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Selective catalytic oxidation of ammonia over nano Cu/zeolites with different topologies

Wang, H; Zhang, R; Liu, Y; Li, P; Chen, H; Wang, FR; Teoh, WY; (2020) Selective catalytic oxidation of ammonia over nano Cu/zeolites with different topologies. Environmental Science: Nano , 7 (5) pp. 1399-1414. 10.1039/d0en00007h. Green open access

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Abstract

The selective catalytic oxidation of ammonia (NH3-SCO) is the last mitigation step in exhaust treatment using a 4-way catalytic converter to convert any excess and unreacted NH3 (that was used as a reductant of NOx) into environmentally benign N2 and H2O. Here, we report a series of highly reactive and selective nano Cu/zeolites for the NH3-SCO reaction. The NH3-SCO activity was found in the order nano Cu/ZSM-5 (MFI topology) > Cu/Beta (BEA) > Cu/MCM-49 (MWW) > Cu/Y (FAU) > Cu/Mordenite (MOR) > Cu/Ferrierite (FER). The best catalyst, i.e., nano Cu/ZSM-5, achieves 98% NH3 conversion at 250 °C with the N2 yield maintained at >98% even at up to 500 °C. When assessed under practical exhaust conditions in the presence of moisture (5% H2O) as well as that after hydrothermal aging (5% H2O, 850 °C, 8 h), the nano Cu/ZSM-5 exhibited only minor deactivation as a result of its good retention of Cu dispersion, pore structure and specific surface area. Furthermore, small micropore (10-membered ring, 10-MR) topologies were found to be crucial in maintaining high N2 yields. For Cu/Y and Cu/Mordenite, composed of 12-MR pores that are non-interconnected with smaller pores, their N2 yields were compromised by forming NOx at temperatures above 400 °C. Based on the in situ DRIFTS study, the iSCR mechanism appears to be applicable for all fresh and aged Cu/zeolites with the exception of fresh Cu/MCM-49 that follows the imide mechanism.

Type: Article
Title: Selective catalytic oxidation of ammonia over nano Cu/zeolites with different topologies
Open access status: An open access version is available from UCL Discovery
DOI: 10.1039/d0en00007h
Publisher version: https://doi.org/10.1039/d0en00007h
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery.ucl.ac.uk/id/eprint/10101750
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