Al-PILC负载铜铁复合氧化物在NH<sub>3</sub>选择性催化还原NO中的协同作用

朱斌; 费兆阳; 陈献; 汤吉海; 崔咪芬; 乔旭

Al-PILC负载铜铁复合氧化物在NH₃选择性催化还原NO中的协同作用

朱斌¹,
费兆阳^1,2,
陈献¹,
汤吉海¹,
崔咪芬¹,
乔旭^1,2,

1.
南京工业大学化学化工学院, 江苏南京 210009;
2.
南京工业大学材料化学工程国家重点实验室, 江苏南京 210009

基金项目: 国家自然科学基金（21306089）；国家科技支撑计划（2011BAE18B01）；江苏省高校自然科学基金（13KJB530006）；江苏省科技支撑计划（BE2011830）。

详细信息

通讯作者:
乔旭，Tel：025-83587168，E-mail：qct@njtech.edu.cn。

中图分类号: O643.3
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出版历程
- 收稿日期: 2014-03-27
- 修回日期: 2014-06-06
- 刊出日期: 2014-09-30

Synergetic effect of Cu-Fe composite oxides supported on Al-PILC for SCR of NO with NH₃

1.
College of Chemistry and Chemical Engineering, Nanjing University of Technology, Nanjing 210009, China;
2.
State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing University of Technology, Nanjing 210009, China

摘要

摘要: 以铝柱撑黏土（Al-PILC）为载体采用旋蒸-浸渍法制备了铜、铁单组分催化剂（Cu/Al-PILC、Fe/Al-PILC）和铜铁复合氧化物催化剂（CuFe/Al-PILC），并测试其对NH₃选择性催化还原NO反应（NH₃-SCR）的催化性能。相比Cu/Al-PILC 和Fe/Al-PILC，CuFe/Al-PILC活性组分之间有较强的协同效应，显著提高了催化剂的脱硝性能。CuFe/Al-PILC在290~450℃的宽温区NO脱除效率保持90%以上，最高可达97%。此外，CuFe/Al-PILC有很好的抗水抗硫性能，催化活性不受反应气氛中水蒸气和SO₂的影响。XRD、UV-vis、XPS和N₂吸附脱附表征结果表明，CuFe/Al-PILC中活性组分相互作用生成CuFe₂O₄，有利于活性组分在载体表面分散，提高催化剂的比表面积和孔容；H₂-TPR表征结果表明，CuFe/Al-PILC活性组分在载体表面生成的CuFe₂O₄改善了催化剂氧化还原性能，有利于NH₃ 对NO选择性的还原；NH₃-TPD表征结果表明，CuFe/Al-PILC在较宽温区范围内对NH₃都有很好的吸附，这有利于提高催化剂表面还原物种的浓度，从而保证催化剂在较宽温区范围内具有较好的NO脱除效率。
- 选择性还原 /
- 脱硝 /
- 铝柱撑黏土 /
- 铜铁复合催化剂 /
- 协同作用
Abstract: Cu/Al-PILC, Fe/Al-PILC and CuFe/Al-PILC were prepared by rotary evaporation-impregnation method using Al-PILC as support. Selected catalytic reduction of NO with NH₃ (NH₃-SCR) was carried out in a fixed bed reactor to evaluate their catalytic performance. Compared to Cu/Al-PILC and Fe/Al-PILC, CuFe/Al-PILC showed better NO removal efficiency (97%) and a wider temperature range (290~450℃) of 90% DeNO because of the strong synergetic effect of Cu-Fe composite oxides. Moreover, CuFe/Al-PILC showed good resistance to water vapor and SO₂. XRD, UV-vis, XPS and N₂ adsorption were used to characterize the structure of the catalysts. A new phase CuFe₂O₄ formed in CuFe/Al-PILC, which changed the surface properties of CuFe/Al-PILC, improved the dispersion of Cu and Fe on the Al-PILC surface and increased A_BET and v_p of CuFe/Al-PILC. H₂-TPR confirmed the existence of CuFe₂O₄, which improved the re-dox property of CuFe/Al-PILC. The result of NH₃-TPD implied that the surface acidity of CuFe/Al-PILC made it possible to adsorb and desorb NH₃ in a wide temperature range. The concentration of reducible species on the surface of CuFe/Al-PILC increased, which resulted in high NO removal efficiency.
- SCR /
- DeNO /
- Al-PILC /
- Cu-Fe composite oxides catalyst /
- synergetic effect

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