsted acid sites formed on the Fe-PILC surface. The main catalytic activity center of C₃H₆ and NO reaction was the Lewis acid site.
- lean-burn conditions /
- Fe-PILC /
- C₃H₆ /
- selective catalytic reduction /
- NO

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图 1 不同催化剂的NO转化率(a)、C₃H₆转化率(b)和N₂选择性(c)

Figure 1 NO conversion (a), C₃H₆ conversion (b), N₂ selectivity (c) of different catalysts

flow rate=100 mL/min, $φ$(NO)=0.1%, $φ$(C₃H₆)=0.1%, $φ$(O₂)=1%, N₂=balance and GHSV=15000 h^-1

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图 2 水蒸气和SO₂对1.0Fe-PILC催化剂活性的影响

Figure 2 Influence of water vapor and SO₂ on 1.0Fe-PILC catalyst

reaction conditions: $φ$(NO)=0.1%, $φ$(C₃H₆)=0.1%, $φ$(O₂)=1%, $φ$(SO₂)=0.02%, $φ$(H₂O)=10%, He=balance and GHSV=15000 h^-1

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图 3 催化剂的物理吸附-脱附等温线(a)和孔径分布图(b)

Figure 3 N₂ adsorption/desorption isotherms (a) and BJH pore size distribution (b) of the catalysts

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图 4 催化剂的XRD谱图

Figure 4 XRD patterns of the catalysts

a: Na-Mont; b: 0.2Fe-PILC; c: 0.5Fe-PILC; d: 1.0Fe-PILC; e: 1.5Fe-PILC

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图 5 Fe-PILC催化剂的H₂-TPR谱图

Figure 5 H₂-TPR profiles of Fe-PILC catalysts

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图 6 催化剂的紫外吸收光谱谱图

Figure 6 UV-vis adsorption spectra of the catalysts

a: 0.2Fe-PILC; b: 1.5Fe-PILC; c: 1.0Fe-PILC

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图 7 不同催化剂的吡啶吸附红外光谱谱图

Figure 7 Py-FTIR spectra of different catalysts

(a): 150 ℃ desorption; (b): 300 ℃ desorption

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表 1 不同催化剂的物理特性

Table 1 Physical properties of different catalysts

Catalyst	Fe w/(mg·g^-1)^a	A_BET/(m²·g^-1)	Pore volume v/(cm³·g^-1)	Pore diameter d/nm
Na-Mont	-	48.6	0.116	9.58
0.2Fe-PILC	142.91	92.0	0.233	8.11
1.0Fe-PILC	180.25	194.7	0.271	6.26
1.5Fe-PILC	190.49	181.2	0.228	5.56
^a: ICP analysis results

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表 2 不同催化剂的B酸和L酸含量

Table 2 Brønsted and Lewis acid content of different catalysts

Sample	150 ℃ desorption /(μmol·g^-1)		300 ℃ desorption/(μmol·g^-1)
Sample	B	L	B	L
Na-Mont	0	45.27	0	23.19
0.2Fe-PILC	2.68	49.01	1.06	35.96
1.0Fe-PILC	4.60	108.87	1.25	58.59
1.5Fe-PILC	2.88	84.63	1.14	52.45

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