NH3-SCR reaction mechanisms of NbOx/Ce0.75Zr0.25O2 catalyst: DRIFTS and kinetics studies
Artikel i vetenskaplig tidskrift, 2016

A NbOx/Ce0.75Zr0.25O2 (NbCZ) catalyst was synthesized by a citric acid-aided sol-gel method. It shows that above 80% NOx conversion and above 95% N-2 selectivity for the selective catalytic reduction of NOx by ammonia over this catalyst are achieved in the temperature range 200-450 degrees C. Based on the DRIFTS and kinetic studies over NbCZ and Ce0.75Zr0.25O2, the promotion mechanism by niobia loading was elucidated with an overall reaction pathway. Two different reaction routes, "L-H" mechanism via "NH4NO3 + NO" at low temperatures (<200 degrees C) and "E-R" mechanism via "NH2 + NO" at high temperatures (>350 degrees C), are presented. The niobia addition increases the surface acidity and promotes the formation of nitrates species at low temperatures. In this way, the reaction between the ads-NH3 and nitrates species is accelerated to form NH4NO3 intermediates, which then decompose to N-2 and H2O. The reaction of the ads-NH3 species with gaseous NOx at high temperatures is also promoted due to the enhanced acidity and weakened thermal stability of nitrates after niobia loading.

Mechanism

Niobia modification

CeO2-ZrO2 mixed oxides

DRIFTS

NH3-SCR

Författare

Z. R. Ma

National Institute of Clean-and-Low-Carbon Energy (NICE)

Tsinghua University

X. D. Wu

Tsinghua University

Hanna Härelind

Chalmers, Kemi och kemiteknik, Tillämpad kemi, Teknisk ytkemi

Kompetenscentrum katalys (KCK)

D. Weng

Tsinghua University

B. D. Wang

National Institute of Clean-and-Low-Carbon Energy (NICE)

Z. C. Si

Tsinghua University

Journal of Molecular Catalysis A: Chemical

1381-1169 (ISSN)

Vol. 423 172-180

Drivkrafter

Hållbar utveckling

Styrkeområden

Transport

Materialvetenskap

Ämneskategorier

Fysikalisk kemi

Materialkemi

DOI

10.1016/j.molcata.2016.06.023