三维有序大孔钙钛矿型La1–xKxNiO3催化剂提高炭烟催化燃烧活性:K取代的作用

doi:10.1016/S1872-2067(18)63269-9

催化学报 ›› 2019, Vol. 40 ›› Issue (5): 722-732.DOI: 10.1016/S1872-2067(18)63269-9

三维有序大孔钙钛矿型La_1–xK_xNiO₃催化剂提高炭烟催化燃烧活性:K取代的作用

梅雪垒, 熊靖, 韦岳长, 王楚君, 吴强强, 赵震, 刘坚

中国石油大学(北京)理学院, 重质油加工国家重点实验室, 北京 102249

收稿日期:2018-10-23 修回日期:2018-11-21 出版日期:2019-05-18 发布日期:2019-03-30
通讯作者: 韦岳长
基金资助:
国家自然科学基金（21673142）；移动源排放控制技术国家工程实验室（NELMS2017A05）；中国石油创新基金（2018D–5007–0505）；中国石油大学（北京）科学基金（242017QNXZ02，2462018BJC005）.

Three-dimensional ordered macroporous perovskite-type La_1-xK_xNiO₃ catalysts with enhanced catalytic activity for soot combustion: the Effect of K-substitution

Xuelei Mei, Jing Xiong, Yuechang Wei, Chujun Wang, Qiangqiang Wu, Zhen Zhao, Jian Liu

State Key Laboratory of Heavy Oil Processing, College of Science, China University of Petroleum-Beijing, Beijing 102249, China

Received:2018-10-23 Revised:2018-11-21 Online:2019-05-18 Published:2019-03-30
Contact: 10.1016/S1872-2067(18)63269-9
Supported by:
This work was supported by the National Natural Science Foundation of China (21673142), National Engineering Laboratory for Mobile Source Emission Control Technology (NELMS2017A05), PetroChina Innovation Foundation (2018D-5007-0505), and Science Foundation of China University of Petroleum, Beijing (242017QNXZ02, 2462018BJC005).

摘要/Abstract

摘要：

催化炭烟燃烧的本质是典型的固体（炭烟颗粒）-固体（催化剂）-气体（O₂和NO）三相深度氧化反应.因此炭烟燃烧性能不仅与催化剂的本征活性有关，同时也与催化剂和炭烟颗粒之间的接触效率有关.钙钛矿型（ABO₃）氧化物具有高热稳定性和高催化活性，在钙钛矿型氧化物中A位通常为稀土元素，B位通常为过渡金属元素，钙钛矿的A，B位离子都可以被半径相近的其他元素部分取代，而且物相结构不发生变化.我们组前期研究发现，用碱金属部分取代钙钛矿型氧化物中的A位，可以有效提高其催化活性.同时发现三维有序大孔（3DOM）结构可以有效的增加催化剂与碳烟颗粒的接触效率.基于此，本文利用胶体晶体模板法成功制备了3DOM La_1-xK_xNiO₃钙钛矿型催化剂，并采用SEM，TEM，HRTEM，Elements mapping，XRD，Raman，XPS和H₂-TPR等手段对其物理化学性能进行了表征，进一步探讨K取代对3DOM La_1-xK_xNiO₃催化剂炭烟催化燃烧性能的影响.
SEM和TEM照片显示，制备的3DOM La_1-xK_xNiO₃催化剂孔道三维有序贯通，孔径均一，孔壁厚度均匀，每个大孔下面展示清晰可见的小孔窗，大孔孔径大约为260 nm，这有利于炭烟颗粒在气流的协助下进入催化剂的孔道之内，从而提高炭烟与催化剂之间的接触效率.3DOM结构催化剂具有大的比表面积（24-27 m²g^-1），且K的取代对其比表面积无太大的影响.XRD和Raman谱证实了催化剂的钙钛矿结构，且K能够取代La并进入钙钛矿氧化物的晶格中.XPS和H₂-TPR表征发现，K取代La之后，B位的Ni元素的价态有所提升，表面活性氧物种密度增加，其中3DOM La_0.95K_0.05NiO₃催化剂具有最高的Ni⁴⁺的含量和活性氧含量.3DOM La_1-xK_xNiO₃催化剂展示了高的炭烟燃烧催化性能，且K的取代能够明显促进其催化炭烟燃烧活性.在松散接触条件下，催化剂炭烟催化燃烧活性的顺序为：3DOM La_0.95K_0.05NiO₃ > 3DOM La_0.90K_0.10NiO₃> 3DOM La_0.80K_0.20NiO₃ > 3DOM La_0.99K_0.01NiO₃> 3DOM LaNiO₃ > particle-type LaNiO₃.其中，3DOM La_0.95K_0.05NiO₃催化剂展示了最高的炭烟燃烧催化性能，其T₅₀和S_CO2值分别为338℃和98.2%，这与Pt基催化剂活性相当.另外，对炭烟催化燃烧性能的影响因素进行了探讨：一方面，三维有序大孔结构有效提高催化剂活性；另一方面，K元素的取代提高了Ni的价态，从而提升了表面活性氧物种数量，这对炭烟催化燃烧起着至关重要的作用.

关键词: 三维有序大孔材料, 镍酸镧, 钾, 钙钛矿, 炭烟燃烧

Abstract:

Three-dimensional ordered macroporous (3DOM) La_1-xK_xNiO₃ perovskite-type catalysts were successfully prepared by a colloidal crystal template method and characterized by scanning electron microscopy, transmission electron microscopy, high-resolution transmission electron microscopy, energy-dispersive X-ray scattering elemental mapping, X-ray diffraction, Raman and X-ray photoelectron spectroscopy, and temperature-programmed reduction of H₂. Further, their catalytic activity in soot combustion was determined by temperature-programmed oxidation reaction. K substitution into the LaNiO₃ lattice led to remarkably improved catalytic activity of this catalyst in soot combustion. Amongst various catalysts, La_0.95K_0.05NiO₃ exhibited the highest activity in soot combustion (with its T₅₀ and S_CO₂ values being 338℃ and 98.2%, respectively), which is comparable to the catalytic activities of Pt-based catalysts under the condition of poor contact between the soot and the catalyst. K-substitution improves the valence state of Ni and increases the number of oxygen vacancies, thereby leading to increased density of surface-active oxygen species. The active oxygen species play a vital role in catalyzing the elimination of soot. The perovskite-type La_1-xK_xNiO₃ nanocatalysts with 3DOM structure without noble metals have potential for practical applications in the catalytic combustion of diesel soot particles.

Key words: Three-dimensional ordered, macroporous material, LaNiO₃ Potassium, Perovskite, Soot combustion

梅雪垒, 熊靖, 韦岳长, 王楚君, 吴强强, 赵震, 刘坚. 三维有序大孔钙钛矿型La_1–xK_xNiO₃催化剂提高炭烟催化燃烧活性:K取代的作用[J]. 催化学报, 2019, 40(5): 722-732.

Xuelei Mei, Jing Xiong, Yuechang Wei, Chujun Wang, Qiangqiang Wu, Zhen Zhao, Jian Liu. Three-dimensional ordered macroporous perovskite-type La_1-xK_xNiO₃ catalysts with enhanced catalytic activity for soot combustion: the Effect of K-substitution[J]. Chinese Journal of Catalysis, 2019, 40(5): 722-732.

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三维有序大孔钙钛矿型La_1–xK_xNiO₃催化剂提高炭烟催化燃烧活性:K取代的作用

Three-dimensional ordered macroporous perovskite-type La_1-xK_xNiO₃ catalysts with enhanced catalytic activity for soot combustion: the Effect of K-substitution

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