Fe/Al-SiO<sub>2</sub>复合金属氧化物用于燃煤烟气中汞的脱除

李扬; 陈伟; 赵永椿; 李海龙; 张军营; 李杰; 胡浩权

Fe/Al-SiO₂复合金属氧化物用于燃煤烟气中汞的脱除

李扬¹,
陈伟¹,
赵永椿²,
李海龙³,
张军营²,
李杰⁴,
胡浩权^1, ,

1.
大连理工大学化工学院, 精细化工国家重点实验室, 煤化工研究所, 辽宁大连 116024
2.
华中科技大学煤燃烧重点实验室, 湖北武汉 430074
3.
中南大学能源科学与工程学院, 湖南长沙 410083
4.
大连理工大学环境学院, 辽宁大连 116024

基金项目:

国家自然科学基金 21776039

国家自然科学基金青年科学基金 51306028

中央高校基本科研业务费 DUT2018TB0

详细信息

中图分类号: X701.7
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- 被引次数: 0
出版历程
- 收稿日期: 2019-05-14
- 修回日期: 2019-10-17
- 网络出版日期: 2021-01-23
- 刊出日期: 2019-12-10

Removal of elemental mercury from flue gas by Fe/Al-SiO₂ complex

1.
State Key Laboratory of Fine Chemicals, Institute of Coal Chemical Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
2.
State Key of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China
3.
School of Energy Science and Engineering, Central South University, Changsha 410083, China
4.
School of Environmental Science and Technology, Dalian 116024, China

Funds:

the National Natural Science Foundation of China 21776039

National Natural Science Foundation for Young Scientist of China 51306028

the Fundamental Research Funds for the Central Universities DUT2018TB0

More Information

Corresponding author: HU Hao-quan, Tel: 0411-84986157, E-mail: hhu@dlut.edu.cn

摘要

摘要: 采用不同方法制备了Fe/Al-SiO₂复合金属氧化物以模拟赤泥成分，模拟烟气条件下考察其脱汞性能。结果表明，采用溶胶-凝胶法得到的复合金属氧化物在300-450 ℃具有优异的脱汞性能，其中，在350 ℃、3 h内平均脱汞率可达到94.8%。Fe₂O₃为Hg⁰的氧化提供了晶格氧和化学吸附氧；SiO₂形成的硅溶胶则有利于活性组分Fe₂O₃的分散，增强了Hg⁰与活性位的接触。基本模拟烟气中存在微量HCl和NO时，Hg⁰脱除率接近100%；当烟气中存在0.2 mL/min、0.4 mL/min的SO₂时，吸附剂的平均脱汞率分别降至90.7%、53.4%，这主要是由于SO₂与Fe₂O₃反应生成Fe₂（SO₄）₃，导致了Fe₂O₃的失活并抑制汞的脱除。
- 吸附剂 /
- 元素汞 /
- 烟道气 /
- Fe/Al-SiO₂
Abstract: The Fe/Al-SiO₂ composite metal oxides were prepared by various methods to simulate the composition of red mud. A series of experiments were carried out to study the mercury removal performance from simulated flue gas. The results show that the composite metal oxide obtained by sol-gel method has an excellent mercury removal performance in a temperature range of 300-450 ℃. Among them, average mercury removal efficiency can reach 94.8% within 3 h at 350 ℃. Fe₂O₃ provides lattice oxygen and chemical adsorbed oxygen for the oxidation of Hg⁰, and SiO₂ is conducive to the dispersion of the active component Fe₂O₃, which enhances the contact between Hg⁰ and the active sites. In the presence of trace HCl and NO in flue gas, the removal efficiency of Hg⁰ is close to 100%. However, the average mercury removal efficiency reduces to 90.7% and 53.4% respectively after adding 0.2 mL/min and 0.4 mL/min SO₂, since the reaction of SO₂ and Fe₂O₃ produces Fe₂(SO₄)₃, leading to the deactivation of Fe₂O₃.
- sorbents /
- elemental mercury /
- flue gas /
- Fe/Al-SiO₂

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图 1 实验装置示意图

Figure 1 Schematic diagram of experimental device

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图 2 样品N₂吸附-脱附等温线

Figure 2 Nitrogen adsorption isotherm curves of samples prepared by different methods

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图 3 不同制备方法得到的Fe/Al-SiO₂的脱汞效率

Figure 3 Mercury removal rate of Fe/Al-SiO₂ complex prepared by different methods

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图 4 吸附剂的制备方法及组分对脱汞的影响

Figure 4 Influence of different preparation methods and components of sorbents on mercury removal

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图 5 反应温度对脱汞效率的影响

Figure 5 Effect of reaction temperature on mercury removal

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图 6 不同气氛对脱汞效率的影响

Figure 6 Effects of different atmospheres on mercury removal

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图 7 反应前后Fe/Al-SiO₂吸附剂的H₂-TPR谱图

Figure 7 H₂-TPR profiles of Fe/Al-SiO₂ before and after the reaction

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图 8 SFG反应前后FAS样品O 1s、Fe 2p及Hg 4f分析

Figure 8 O 1s, Fe 2p and Hg 4f analysis of FAS samples before and after reaction in SFG

(a): O 1s; (b): Fe 2p; (c): Hg 4f

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图 9 SG-FAS在各气氛中反应后的Hg-TPD谱图

Figure 9 Hg-TPD curve of SG-FAS after reaction in different atmospheres

(a): SFG; (b): 0.01‰ HCl; (c): 0.2‰ SO₂; (d): 0.2‰ NO

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表 1 不同制备方法得到的样品比表面积和孔容

Table 1 Specific surface area and pore volume of samples prepared by different methods

Sample	Specific surface area A /(m²·g^-1)	Pore volume v /(cm³·g^-1)
I-FAS	46	0.215
UI-FAS	32	0.078
SG-FS	403	0.672
SG-AS	370	0.861
SG-FAS	344	0.484

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