Ag对Fe/Al-PILC的SCR-C<sub>3</sub>H<sub>6</sub>脱硝特性的影响

张显威; 苏亚欣; 程江浩; 林睿; 温妮妮; 邓文义; 周皞

Ag对Fe/Al-PILC的SCR-C₃H₆脱硝特性的影响

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:

上海市自然科学基金 19ZR1400700

江苏省自然科学基金 BK20181161

中央高校基本科研业务费 2232019D3-24

详细信息

中图分类号: X511
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出版历程
- 收稿日期: 2019-06-17
- 修回日期: 2019-09-09
- 网络出版日期: 2021-01-23
- 刊出日期: 2019-11-10

Effect of Ag on deNO_x performance of SCR-C₃H₆ over Fe/Al-PILC catalysts

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

Funds:

the Natural Science Foundation of Shanghai 19ZR1400700

Jiangsu Province Natural Science Foundation BK20181161

the Fundamental Research Funds for the Central Universities 2232019D3-24

More Information

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

摘要

摘要: 为提高低温段（< 300℃）铝柱撑蒙脱土负载铁基催化剂的脱硝效率，采用银离子对其进行修饰。通过超声浸渍法合成银-铁双金属催化剂，并于固定床反应器中评价催化剂性能。结果表明，Ag的引入显著改善了Fe/Al-PILC催化剂的低温催化活性。在250℃时，Ag-Fe/Al-PILC催化剂的NO转化率达到60%以上，高于Fe/Al-PILC催化剂20%的NO的转化率，其中，2.1Ag-Fe/Al-PILC在250℃时NO转化率达到82%，N₂选择性达到100%。而且，引入银离子后的双金属催化剂保持了铁基催化剂较好的抗H₂O和SO₂性能。通过多种技术探究催化剂的微观结构和物理化学性质。根据N₂吸附-脱附测试结果表明，双金属催化剂形成了稳定的整体结构，并具有较大的内比表面积。同时，XRD和UV-vis表征结果显示，在催化剂表面形成的银-铁固溶体、Ag⁺和Ag_n^δ+物种是影响其低温活性的关键因素。Ag-Fe/Al-PILC的低温活性与形成的银-铁固溶体有关，同时在催化剂表面形成的Ag⁺和Ag_n^δ+物种是影响其低温活性的关键因素。XPS结果表明，Ag和Fe之间存在电子转移，形成了双金属协同作用，改变了催化剂表面的银、铁成分含量及其价态。H₂-TPR结果表明，Ag促使Fe/Al-PILC还原特征峰出现在低温区，提高了其低温还原性能。表面酸性的Py-FTIR分析结果表明，Ag-Fe/Al-PILC催化剂同时存在Lewis酸和Brønsted酸，且Ag提高了Brønsted酸的稳定性。
- 选择性催化还原 /
- 柱撑黏土 /
- Ag-Fe/Al-PILC
Abstract: Silver has been widely used to modify the iron-based catalyst supported on alumina pillared montmorillonite to enhance its activity at lower temperature (< 300℃). Bimetallic Ag-Fe/Al-PILC (Pillared interlayer clay) was prepared by the ultrasonic impregnation method and performance was tested on a fixed bed reactor. And the experiment results showed that silver obviously improved the catalyst activity at a lower temperature. The NO conversion efficiency of Ag-Fe/Al-PILC at 250℃ was 60%, which was higher than Fe/Al-PILC (20%). The maximum 82% NO conversion and 100% N₂ selectivity were obtained by 2.1Ag-Fe/Al-PILC at 250℃. Moreover, Ag-Fe/Al-PILC revealed better anti-hydrogen peroxide and anti-sulfur dioxide ability. The catalyst characterization was conducted by several techniques with respect to the microstructure and physicochemical properties. According to the effects of N₂-adsorption and desorption tests, Ag-Fe/Al-PILC formed a stable overall structure and had a large internal specific surface area. Besides, XRD and UV-vis proved that the Ag-Fe solid solution, Ag⁺ and Ag_n^δ+ species formed on the surface of the catalyst are the key factors affecting its low-temperature activity. XPS results suggested that there was electron transfer between Ag and Fe, which formed a synergistic effect of bimetals and changed the content of Ag and Fe and their valence state on the catalyst surface. The findings of H₂-TPR indicated that the modification of Ag promoted the shift of the Fe/Al-PILC reduction peak toward low temperature, which boosted the low-temperature reduction capacity of the catalyst. The surface acidity analysis by Py-FTIR indicated that Lewis acid and Brønsted acid existed simultaneously and Ag enhanced the stability of Brønsted acid.
- selective catalytic reduction /
- pillared clay /
- Ag-Fe/Al-PILC

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图 1 Ag负载量对NO和C₃H₆转化率及N₂选择性的影响

Figure 1 Effect of Ag loading on the conversion of NO and C₃H₆ conversion and N₂ selectivity

