化工进展 ›› 2023, Vol. 42 ›› Issue (6): 2954-2962.DOI: 10.16085/j.issn.1000-6613.2022-1453
H2-SCR改性铂系催化剂低温脱硝的应用及性能强化挑战
张巍1,2(
), 秦川1,2, 谢康1,2, 周运河1,2, 董梦瑶1,2, 李婕1,2, 汤云灏1,2, 马英3, 宋健4
- 1.长沙理工大学能源与动力工程学院，湖南 长沙 410114
2.可再生能源电力技术湖南省重点实验室，湖南 长沙 410114
3.永清环保股份有限公司，湖南 长沙 410330
4.湖南大唐节能科技有限公司，湖南 长沙 410007
-
收稿日期:2022-08-03修回日期:2022-12-25出版日期:2023-06-25发布日期:2023-06-29 -
通讯作者:张巍 -
作者简介:张巍（1974—），男，博士，副教授，硕士生导师，研究方向为高效清洁燃烧与污染物控制。E-mail：weizhang@csust.edu.cn。 -
基金资助:国家留学基金(201808430112);湖南省自然科学基金(2020JJ4098);湖南省教育厅科学研究项目重点项目(21A0216);长沙理工大学青年教师成长计划(2019QJCZ044);“可再生能源电力技术”湖南省重点实验室开放基金(2018ZNDL004)
Application and performance enhancement challenges of H2-SCR modified platinum-based catalysts for low-temperature denitrification
ZHANG Wei1,2(), QIN Chuan1,2, XIE Kang1,2, ZHOU Yunhe1,2, DONG Mengyao1,2, LI Jie1,2, TANG Yunhao1,2, MA Ying3, SONG Jian4
- 1.School of Energy and Power Engineering, Changsha University of Science and Technology, Changsha 410114, Hunan, China
2.Key Laboratory of Renewable Energy and Electric Power Technology of Hunan Province, Changsha 410114, Hunan, China
3.Yonker Environmental Protection Company Limited, Changsha 410330, Hunan, China
4.Hunan Datang Energy-saving Technology Company Limited, Changsha 410007, Hunan, China
-
Received:2022-08-03Revised:2022-12-25Online:2023-06-25Published:2023-06-29 -
Contact:ZHANG Wei
摘要：
氮氧化物（NO x ）的排放严重危害了生态环境和人类健康，其主要来源有固定源烟气排放和移动源尾气排放。近年来，利用氢气选择性催化还原（H2-SCR）改性铂系催化剂控制移动源NO x 的相关研究引起了广泛的关注，由于不同的改性方法可以促进铂与载体之间的电子迁移，从而形成双功能反应机制酸位点，因而通过深入认识铂系H2-SCR催化剂的NO x 催化反应机制并获得良好的改性方法对于开发高效移动源脱硝催化剂具有深远的意义。本文综述了铂系H2-SCR脱硝催化剂的种类，阐述了其表面的H2/NO吸附机制、NO氧化还原机制和双功能反应机制，总结了提高铂系H2-SCR催化剂的稳定性、抗硫性和选择性的强化方法。进一步阐述了金属氧化物和分子筛负载型铂系H2-SCR催化剂可变的多价态，电子迁移能力，NO、H2和O2在催化剂表面的反应机理，并对铂负载减量化降低成本的相关研究进行了展望。
中图分类号:
引用本文
张巍, 秦川, 谢康, 周运河, 董梦瑶, 李婕, 汤云灏, 马英, 宋健. H2-SCR改性铂系催化剂低温脱硝的应用及性能强化挑战[J]. 化工进展, 2023, 42(6): 2954-2962.
ZHANG Wei, QIN Chuan, XIE Kang, ZHOU Yunhe, DONG Mengyao, LI Jie, TANG Yunhao, MA Ying, SONG Jian. Application and performance enhancement challenges of H2-SCR modified platinum-based catalysts for low-temperature denitrification[J]. Chemical Industry and Engineering Progress, 2023, 42(6): 2954-2962.
