Catalysis and In Situ Studies of Rh1/Co3O4 Nanorods in Reduction of NO with H2

Abstract

Efficient use of precious metal atoms in heterogeneous catalysis is important in chemical transformation and environmental remediation. Co 3 O 4 with singly dispersed Rh atoms, Rh 1 /Co 3 O 4, was synthesized for reduction of nitric oxide with hydrogen. Studies using extended X-ray absorption fine structure (EXAFS) showed that the singly dispersed Rh atoms are bonded to surface oxygen atoms before catalysis. In situ studies using ambient pressure X-ray photoelectron spectroscopy (AP-XPS), EXAFS, and X-ray Absorption Near Edge Structure (XANES) suggested that the surface of Rh 1 /Co 3 O 4 with singly dispersed Rh atoms is restructured into a new geometry at 220 °C in the mixture of reactant gases (NO and H 2 ). It forms RhCo n nanoclusters singly dispersed in the surface layer of Co 3 O 4 . The restructured catalyst, RhCo n /Co 3 O 4 exhibits a much better catalytic performance in contrast to Rh 1 /Co 3 O 4 without a restructuring. RhCo n /Co 3 O 4 is highly active for reduction of nitric oxide with hydrogen. Selectivity to the production of N 2 at 220 °C is 87% and reaches 97% at 300 °C. In situ studies showed this catalyst maintains its single dispersion of Rh atoms up to 300 °C during catalysis.