The Active Sites of a Rod-Shaped Hollandite DeNOx Catalyst.

Abstract

The identification of catalytically active sites (CASs) in heterogeneous catalysis is of vital importance to design and develop improved catalysts, but remains a great challenge. The CASs have been identified in the low-temperature selective catalytic reduction of nitrogen oxides by ammonia (SCR) over a hollandite manganese oxide (HMO) catalyst with a rod-shaped morphology and one-dimensional tunnels. Electron microscopy and synchrotron X-ray diffraction determine the surface and crystal structures of the one-dimensional HMO rods closed by {100} side facets and {001} top facets. A combination of X-ray absorption spectra, molecular probes with potassium and nitric oxide, and catalytic tests reveals that the CASs are located on the {100} side facets of the HMO rods rather than on the top facets or in the tunnels, and hence semi-tunnel structural motifs on the {100} facets are evidenced to be the CASs of the SCR reaction. This work paves the way to further investigate the intrinsic mechanisms of SCR reactions.