Chemical deactivation of Cu-SAPO-18 deNOx catalyst caused by basic inorganic contaminants in diesel exhaust

doi:10.1016/S1872-2067(19)63312-7

Chinese Journal of Catalysis ›› 2019, Vol. 40 ›› Issue (4): 590-599.DOI: 10.1016/S1872-2067(19)63312-7

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Chemical deactivation of Cu-SAPO-18 deNO_x catalyst caused by basic inorganic contaminants in diesel exhaust

Shujun Ming^a, Lei Pang^b, Chi Fan^a, Wen Guo^a, Yahao Dong^a, Peng Liu^a, Zhen Chen^a, Tao Li^a

a Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China;
b DongFeng Trucks R & D Center, Wuhan 430056, Hubei, China

Received:2018-11-19 Revised:2019-01-11 Online:2019-04-18 Published:2019-03-14
Supported by:
This work was supported by the National Natural Science Foundation of China (21473064).

Abstract

Abstract:

Contaminants (K, Na, Ca, and Mg) were introduced into Cu-SAPO-18 via incipient wetness impregnation to investigate their effect on the selective catalytic reduction of NO_x with NH₃ (NH₃-SCR) over Cu-SAPO-18. After the introduction of contaminants into Cu-SAPO-18, the quantity of acidic sites and Cu²⁺ species in catalyst decreases owing to the replacement of H⁺ and Cu²⁺ by K⁺, Na⁺, Ca²⁺, and Mg²⁺. Furthermore, the loss of isolated Cu²⁺ induces the generation of CuO and CuAl₂O₄-like phases, which causes further loss in the Brunauer-Emmett-Teller surface area of the catalyst. Consequently, the deNO_x performance of the contaminated Cu-SAPO-18 catalysts drops. Such decline in NH₃-SCR performance becomes more pronounced by increasing the contaminant contents from 0.5 to 1.0 mmol/g_catal. In addition, the deactivation influence of the contaminants on Cu-SAPO-18 is presented in the order of K > Na > Ca > Mg, which is consistent with the order of reduction of acidic sites. To a certain degree, the effect of the acidic sites on the deactivation of Cu-SAPO-18 might be more significant than that of isolated Cu²⁺ and the catalyst framework. Moreover, kinetic analysis of NH₃-SCR was conducted, and the results indicate that there is no influence of contaminants on the NH₃-SCR mechanism.

Key words: Cu-SAPO-18 catalyst, Basic inorganic contaminant, Selective catalytic reduction of NO_x with NH₃, Acidic site, Isolated Cu²⁺

Shujun Ming, Lei Pang, Chi Fan, Wen Guo, Yahao Dong, Peng Liu, Zhen Chen, Tao Li. Chemical deactivation of Cu-SAPO-18 deNO_x catalyst caused by basic inorganic contaminants in diesel exhaust[J]. Chinese Journal of Catalysis, 2019, 40(4): 590-599.

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Chemical deactivation of Cu-SAPO-18 deNO_x catalyst caused by basic inorganic contaminants in diesel exhaust

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