La0.7Sr0.3CoO3-δ钙钛矿催化剂表征及其催化氧化碳黑性能研究

方乐; 虞敬; 郭冠伦

La_0.7Sr_0.3CoO_3-δ钙钛矿催化剂表征及其催化氧化碳黑性能研究

方乐^{1, 2},
虞敬^{1, 2},
郭冠伦^{1, 2, ,}

1.
武汉理工大学现代汽车零部件技术湖北省重点实验室, 湖北武汉 430070
2.
武汉理工大学汽车零部件技术湖北省协同创新中心, 湖北武汉 430070

详细信息

中图分类号: TQ426.83
计量
- 文章访问数: 120
- HTML全文浏览量: 41
- PDF下载量: 11
- 被引次数: 0
出版历程
- 收稿日期: 2020-04-03
- 修回日期: 2020-05-22
- 网络出版日期: 2021-01-23
- 刊出日期: 2020-06-10

Study on the characterization of La_0.7Sr_0.3CoO_3-δ perovskite catalyst and its catalytic performance for carbon black oxidation

FANG Le^{1, 2},
YU Jing^{1, 2},
GUO Guan-lun^{1, 2
, ,}

1.
Hubei Key Laboratory of Advanced Technology for Automotive Components, Wuhan University of Technology, Wuhan 430070, China
2.
Hubei Collaborative Innovation Center for Automotive Components Technology, Wuhan University of Technology, Wuhan 430070, China

More Information

Corresponding author: GUO Guan-lun, E-mail: glguo@whut.edu.cn

摘要

摘要: 为了研究La_0.7Sr_0.3CoO_3-δ钙钛矿催化剂对碳黑的催化氧化过程，本研究通过研究催化剂和碳黑的两种不同接触方式，即紧密接触与松散接触，讨论了其对碳黑催化氧化过程的影响。结果表明，与松散接触和无催化剂接触条件相比，紧密接触条件下碳黑的t_ig（起燃温度）分别下降了89.5和157.4℃，同时随着催化剂/碳黑的比例增加，碳黑氧化的t_ig、t_m（最大转化温度）、t_f（燃净温度）均向低温区域移动，表明该催化剂对碳黑有着良好的催化氧化性能。
- La_0.7Sr_0.3CoO_3-δ型钙钛矿 /
- 碳黑氧化 /
- 接触方式
Abstract: In order to study the catalytic oxidation process of carbon black over La_0.7Sr_0.3CoO_3-δ perovskite catalyst, two different contact modes of the catalyst and carbon black were designed, namely intimate contact and loose contact, and used to observe the reaction behavior. The results showed that the t_ig (light-off temperature) of carbon black decreased by 89.5 and 157.4℃ under intimate contact conditions compared with the loose contact and no catalyst contact conditions. Meanwhile, as the ratio of catalyst/carbon black increased, the t_ig, t_m (maximum conversion temperature) and t_f (burn-up temperature) of the carbon black all shifted to the low temperature, indicating that the catalyst had good catalytic performance for carbon black oxidation.
- La_0.7Sr_0.3CoO_3-δ perovskite /
- carbon black oxidation /
- contact mode

HTML全文

下载: 全尺寸图片幻灯片

图 1 活性测试装置示意图

Figure 1 Schematic diagram of the activity test device

下载: 全尺寸图片幻灯片

图 2 La_0.7Sr_0.3CoO_{3- δ} 粉末的XRD谱图

Figure 2 XRD patterns of the La_0.7Sr_0.3CoO_{3- δ} powder

下载: 全尺寸图片幻灯片

图 3 催化剂Co 2p的XPS谱图

Figure 3 XPS spectrum of Co 2p of the catalyst

下载: 全尺寸图片幻灯片

图 4 催化剂O 1s的XPS谱图

Figure 4 XPS spectrum of O 1s of the catalyst

下载: 全尺寸图片幻灯片

图 5 催化剂的H₂-TPR谱图

Figure 5 H₂-TPR profile of the catalyst

下载: 全尺寸图片幻灯片

图 6 催化剂的O₂-TPD谱图

Figure 6 O₂-TPD profile of the catalyst

下载: 全尺寸图片幻灯片

图 7 在松/紧接触和无催化剂下碳黑的燃烧活性

Figure 7 Combustion activity of carbon black in loose/intimate contact and no catalyst

下载: 全尺寸图片幻灯片

图 8 在不同混合比下出口CO₂生成量

Figure 8 CO₂ concentration at outlet under different mixing ratios

下载: 全尺寸图片幻灯片

图 9 在不同混合比下碳黑燃烧的特征温度

Figure 9 Characteristic temperature of carbon black combustion under different mixing ratios

下载: 全尺寸图片幻灯片

表 1 松/紧接触以及无催化作用下的特征温度值

Table 1 Characteristic temperature values of loose/intimate contact and no catalyst

Catalytic conditions	t_ig /℃	t_m /℃	t_f /℃
Tight contact	367.0	495.6	608.4
Loose contact	456.5	587.8	687.1
No catalyst	524.4	660.5	750.0

下载: 导出CSV

参考文献(18)

