Copper Doping Promotion on Ce/CAC-CNT Catalysts with High Sulfur Dioxide Tolerance for Low-Temperature NH3–SCR

The stumbling block to the ever-increasing need for improving air quality remains nitrogen oxides (NO x ). The copper-introduced Ce/CAC-CNT (Cu x Ce/CAC-CNTs) catalyst using the in situ-growth-prepared activated carbon and carbon-nanotube composite (CAC-CNT) carrier with high sulfur dioxide toleranc...

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Veröffentlicht in:ACS sustainable chemistry & engineering 2021-01, Vol.9 (2), p.987-997
Hauptverfasser: Yang, Lin, Wang, Pengchen, Yao, Lu, Meng, Xiaomi, Jia, Charles Q, Jiang, Xia, Jiang, Wenju
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Sprache:eng
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Zusammenfassung:The stumbling block to the ever-increasing need for improving air quality remains nitrogen oxides (NO x ). The copper-introduced Ce/CAC-CNT (Cu x Ce/CAC-CNTs) catalyst using the in situ-growth-prepared activated carbon and carbon-nanotube composite (CAC-CNT) carrier with high sulfur dioxide tolerance was successfully applied to low-temperature NH3–SCR in this study. The findings indicate that the Cu x Ce/CAC-CNTs obtained at a 0.2 Cu/Ce molar ratio and the calcination temperature of 450 °C showed the highest 100% NO conversion with 95.8% N2 selectivity at 150 °C and 10 000 h–1. The incorporation of Cu improved the Cu0.2Ce/CAC-CNTs in Lewis acid, lattice oxygen (31.99%), and Ce3+ (26.03%). The accelerated NH3 adsorption on acid sites, the encouraging electron transfer by the Ce4+ + Cu+ ↔ Ce3+ + Cu2+ redox circle, and the more surface chemisorbed oxygen (Oβ) improved the catalytic activity of Cu0.2Ce/CAC-CNTs. The NH3–SCR of Cu0.2Ce/CAC-CNTs largely follows the L–H mechanism, together with a certain degree of “Fast SCR.” The added Cu species effectively prevented surface SO2 adsorption and oxidation, and the Cu0.2Ce/CAC-CNTs restored more than 94% SCR activity after 8 h of poisoning in 50 ppm SO2 and 5 vol % H2O.
ISSN:2168-0485
2168-0485
DOI:10.1021/acssuschemeng.0c08490