La0.7Sr0.3Co1-xFexO3催化剂氮氧化物储存及抗硫性能

doi:10.3866/PKU.WHXB201203311

物理化学学报 >> 2012, Vol. 28 >> Issue (06): 1474-1480.doi: 10.3866/PKU.WHXB201203311

La_0.7Sr_0.3Co_1-xFe_xO₃催化剂氮氧化物储存及抗硫性能

马爱静¹, 王绍增¹, 邹鸿鹄¹, 孟明¹, 李志军², 鲍骏³, 李新刚¹

1. 天津大学化工学院, 天津市应用催化科学与工程重点实验室, 天津 300072;
2. 天津大学内燃机燃烧学国家重点实验室, 天津 300072;
3. 中国科学技术大学国家同步辐射实验室, 合肥 230029

收稿日期:2012-01-16 修回日期:2012-03-31 发布日期:2012-05-17
通讯作者: 李新刚 E-mail:xingang_li@tju.edu.cn
基金资助:
国家自然科学基金(20806056, U1162103), 国家高技术研究发展计划(863 计划) (2008AA06Z323), 天津市自然科学基金(11JCYBJC03700), 教育部新世纪优秀人才支持计划(NCET-10-0615), 教育部留学归国人员科研启动基金(2011-1568)以及天津大学内燃机燃烧学国家重点实验室开放基金(K2012-05)资助项目

The Performance of the NO_x Storage Capacity and Sulfur Tolerance of the La_0.7Sr_0.3Co_1-xFe_xO₃ Catalyst

MAAi-Jing¹, WANG Shao-Zeng¹, ZOU Hong-Hu¹, MENG Ming¹, LI Zhi-Jun², BAO Jun³, LI Xin-Gang¹

1. Tianjin Key Laboratory of Applied Catalysis Science & Technology, School of Chemical Engineering & Technology, Tianjin University, Tianjin 300072, P. R. China;
2. State Key Laboratory of Engines, Tianjin University, Tianjin 300072, P. R. China;
3. National Synchrotron Radiation Laboratory, University of Science & Technology of China, Hefei 230029, P. R. China

Received:2012-01-16 Revised:2012-03-31 Published:2012-05-17
Contact: LI Xin-Gang E-mail:xingang_li@tju.edu.cn
Supported by:
The project was supported by the National Natural Science Foundation of China (20806056, U1162103), National High Technology Research and Development Program of China (863 project) (2008AA06Z323), Natural Science Foundation of Tianjin, China (11JCYBJC03700), Program for New Century Excellent Talents in University of China (NCET-10-0615), Scientific Research Foundation for the Returned Overseas Chinese Scholars, State Education Ministry (2011-1568), and State Key Laboratory of Engines, Tianjin University, China (K2012-05).

摘要/Abstract

摘要： 采用溶胶-凝胶法通过在静态空气中700 °C 焙烧制备了不同Fe 掺杂量的La_0.7Sr_0.3Co_1-xFe_xO₃ (x=0,0.2, 0.6, 1.0)系列钙钛矿催化剂. 考察了Fe掺杂量对催化剂的结构、氮氧化物储存、抗硫及再生性能的影响. 研究结果表明: 在La_0.7Sr_0.3CoO₃钙钛矿B位用Fe部分取代Co, 可有效提高SrCO₃物相的分散, X射线衍射(XRD)结果显示样品中基本为钙钛矿物相. 随着Fe掺杂量的增加, 催化剂的NO_x储存量(NSC)下降. 对预硫化样品进行NO_x储存测试, 发现La_0.7Sr_0.3CoO₃催化剂由于表面沉积了硫酸盐, 同时钙钛矿结构也遭到了部分破坏, 使得NO_x储存量和NO氧化能力均大幅度下降, NO_x储存量下降了64.2%, NO-to-NO₂转化率从72.8%降至43.4%.掺杂Fe元素后, 催化剂的抗硫性能都有不同程度的提高, 特别是Fe掺杂量为60%的样品具有最佳的抗硫性能和可再生性能. 与新鲜样品相比较, 再生后样品的NO_x储存量仅下降16.6%, 而NO-to-NO₂转化率为69.1%, 几乎与新鲜样品相同.

关键词: 稀燃, 氮氧化物, 储存, 钙钛矿, 抗硫, 再生, La_0.7Sr_0.3Co_1-xFe_xO₃

Abstract: In this paper, a series of La_0.7Sr_0.3Co_1-xFe_xO₃ (x=0, 0.2, 0.6, and 1.0) catalysts was synthesized by a sol-gel method with calcination at 700 °C in static air. The effect of the Fe doping on the structure, the performance of the NO_x storage, sulfur tolerance and regeneration of the perovskite catalysts was investigated. Our results showed that the partial substitution of Co with Fe improved the depersion of the SrCO₃ phase, and that the perovskite phase became the only species detected from the X-ray diffraction (XRD) patterns. The NO_x storage capacity (NSC) of the catalysts dropped following an increase in the proportion of Fe doping. The deposition of sulfate on the surface and the partial structural damage of the La_0.7Sr_0.3CoO₃ catalyst led to a dramatic reduction in the NSC and the NO oxidation capacity after the sulfation treatment: the NSC being reduced by 64.2%, and the conversion of NO-to-NO₂ falling to 43.4% from 72.8%. The sulfur tolerance of the perovskite catalyst, however, was improved after doping with Fe at the B sites of the La_0.7Sr_0.3CoO₃ catalyst. Of all of these catalysts, the perovskite with 60% of Fe doping (the Fe60 sample) gave the best performance for sulfur tolerane properties and regeneration ability. The NSC of the Fe60 sample was reduced by only 16.6%, and the NO-to-NO₂ conversion reached the value almost similar to that of the fresh sample (i.e. 69.1%).

Key words: Lean-burn, NO_x, Storage, Perovskite, Sulfur tolerance, Regeneration, La_0.7Sr_0.3Co_1-xFe_xO₃

马爱静, 王绍增, 邹鸿鹄, 孟明, 李志军, 鲍骏, 李新刚. La_0.7Sr_0.3Co_1-xFe_xO₃催化剂氮氧化物储存及抗硫性能[J]. 物理化学学报, 2012, 28(06), 1474-1480. doi: 10.3866/PKU.WHXB201203311

MAAi-Jing, WANG Shao-Zeng, ZOU Hong-Hu, MENG Ming, LI Zhi-Jun, BAO Jun, LI Xin-Gang. The Performance of the NO_x Storage Capacity and Sulfur Tolerance of the La_0.7Sr_0.3Co_1-xFe_xO₃ Catalyst[J]. Acta Phys. -Chim. Sin. 2012, 28(06), 1474-1480. doi: 10.3866/PKU.WHXB201203311

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201203311

https://www.whxb.pku.edu.cn/CN/Y2012/V28/I06/1474

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La_0.7Sr_0.3Co_1-xFe_xO₃催化剂氮氧化物储存及抗硫性能

The Performance of the NO_x Storage Capacity and Sulfur Tolerance of the La_0.7Sr_0.3Co_1-xFe_xO₃ Catalyst

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