化工进展 ›› 2023, Vol. 42 ›› Issue (3): 1321-1331.DOI: 10.16085/j.issn.1000-6613.2022-1006
柴油车用NH3-SCR铜基分子筛催化剂孤立态Cu2+研究进展
张晨光1(
), 封硕1, 邢玉烨2, 沈伯雄1,2(), 苏立超3
- 1.河北工业大学能源与环境工程学院，天津市清洁能源利用与污染物控制重点实验室，天津 300401
2.河北工业大学化工学院，天津 300401
3.邻筑（河北）工程产业技术研究有限公司，河北 保定 054001
-
收稿日期:2022-05-30修回日期:2022-10-24出版日期:2023-03-15发布日期:2023-04-10 -
通讯作者:沈伯雄 -
作者简介:张晨光（1999—），男，硕士研究生，研究方向为烟气中污染物控制。E-mail：2287588410@qq.com。 -
基金资助:国家自然科学基金联合资助项目(U20A20302);天津市重点研发项目(19ZXZSN00050);河北省重点研发项目(20373701D);河北省重大科技攻关项目(22183701Z)
Research progress of isolated Cu2+ in copper based zeolite NH3-SCR catalyst for diesel vehicles
ZHANG Chenguang1(), FENG Shuo1, XING Yuye2, SHEN Boxiong1,2(), SU Lichao3
- 1.Key Laboratory of Clean Energy Utilization and Pollution Control in Tianjin, College of Energy and Environmental Engineering, Hebei University of Technology, Tianjin 300401, China
2.College of Chemical Engineering, Hebei University of Technology, Tianjin 300401, China
3.Linzhu(Hebei) Engineering Industry Technology Research Corporation Limited, Baoding 054001, Hebei, China
-
Received:2022-05-30Revised:2022-10-24Online:2023-03-15Published:2023-04-10 -
Contact:SHEN Boxiong
摘要：
NH3选择催化还原技术（NH3-SCR）作为一种高效去除NO x 的手段，已广泛地应用到柴油车尾气脱硝过程当中。车用NH3-SCR技术常采用铜基分子筛作为催化剂，尾气中的氮氧化物可在催化剂的作用下，与NH3反应转化为N2；但在实际应用过程中，N2O的生成、催化剂的水热老化与尾气中的SO2会影响铜基分子筛催化剂的脱硝性能。因此，本文以Cu-SSZ-13分子筛催化剂中孤立态Cu2+的研究进展为基础，总结了Cu-SSZ-13中两种孤立态Cu2+对NH3-SCR反应与N2O生成的影响；综述了两种孤立态Cu2+对水热老化与SO2响应的差异；归纳了诱导Cu-2Z生成的手段。同时，本文以Cu-LTA分子筛催化剂的研究现状为例，简要回顾了Cu-LTA中孤立态Cu2+的研究进展，对Cu-LTA的研究趋势与应用前景作出了展望。本文可为其他类型的铜基分子筛催化剂在柴油车尾气脱硝领域的研究提供思路，即明确分子筛中两种孤立态Cu2+相关性质，通过调控孤立态Cu2+对催化剂进行合理设计，在保持高催化活性的同时，进一步提升催化剂的水热稳定性与SO2抗性。
中图分类号:
引用本文
张晨光, 封硕, 邢玉烨, 沈伯雄, 苏立超. 柴油车用NH3-SCR铜基分子筛催化剂孤立态Cu2+研究进展[J]. 化工进展, 2023, 42(3): 1321-1331.
ZHANG Chenguang, FENG Shuo, XING Yuye, SHEN Boxiong, SU Lichao. Research progress of isolated Cu2+ in copper based zeolite NH3-SCR catalyst for diesel vehicles[J]. Chemical Industry and Engineering Progress, 2023, 42(3): 1321-1331.
