Trimetallic FeNiCu Atomic Clusters Supported on Carbon Matrix: Highly Active Catalysts for C3H6-SCR of NO

ACS Appl Mater Interfaces. 2024 Nov 18. doi: 10.1021/acsami.4c11698. Online ahead of print.

Abstract

C3H6-SCR denitrification technology faces catalyst deactivation problems and low catalytic performance at medium-low temperatures. This study utilized the intermetallic synergies to prepare atomic cluster catalysts (FeNiCu/NC) by anchoring Fe-Ni-Cu on a carbon matrix to enhance the C3H6-SCR performance at medium-low temperatures. The synergistic effect of the Fe-Ni-Cu is reflected in the differences in the physicochemical properties of the catalysts, which is proved by several characterization techniques. Results showed that the FeNiCu/NC catalyst had a larger surface area (541.4 m2/g) and there were no metal oxides on the surface of the catalyst but abundant defective sites that anchored Fe/Ni/Cu atoms through N atoms to form M-Nx active sites and atomic clusters. The hollow carbon morphology provides sufficient active sites for C3H6-SCR. The coordination environments of active sites were M-Nx-C, Fe2/FeCu2/FeNi2, Ni3/NiFe/NiCu2, and Cu4/CuFe2/CuNi2, where the synergistic action of trimetal leads to the presence of Fe-Ni-Cu-Nx-C. The synergistic action of the Fe-Ni-Cu significantly improved the C3H6-SCR performance at medium-low temperatures. The FeNiCu/NC exhibited an 81% NO conversion at 150 °C under 2% O2, 15% and 20% higher than FeNi/NC and FeCu/NC catalysts, respectively. Even at 4% O2, the FeNiCu/NC catalyst was active to remove 78% NO and achieve a 93% N2 selectivity at 150 °C and maintained a 100% NO conversion at 300-425 °C. The DRIFTS results demonstrated that NO and C3H6 could combine with active O at metal cluster, M-Nx, or defective oxygen sites to produce various intermediate species, wherein acetates and nitrates were the main active intermediates. Based on the DRIFTS results, a reaction pathway for C3H6-SCR over the FeNiCu/NC catalyst was proposed.

Keywords: C3H6−SCR; FeNiCu/NC catalyst; NO; metal atomic clusters; synergistic effect.