(a): NO conversion; (b): C₃H₆ conversion; (c): N₂ selectivity; (d): effect of iron loading φ_NO=0.05%, φ_C₃H₆=0.2%, φ_O₂=1%, N₂ balance, GHSV=22000h^-1

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图 2 350℃时SO₂和H₂O对催化剂活性的影响

Figure 2 Effect of SO₂ and H₂O on catalytic activity at 350℃

(a): φ_NO=0.05%, φ_C₃H₆=0.2%, φ_O₂=1%, φ_SO₂=0.02%, N₂ balance, GHSV=22000h^-1; (b): φ_NO=0.05%, φ_C₃H₆=0.2%, φ_O₂=1%, φ_H₂O=7%, N₂ balance, GHSV=22000h^-1

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图 3 不同催化剂的N₂吸附-脱附等温曲线及孔径分布

Figure 3 N₂ adsorption-desorption isotherm curve and pore size distribution of different catalysts

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图 4 催化剂的XRD谱图

Figure 4 XRD patterns of the catalysts

a: Fe/Al-PILC; b: 0.4Ag-Fe/Al-PILC; c: 2.1Ag-Fe/Al-PILC; d: 3.3Ag-Fe/Al-PILC

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图 5 催化剂的H₂-TPR谱图

Figure 5 H₂-TPR profiles of the catalyst samples

a: 0.4Ag-Fe/Al-PILC; b: 2.1Ag-Fe/Al-PILC; c: 3.3Ag-Fe/Al-PILC; d: Fe/Al-PILC

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图 6 催化剂的紫外吸收谱图

Figure 6 UV-vis adsorption spectra of catalysts

a: 2.1Ag-Fe/Al-PILC; b: 0.4Ag-Fe/Al-PILC; c: Fe/Al-PILC; d: 3.3Ag-Fe/Al-PILC

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图 7 催化剂中Ag和Fe元素的XPS谱图

Figure 7 XPS spectra of Cu and Fe element in catalysts

a: 0.4Ag-Fe/Al-PILC; b: 2.1Ag-Fe/Al-PILC; c: 3.3Ag-Fe/Al-PILC

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图 8 不同催化剂的吡啶吸附红外光谱谱图

Figure 8 Py-FTIR spectra of different catalysts

a: 0.4Ag-Fe/Al-PILC; b: 2.1Ag-Fe/Al-PILC; c: 3.3Ag-Fe/Al-PILC

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表 1 不同催化剂的比表面积和孔结构

Table 1 Specific surface area and pore structure of different catalysts

Catalyst	Ag loading^a w/%	A_BET^b/(m²·g^-1)	v_p/(cm³·g^-1)	d_p^c/nm
Fe/Al-PILC	-	184	0.260	4.84
0.4Ag-Fe/Al-PILC	0.4	87	0.112	5.14
2.1Ag-Fe/Al-PILC	2.1	72	0.105	5.59
3.3Ag-Fe/Al-PILC	3.3	65	0.092	5.71
^a: the Fe loading was measured by ICP analysis; ^b: total surface area was determined from the BET equatio; ^c: the pore diameter was obtained by the BJH method

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表 2 Ag和Fe元素的结合能及Ag和Fe原子在催化剂表面的百分比

Table 2 Binding energy of Ag and Fe elements and percentage of Ag and Fe atoms on the catalyst surface

Sample	Binding energy E/eV			Surface atomic /%
Sample	Ag 3d_5/2	Fe 2p_3/2	Fe 2p_1/2	Fe	Ag
2.1Ag-Fe/Al-PILC	368.5	711.7	724.6	23.9	4.6
2.1Ag/Al-PILC	368.7	-	-	-	5.2
Fe/Al-PILC	-	711.2	724.3	22.1	-

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表 3 Ag⁺和Ag⁰在催化剂表面的百分比

Table 3 Percentage of Ag⁺ and Ag⁰ on the catalyst surface

Sample	0.4Ag-Fe/Al-PILC	2.1Ag-Fe/Al-PILC	3.3Ag-Fe/Al-PILC
Ag⁺(368eV)	18%	34%	28%
Ag⁰(368.8eV)	82%	66%	72%

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表 4 不同催化剂酸性位的含量

Table 4 Acid amount of different catalysts

Sample	Acid amount/(μmol·g^-1)
	40℃ desorption		170℃ desorption		300℃ desorption
	B	L	B	L	B	L
Fe/Al-PILC	-	-	6.91	46.95	0.00	34.43
0.4Ag-Fe/Al-PILC	2.83	96.95	1.81	35.19	0.77	11.91
2.1Ag-Fe/Al-PILC	7.94	95.80	2.84	48.04	2.33	37.38
3.3Ag-Fe/Al-PILC	3.85	177.59	1.69	89.99	0.757	31.67

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