表1 近年来文献中报道的金属氧化物负载铂系H2-SCR催化剂
| 催化剂 | 制备方法 | 最佳反应温度/最佳脱硝 效率/最佳N2选择性 | 反应条件 | 参考 文献 |
|---|---|---|---|---|
| Pt/MnO x | 共沉淀法 | 100℃/64%/30% | 0.048mL/min NO，5%（体积分数）O2，He平衡，空速（GHSV）为78000h-1 | [ |
| Pt/ZrO2 | 浸渍法 | 150℃/71%/75% | 0.2mL/min NO x，1mL/min H2，10%（体积分数）O2，N2为平衡气，温度60~280℃， 总流量200mL/min | [ |
| Pt/MgO | 浸渍法 | 150℃/71.4%/62% | 0.2mL/min NO x，1mL/min H2，10%（体积分数）O2，N2为平衡气，温度60~280℃， 总流量200mL/min | [ |
| Pt/Al2O3 | 浸渍法 | 91℃/88%/90% | 4.8mL/min NO，1vol% H2, 5vol% O2，N2为平衡气，温度20~350℃，总流量2400mL/min，GHSV为12000h-1 | [ |
| Pt/Mg3Al1O x | 共沉淀法 | 200~220℃/92%/60% | 0.125mL/min NO x，0.5%~2%（体积分数）H2，0~10%（体积分数）O2，Ar为平衡气， 总流量200~300mL/min，GHSV为12000h-1 | [ |
| Pt/Ce0.5Zr0.5O2 | 溶胶-凝胶法 | 120~220℃/92%/78% | 0.03mL/min NO，2.5%（体积分数）O2，0.8%（体积分数）H2，10%（体积分数）CO2，15%（体积分数）H2O，0.5%（体积分数）C3H6，总流量200mL/min，GHSV为33000h-1 | [ |
| Pt/MgO-CeO2 | 湿浸渍法 | 150℃/94%/80% | 0.25%（摩尔分数）NO，1.0%（摩尔分数）H2，5%（摩尔分数）O2，He为平衡气体，总流量100mL/min，GHSV为80000h-1 | [ |
表1 近年来文献中报道的金属氧化物负载铂系H2-SCR催化剂
| 催化剂 | 制备方法 | 最佳反应温度/最佳脱硝 效率/最佳N2选择性 | 反应条件 | 参考 文献 |
|---|---|---|---|---|
| Pt/MnO x | 共沉淀法 | 100℃/64%/30% | 0.048mL/min NO，5%（体积分数）O2，He平衡，空速（GHSV）为78000h-1 | [ |
| Pt/ZrO2 | 浸渍法 | 150℃/71%/75% | 0.2mL/min NO x，1mL/min H2，10%（体积分数）O2，N2为平衡气，温度60~280℃， 总流量200mL/min | [ |
| Pt/MgO | 浸渍法 | 150℃/71.4%/62% | 0.2mL/min NO x，1mL/min H2，10%（体积分数）O2，N2为平衡气，温度60~280℃， 总流量200mL/min | [ |
| Pt/Al2O3 | 浸渍法 | 91℃/88%/90% | 4.8mL/min NO，1vol% H2, 5vol% O2，N2为平衡气，温度20~350℃，总流量2400mL/min，GHSV为12000h-1 | [ |
| Pt/Mg3Al1O x | 共沉淀法 | 200~220℃/92%/60% | 0.125mL/min NO x，0.5%~2%（体积分数）H2，0~10%（体积分数）O2，Ar为平衡气， 总流量200~300mL/min，GHSV为12000h-1 | [ |
| Pt/Ce0.5Zr0.5O2 | 溶胶-凝胶法 | 120~220℃/92%/78% | 0.03mL/min NO，2.5%（体积分数）O2，0.8%（体积分数）H2，10%（体积分数）CO2，15%（体积分数）H2O，0.5%（体积分数）C3H6，总流量200mL/min，GHSV为33000h-1 | [ |
| Pt/MgO-CeO2 | 湿浸渍法 | 150℃/94%/80% | 0.25%（摩尔分数）NO，1.0%（摩尔分数）H2，5%（摩尔分数）O2，He为平衡气体，总流量100mL/min，GHSV为80000h-1 | [ |
图1 Pt/HZSM-5在H2-SCR中不同位置Pt作用示意图[28]
图1 Pt/HZSM-5在H2-SCR中不同位置Pt作用示意图[28]
图2 Pt表面和Pt–HY界面上N2和N2O的生成路径[37]
图2 Pt表面和Pt–HY界面上N2和N2O的生成路径[37]
图3 Pt/MgO-CeO2催化剂上H2选择性催化还原的机理[39]
图3 Pt/MgO-CeO2催化剂上H2选择性催化还原的机理[39]
图4 Pt/BG催化剂上H2-SCR在过量氧存在下的双功能催化机理[41]
图4 Pt/BG催化剂上H2-SCR在过量氧存在下的双功能催化机理[41]
图5 负载型Pt催化剂H2-SCR中酸性载体吸附过程[18]
图5 负载型Pt催化剂H2-SCR中酸性载体吸附过程[18]
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