Interpretation of NH 3 -TPD Profiles from Cu-CHA Using First-Principles Calculations
Journal article, 2019

Temperature-programmed desorption (TPD) with ammonia is widely used for zeolite characterization revealing information on acidity and adsorption sites. The interpretation of TPD measurements is, however, often challenging. One example is the NH 3 -TPD profile from Cu-chabazite (Cu-CHA) which generally is deconvoluted in three peaks with contributions from NH 3 on Lewis acid sites, copper sites and Brønsted acid sites. Here, we use density functional theory calculations combined with kinetic simulations to analyze this case. We find a large number of possible species, giving rise to overlapping features in the NH 3 -TPD. The experimental low-temperature peak (below 200∘C) is assigned to NH 3 desorption from Lewis acid sites together with NH 3 desorption from a [Cu(II)(OH)(NH3)3]+ complex. The intermediate-temperature peak (250-350∘C) is attributed to decomposition of a linear [Cu(I)(NH3)2]+ complex and a residual from [Cu(II)(OH)(NH3)3]+. The high-temperature peak is predicted to have contributions from Brønsted acid sites (NH4+), [Cu(I)NH3]+ and [Cu(II)(NH3)4]2+. The present work shows that NH 3 -TPD from Cu-CHA can be reconciled with copper complexes as NH 3 storage sites.

Cu-CHA

Zeolites

Acidity

NH -TPD 3

Author

Lin Chen

Chalmers, Physics, Chemical Physics

Ton Janssens

Umicore

Magnus Skoglundh

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry, Polymer Technology

Henrik Grönbeck

Chalmers, Physics, Chemical Physics

Topics in Catalysis

1022-5528 (ISSN) 1572-9028 (eISSN)

Vol. 62 1-4 93-99

Subject Categories

Inorganic Chemistry

Theoretical Chemistry

Organic Chemistry

DOI

10.1007/s11244-018-1095-y

More information

Latest update

7/12/2019