Citation: FAN Feng-Qi, MENG Ming, TIAN Ye, ZHENG Li-Rong, ZHANG Jing, HU Tian-Dou. Effect of Cu Loading on the Structure and Catalytic Performance of the LNT Catalyst CuO-K₂CO₃/TiO₂[J]. Acta Physico-Chimica Sinica, ;2015, 31(9): 1761-1770. doi: 10.3866/PKU.WHXB201507291 shu

Effect of Cu Loading on the Structure and Catalytic Performance of the LNT Catalyst CuO-K₂CO₃/TiO₂

1.
1 Collaborative Innovation Center of Chemical Science and Engineering Tianjin, Tianjin Key Laboratory of Applied Catalysis Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, P. R. China;
2 Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, P. R. China

Received Date: 17 April 2015
Available Online: 29 July 2015
Fund Project: 国家自然科学基金(21276184, U1332102, 21476160) (21276184, U1332102, 21476160) 高等学校博士学科点专项科研基金(20120032110014) (20120032110014) 天津市自然科学基金(12JCYBJC14000, 15JCZDJC37400) (12JCYBJC14000, 15JCZDJC37400)中国大学学科人才引进计划(B06006)资助 (B06006)

A series of non-platinic lean NO_x trap (LNT) CuO-K₂CO₃/TiO₂ catalysts with different Cu loadings were prepared by sequential impregnation, and they showed relatively od performance for lean NO_x storage and reduction. The catalyst containing 8% (w) CuO showed not only the largest NO_x storage capacity of 1.559 mmol·g^-1 under lean conditions, but also the highest NO_x reduction percentage of 99% in cyclic lean/rich atmospheres. Additionally, zero selectivity of NO_x to N₂O was achieved over this catalyst during NO_x reduction. Multiple techniques, including X-ray diffraction (XRD), high-resolution transmission electron microscopy (HR-TEM), temperature-programmed desorption of CO₂ (CO₂-TPD), extended X-ray absorption fine structure (EXAFS), temperature-programmed reduction of H₂ (H₂-TPR), and in-situ diffuse reflectance Fourier-transform infrared spectroscopy (DRIFTS), were used for catalyst characterization. The results indicate that highly dispersed CuO is the main active phase for oxidation of NO to NO₂ and reduction of NO_x to N₂. The strong interaction between K₂CO₃ and CuO was clearly revealed, which favors NO_x adsorption and storage. The appearance of negative bands at around 1436 and 1563 cm^-1, corresponding to CO₂ asymmetric stretching in bicarbonates and -C=O stretching in bidentate carbonates, showed the involvement of carbonates in NO_x storage. After using the catalysts for 15 cycles of NO_x storage and reduction in alternative lean/rich atmospheres, the CuO species in the catalysts showed little change, indicating high catalytic stability. Based on the results of in-situ DRIFTS and the other characterizations, a model describing the NO_x storage processes and the distribution of CuO and K₂CO₃ species is proposed.
- NO_x,
- Storage,
- Reduction,
- Copper oxide,
- Potassium carbonate
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Effect of Cu Loading on the Structure and Catalytic Performance of the LNT Catalyst CuO-K2CO3/TiO2

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通讯作者: 陈斌, bchen63@163.com

Effect of Cu Loading on the Structure and Catalytic Performance of the LNT Catalyst CuO-K₂CO₃/TiO₂