Jump to main content
Jump to site search


Interfacial electronic effects of palladium nanocatalysts on the by-product ammonia selectivity during nitrite catalytic reduction

Author affiliations

Abstract

Catalytic denitrification is an emerging technology that can remove nitrate and nitrite from water. However, the undesirable formation of ammonia requires further suppression. By preparing three types of Pd-based nanocatalysts with different electronic structures as model catalysts, we demonstrate the interfacial electronic effects induced by ethanol (EtOH) and 1-dodecanethiol (C12T) modifications on the selectivity of nitrite catalytic reduction. XPS and in situ DRIFTS spectral characterization studies illustrate that the electron density of the Pd surface atoms increased with the ethanol modification and decreased with the 1-dodecanethiol modification. The nitrite reduction results show that the Pd–EtOH@MIL-101 catalyst (Pdδ) exhibited an unexpectedly low ammonia selectivity of 0.31%, while a higher value of 10.18% was obtained for the Pd–C12T@MIL-101 catalyst (Pdδ+), which indicated that the electronic structure of Pd can control the ammonia selectivity during the nitrite reduction. Thermodynamics studies revealed that increasing the electron density of the Pd surface atoms reduced the nitrite reaction activation energy and changed the reaction pathways, which resulted in a significant decrease in the ammonia selectivity. The results in this paper may provide new insight into designing and optimizing Pd-based catalysts with low ammonia selectivity for nitrate and nitrite catalytic reduction.

Graphical abstract: Interfacial electronic effects of palladium nanocatalysts on the by-product ammonia selectivity during nitrite catalytic reduction

Back to tab navigation

Supplementary files

Publication details

The article was received on 28 Sep 2017, accepted on 21 Nov 2017 and first published on 21 Nov 2017


Article type: Paper
DOI: 10.1039/C7EN00909G
Citation: Environ. Sci.: Nano, 2018, Advance Article
  •   Request permissions

    Interfacial electronic effects of palladium nanocatalysts on the by-product ammonia selectivity during nitrite catalytic reduction

    Z. Zhang, W. Shi, W. Wang, Y. Xu, X. Bao, R. Zhang, B. Zhang, Y. Guo and F. Cui, Environ. Sci.: Nano, 2018, Advance Article , DOI: 10.1039/C7EN00909G

Search articles by author

Spotlight

Advertisements