Operando X-ray absorption experiments and density functional theory (DFT) calculations are reported that elucidate the role of copper redox chemistry in the selective catalytic reduction (SCR) of NO over Cu-exchanged SSZ-13. Catalysts prepared to contain only isolated, exchanged Cu(II) ions evidence both Cu(II) and Cu(I) ions under standard SCR conditions at 473 K. Reactant cutoff experiments show that NO and NH3 together are necessary for Cu(II) reduction to Cu(I).
View Article and Find Full Text PDFWe describe the use of vitreous carbon as an improved reactor material for an operando X-ray absorption spectroscopy (XAS) plug-flow reactor. These tubes significantly broaden the operating range for operando experiments. Using selective catalytic reduction (SCR) of NO(x) by NH(3) on Cu/Zeolites (SSZ-13, SAPO-34 and ZSM-5) as an example reaction, we illustrate the high-quality XAS data achievable with these reactors.
View Article and Find Full Text PDFThe turn-over-rate (TOR) for the water gas shift (WGS) reaction at 200 degrees C, 7% CO, 9% CO(2), 22% H(2)O, 37% H(2) and balance Ar, of 1.4 nm Au/Al(2)O(3) is approximately 20 times higher than that of 1.6 nm Pt/Al(2)O(3).
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