Cu交换量对Cu-SAPO-34催化剂上NH3选择性催化还原NOx反应的影响

闫春迪; 程昊; 王树东

Cu交换量对Cu-SAPO-34催化剂上NH₃选择性催化还原NO_x反应的影响

1.
中国科学院大连化学物理研究所洁净能源国家实验室, 辽宁大连 116023;
2.
中国科学院大学, 北京 100049

详细信息

通讯作者:
王树东，男，研究员，主要研究方向为催化反应工程领域的基础研究和应用开发，Tel：0411-84379052/84662365; Fax：+86 411 84662365，E-mail：wangsd@dicp.ac.cn。

中图分类号: O643.36
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出版历程
- 收稿日期: 2014-01-09
- 修回日期: 2014-03-27
- 刊出日期: 2014-06-30

Effects of copper content in Cu-SAPO-34 on its catalytic performance in NH₃-SCR of NO_x

1.
Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;
2.
University of Chinese Academy of Sciences, Beijing 100049, China

摘要

摘要: 选用不同种类的铵盐和调变Cu²⁺离子交换时间制备不同铜交换量的Cu-SAPO-34催化剂。并考察了铜交换量对催化剂在氨选择性催化还原（NH₃-SCR）NO_x反应中的催化性能和高温水热稳定性的影响。结果表明，Cu²⁺是Cu-SAPO-34催化剂在NH₃-SCR反应中的主要活性中心，随着Cu交换量的增加催化剂的低温SCR活性先升高后降低。铜交换量为2.37%时，Cu-SAPO-34催化剂的低温活性最好，NO_x转化率在185 ℃时即可达到80.0%，且最高达98.7%。ICP、H₂-TPR、FT-IR和NH₃-TPD等表征结果显示，Cu引入不但产生了新的氨吸附位点，增加了Lewis酸量，而且略微降低了SAPO-34上氨的吸附强度。继续增加Cu交换量反而导致催化剂的SCR活性下降，这是由于大量的Cu²⁺取代了桥式羟基Si-OH-Al中的H，抑制了SCR反应中NH₃在催化剂表面的吸附、储存与迁移。此外，较高Cu交换量也不利于改善Cu-SAPO-34的高温水热稳定性。
- Cu-SAPO-34 /
- 氨选择性催化还原 /
- 铜交换量 /
- 酸性位 /
- 水热稳定性
Abstract: A series of Cu-SAPO-34 catalysts with various Cu contents were prepared by using different kinds of ammonium salts and adjusting Cu²⁺ ion exchange time; their catalytic performance and hydrothermal stability in selectively catalytic reduction of NO_x with NH₃ (NH₃-SCR) were investigated. The results showed that Cu²⁺ ions are the predominant active sites in Cu-SAPO-34 for the NH₃-SCR of NO_x. With the increase of Cu content, the activity of Cu-SAPO-34 at low temperature is increased at first and then decreased. With a Cu content of 2.37%, the Cu-SAPO-34 catalyst exhibits the best low temperature activity; over it, the conversion of NO_x is higher than 80.0% at 185 ℃ and may even reach 98.7%. ICP, H₂-TPR, FT-IR and NH₃-TPD results illustrated that the introduction of Cu into SAPO-34 leads to an addition of new adsorption sites for ammonia, an increase of Lewis acid sites and a decrease of the adsorption strength of NH₃ on SAPO-34. However, a further increase of Cu loading (e.g. 2.90%) results in a decrease of Cu-SAPO-34 activity in SCR, which may be ascribed to the replacement of H in Si-OH-Al by Cu²⁺ that hinders the adsorption, storage and migration of NH₃ in NH₃-SCR. In addition, excessive loading of Cu is probably detrimental to the hydrothermal stability of the Cu-SAPO-34 catalyst.
- Cu-SAPO-34 /
- NH₃-SCR /
- Cu content /
- acid site /
- hydrothermal stability

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参考文献(21)

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Cu交换量对Cu-SAPO-34催化剂上NH₃选择性催化还原NO_x反应的影响

通讯作者:
王树东，男，研究员，主要研究方向为催化反应工程领域的基础研究和应用开发，Tel：0411-84379052/84662365; Fax：+86 411 84662365，E-mail：wangsd@dicp.ac.cn。

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Effects of copper content in Cu-SAPO-34 on its catalytic performance in NH₃-SCR of NO_x

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