In-situ studies of oxidation/reduction of copper in Cu-CHA SCR catalysts: Comparison of fresh and SO2-poisoned catalysts

• SO2-poisoning results in deactivation of Cu-CHA SCR under standard SCR conditions; however regeneration at 700 °C completely restores the SCR performance. To understand the nature of these effects, Cu-species in the fresh and poisoned catalysts were characterized by in-situ temperature-dependent time-resolved Cu K-edge X-ray absorption spectroscopy using the multivariate curve resolution alternating least squares (MCR-ALS) approach and continuous Cauchy wavelet transforms. The extracted chemically-meaningful reference spectra of Cu-species were analyzed by DFT-assisted XANES calculations. Cu-bisulfates were found as the most energetically favorable poisoned Cu-species. The response of Cu-species to a reducing environment differs in the fresh and SO2-poisoned catalysts. Differences in reducibility are related to the formation of quasi-linear Cu-complexes in the SO2-poisoned catalyst formed during heating in H2/He. Heating in H2/He leads to partial desulfurization of the poisoned catalyst. Cooling in H2/He after heating results in more facile formation of Cu-metal clusters in fresh catalyst than in SO2-poisoned.

Ämnesord

NATURVETENSKAP  -- Kemi -- Oorganisk kemi (hsv//swe)

NATURAL SCIENCES  -- Chemical Sciences -- Inorganic Chemistry (hsv//eng)

NATURVETENSKAP  -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)

NATURAL SCIENCES  -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)

NATURVETENSKAP  -- Kemi -- Annan kemi (hsv//swe)

NATURAL SCIENCES  -- Chemical Sciences -- Other Chemistry Topics (hsv//eng)

NATURVETENSKAP  -- Kemi (hsv//swe)

NATURAL SCIENCES  -- Chemical Sciences (hsv//eng)

Nyckelord

NH -SCR 3

regeneration

SO /sulfur poisoning 2

In-situ XANES

Cu-SSZ-13

Publikations- och innehållstyp

art (ämneskategori)

ref (ämneskategori)