图1 柴油机尾气处理系统布局示意图氧化催化剂（DOC）：将碳氢化合物（HCs）、CO等物质氧化为H2O和CO2，部分NO氧化为NO2；颗粒捕集器（DPF）：用于捕集颗粒物（PM），外部热源（external heat source）用于去除DPF单元工作过程中产生的积炭；选择性催化还原催化剂（SCR）：用于还原NO x，此过程需要的NH3源于尿素分解；氨氧化催化剂（AOC）：用于将SCR单元逃逸的NH3氧化为N2
图1 柴油机尾气处理系统布局示意图氧化催化剂（DOC）：将碳氢化合物（HCs）、CO等物质氧化为H2O和CO2，部分NO氧化为NO2；颗粒捕集器（DPF）：用于捕集颗粒物（PM），外部热源（external heat source）用于去除DPF单元工作过程中产生的积炭；选择性催化还原催化剂（SCR）：用于还原NO x，此过程需要的NH3源于尿素分解；氨氧化催化剂（AOC）：用于将SCR单元逃逸的NH3氧化为N2
表1 Cu-SSZ-13催化下作用下NO高效转化的温度区间
| Si/Al | 制备方式 | 测试条件 | 脱硝效率 | 参考文献 |
|---|---|---|---|---|
| 6 | 液相离子交换 | [NO]=[NH3]=500mg/kg，[O2]=5%，体积空速=25000h-1 | ＞90%（175~550℃） | [ |
| 6.5 | 液相离子交换 | [NO]=[NH3]=200mg/kg，[O2]=5%，体积空速=60000h-1 | ＞90%（250~500℃） | [ |
| 11 | 液相离子交换 | [NO]=[NH3]=500mg/kg，[O2]=5%，体积空速=120000h-1 | ＞90%（200~500℃） | [ |
| 24 | 液相离子交换 | [NO]=[NH3]=350mg/kg，[O2]=14%，体积空速=30000h-1 | ＞90%（200~450℃） | [ |
表1 Cu-SSZ-13催化下作用下NO高效转化的温度区间
| Si/Al | 制备方式 | 测试条件 | 脱硝效率 | 参考文献 |
|---|---|---|---|---|
| 6 | 液相离子交换 | [NO]=[NH3]=500mg/kg，[O2]=5%，体积空速=25000h-1 | ＞90%（175~550℃） | [ |
| 6.5 | 液相离子交换 | [NO]=[NH3]=200mg/kg，[O2]=5%，体积空速=60000h-1 | ＞90%（250~500℃） | [ |
| 11 | 液相离子交换 | [NO]=[NH3]=500mg/kg，[O2]=5%，体积空速=120000h-1 | ＞90%（200~500℃） | [ |
| 24 | 液相离子交换 | [NO]=[NH3]=350mg/kg，[O2]=14%，体积空速=30000h-1 | ＞90%（200~450℃） | [ |
图2 CHA型分子筛结构与Cu-SSZ-13结构示意图[22]
图2 CHA型分子筛结构与Cu-SSZ-13结构示意图[22]
图3 两种孤立态Cu2+对N2O生成的影响
图3 两种孤立态Cu2+对N2O生成的影响
图4 Cu-SSZ-13中两种孤立态Cu2+对水热老化、热老化及SO2的响应差异
图4 Cu-SSZ-13中两种孤立态Cu2+对水热老化、热老化及SO2的响应差异
图5 不同合成条件对Cu-SSZ-13中孤立态Cu2+生成的影响
图5 不同合成条件对Cu-SSZ-13中孤立态Cu2+生成的影响
表2 具有不同拓扑结构的铜基催化剂在水热老化前后的脱硝性能
| 催化剂 | 拓扑结构 | 水热老化条件 | 测试条件 | 脱硝效率 | 参考文献 |
|---|---|---|---|---|---|
| Cu-LTA | LTA | [温度]=900℃，[H2O]=10%，[时间]=12h | [NH3]=[NO]=0.05%，体积空速=100000h-1，[O2]=5%，[H2O]=10% | ＞90%(250~600℃)-新鲜，＞80%(250~550℃)-老化 | [ |
