Issue 21, 2024

Modulation of active metal species in MOF-derived catalysts for efficient NO reduction by CO

Abstract

Transition metal oxides are frequently used as catalysts for NO selective catalytic reduction by CO (CO-SCR), but their catalytic activity is limited by the content of active metal species, the lower surface area, and the underdeveloped pore structure. Herein, we prepared three MOF-derived materials (Cu/C, Cu-CuOx/C, and CuO/C), in which active copper species (Cu0, Cu+, and Cu2+), specific surface areas, and porosity were modulated through different heat treatment conditions. Moreover, these composite materials can be used as efficient catalysts for CO-SCR. In particular, it is demonstrated that the Cu/C catalysts containing only Cu0 species could exhibit 100% NO conversion from 350 °C to 500 °C, nearly 100% N2 selectivity, and devoid of any by-product N2O generation. Cu/C is one of the best MOF-derived catalysts reported to date. Thermal catalytic experiments revealed that the occupancies of reductive copper species (Cu0) showed a positive correlation with the materials' catalytic activity. In situ FTIR and DFT analysis elucidated that Cu/C catalysts with Cu0 as the active site have lower activation energy and higher energy gain. The high catalytic activity of Cu/C is attributed to the fact that its Cu0 species has low activation energy and a low reaction energy barrier in the ONNO dissociation step, which is always the decisive step in CO-SCR, and thus this makes the Cu/C catalysts more susceptible to CO-SCR reactions in the range of the conversion temperature. This work provides a new strategy to modulate the ratio of active metal species, specific surface area, and pore structure of CO-SCR catalysts, which can exhibit high catalytic activity.

Graphical abstract: Modulation of active metal species in MOF-derived catalysts for efficient NO reduction by CO

Supplementary files

Article information

Article type
Paper
Submitted
16 Feb 2024
Accepted
18 Apr 2024
First published
18 Apr 2024

J. Mater. Chem. A, 2024,12, 12524-12532

Modulation of active metal species in MOF-derived catalysts for efficient NO reduction by CO

N. Zhou, Z. Yang, Y. Tang, M. Zhang, Y. Zha, M. Liu, F. Yu and J. Liu, J. Mater. Chem. A, 2024, 12, 12524 DOI: 10.1039/D4TA01075B

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