[1]	张翠平, 王铁.内燃机排放与控制[M].北京:机械工业出版社, 2013. ZHANG Cui-ping, WANG Tie. Emission and Control of Internal Combustion Engine[M]. Beijing:Chin Mach Press, 2013.
[2]	GUAN B, ZHAN R, LIN H, HUANG Z. Review of the state-of-the-art of exhaust particulate filter technology in internal combustion engines[J]. J Environ Manage, 2015, 154:225-258. doi: 10.1016/j.jenvman.2015.02.027
[3]	WANG H, LIU J, ZHAO Z, WEI Y C, XU C M. Comparative study of nanometric Co-, Mn- and Fe-based perovskite-type complex oxide catalysts for the simultaneous elimination of soot and NO_x from diesel engine exhaust[J]. Catal Today, 2012, 184(1):288-300. doi: 10.1016/j.cattod.2012.01.005
[4]	GALENDA A, NATILE M M, KRISHNAN V, BERTAGNOLLI H, GLISENTI A. LaSrCoFeO and Fe₂O₃/LaSrCoFeO powders:Synthesis and characterization[J]. Chem Mater, 2007, 19(11):2796-2808. doi: 10.1021/cm062742i
[5]	TANAKA H, MIZUNO N, MISONO M. Catalytic activity and structural stability of La_0.9Ce_0.1Co_1-xFexO₃ perovskite catalysts for automotive emissions control[J]. Appl Catal A:Gen, 2003, 244(2):371-382. doi: 10.1016/S0926-860X(02)00609-9
[6]	NAKAMURA T, MISONO M, YONEDA Y. Catalytic properties of perovskite-type mixed oxides, La_1-xSr_xCoO₃[J]. Chem Inform, 1982, 55(2):394-399. doi: 10.1246-bcsj.55.394/
[7]	URÁN L, GALLEGO J, LI W Y, SANTAMARIA A. Effect of catalyst preparation for the simultaneous removal of soot and NO_x[J]. Appl Catal A:Gen, 2019, 569:157-169. doi: 10.1016/j.apcata.2018.10.029
[8]	TERAOKA Y, NAKANO K, SHANGGUAN W F, KAGAWA S. Simultaneous catalytic removal of nitrogen oxides and diesel soot particulate over perovskite-related oxides[J]. Catal Today, 1996, 27(1/2):107-113. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=a25b4aa924d0532178439f31d27ca8b2
[9]	WANG X Y, HUANG K K, MA W, CONG Y G, GE C D, FENG S H. Defect engineering, electronic structure, and catalytic properties of perovskite oxide La_0.5Sr_0.5CoO_3-δ[J]. Chem-A Eur J, 2017, 23(5):1093-1100. doi: 10.1002/chem.201604065
[10]	WANG X Y, HUANG K K, QIAN J Y, CONG Y G, GE C D, FENG S H. Enhanced CO catalytic oxidation by Sr reconstruction on the surface of La_xSr_1-xCoO_3-δ[J]. Sci Bull, 2017, 62(9):658-664. doi: 10.1016/j.scib.2017.03.017
[11]	YANG J, HU S Y, FANG Y R, HOANG S, LI L, YANG W W, LIANG Z F, WU J, HU J P, XIAO W, PAN C Q, LUO Z, DING J, ZHANG L Z, GUO Y B. Oxygen vacancy promoted O₂ activation over perovskite oxide for low-temperature CO oxidation[J]. ACS Catal, 2019, 9(11):9751-9763. doi: 10.1021/acscatal.9b02408
[12]	XIAO P, ZHU J J, LI H L, JIANG W, WANG T, ZHU Y J, ZHAO Y X, LI J L. Effect of textural structure on the catalytic performance of LaCoO₃ for CO oxidation[J]. ChemCatChem, 2014, 6(6):1774-1781. doi: 10.1002/cctc.201402064
[13]	高永华.钙钛矿型复合氧化物催化剂的制备及其在环境催化中的应用[D].太原: 太原理工大学, 2017. GAO Yong-hua. Preparation of Perovskite Composite oxide catalyst and its application in environmental catalysis[D]. Taiyuan: Taiyuan University of Techndogy, 2017.
[14]	ONRUBIA J A, PEREDA-AYO B, DE-LA-TORRE U, GONZALEZ-VWLASCO J R. Key factors in Sr-doped LaBO₃ (B=Co or Mn) perovskites for NO oxidation in efficient diesel exhaust purification[J]. Appl Catal B:Environ, 2017, 213:198-210. doi: 10.1016/j.apcatb.2017.04.068
[15]	HERNÁNAEZ W Y, TSAMPAS M N, ZHAO C, BOREAVE A, BOSSELET F, VERMOUX P. La/Sr-based perovskites as soot oxidation catalysts for Gasoline Particulate Filters[J]. Catal Today, 2015, 258:525-534. doi: 10.1016/j.cattod.2014.12.021
[16]	MERINO N A, BARBERO B P, GRANGE P, CADUS L E. LaCaCoO perovskite-type oxides:preparation, characterisation, stability, and catalytic potentiality for the total oxidation of propane[J]. J Catal, 2005, 231(1):232-244. https://www.researchgate.net/publication/222142014_La1-xCaxCoO3_perovskite-type_oxides_Preparation_characterisation_stability_and_catalytic_potentiality_for_the_total_oxidation_of_propane
[17]	明彩兵, 叶代启, 易慧, 周遗品. Pt取代的LaCoO₃催化氧化碳烟的研究[J].仲恺农业工程学院学报, 2009, 22(1):20-23. doi: 10.3969/j.issn.1674-5663.2009.01.006 MING Cai-bing, YE Dai-qi, YI Hui, ZHOU Yi-pin. Study on Pt-substituted LaCoO₃ catalytic oxidation of soot[J]. J Zhongkai Univ Agr Eng, 2009, 22(1):20-23. doi: 10.3969/j.issn.1674-5663.2009.01.006
[18]	BUENO-LOPEZ A, KRISHNA K, MAKKEE M, MOULIJN J A. Enhanced soot oxidation by lattice oxygen via La³⁺-doped CeO₂[J]. J Catal, 2005, 230(1):237-248. https://www.researchgate.net/publication/223019608_Enhanced_soot_oxidation_by_lattice_oxygen_via_La3-doped_CeO2