| Cu-SSZ-39 | AFI | [温度]=850℃，[H2O]=10%，[时间]=16h | [NH3]=[NO]=0.05%，体积空速=25000h-1，[O2]=5%，[H2O]=5% | 约100%(225~450℃)-新鲜，＞80%(250~500℃)-老化 | [ |
| Cu-AFX | AFX | [温度]=800℃，[H2O]=5%，[时间]=16h | [NH3]=[NO]=0.03%，体积空速=144000h-1，[O2]=5%，[H2O]=3% | 约100%(250~400℃)-新鲜，约100%(250~350℃)-老化 | [ |
| Cu-ERI | ERI | [温度]=850℃，[H2O]=10%，[时间]=5h | [NH3]=[NO]=0.03%，体积空速=50000h-1，[O2]=5%，[H2O]=3% | ＞90%(250~600℃)-新鲜，＞70%(250~500℃)-老化 | [ |
| Cu-ZJM-7 | KFI | [温度]=850℃，[H2O]=10%，[时间]=12h | [NH3]=[NO]=0.05%，体积空速=80000h-1，[O2]=5%，[H2O]=5% | 约100%(200~400℃)-新鲜，＞80%(250~400℃)-老化 | [ |
| Cu-UZM-35 | MSE | [温度]=800℃，[H2O]=10%，[时间]=24h | [NH3]=[NO]=0.05%，体积空速=100000h-1，[O2]=5%，[H2O]=10% | 约100%(200~450℃)-新鲜，＞80%(250~500℃)-老化 | [ |
表2 具有不同拓扑结构的铜基催化剂在水热老化前后的脱硝性能
| 催化剂 | 拓扑结构 | 水热老化条件 | 测试条件 | 脱硝效率 | 参考文献 |
|---|---|---|---|---|---|
| Cu-LTA | LTA | [温度]=900℃，[H2O]=10%，[时间]=12h | [NH3]=[NO]=0.05%，体积空速=100000h-1，[O2]=5%，[H2O]=10% | ＞90%(250~600℃)-新鲜，＞80%(250~550℃)-老化 | [ |
| Cu-SSZ-39 | AFI | [温度]=850℃，[H2O]=10%，[时间]=16h | [NH3]=[NO]=0.05%，体积空速=25000h-1，[O2]=5%，[H2O]=5% | 约100%(225~450℃)-新鲜，＞80%(250~500℃)-老化 | [ |
| Cu-AFX | AFX | [温度]=800℃，[H2O]=5%，[时间]=16h | [NH3]=[NO]=0.03%，体积空速=144000h-1，[O2]=5%，[H2O]=3% | 约100%(250~400℃)-新鲜，约100%(250~350℃)-老化 | [ |
| Cu-ERI | ERI | [温度]=850℃，[H2O]=10%，[时间]=5h | [NH3]=[NO]=0.03%，体积空速=50000h-1，[O2]=5%，[H2O]=3% | ＞90%(250~600℃)-新鲜，＞70%(250~500℃)-老化 | [ |
| Cu-ZJM-7 | KFI | [温度]=850℃，[H2O]=10%，[时间]=12h | [NH3]=[NO]=0.05%，体积空速=80000h-1，[O2]=5%，[H2O]=5% | 约100%(200~400℃)-新鲜，＞80%(250~400℃)-老化 | [ |
| Cu-UZM-35 | MSE | [温度]=800℃，[H2O]=10%，[时间]=24h | [NH3]=[NO]=0.05%，体积空速=100000h-1，[O2]=5%，[H2O]=10% | 约100%(200~450℃)-新鲜，＞80%(250~500℃)-老化 | [ |
图6 LTA型分子筛结构与Cu-LTA结构示意图[47]
图6 LTA型分子筛结构与Cu-LTA结构示意图[47]
图7 Cu-LTA中两种孤立态Cu2+对水热老化与SO2响应的差异
图7 Cu-LTA中两种孤立态Cu2+对水热老化与SO2响应的差异
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