Performance of Fe-N/C oxygen reduction electrocatalysts towards NO−₂, NO, and NH₂OH electroreduction from fundamental insights into the active center to a new method for environmental nitrite destruction
File(s)
Published version
Author(s)
Kucernak, A
Malko, D
Lopes, T
Type
Journal Article
Abstract
Although major progress has recently been achieved through ex situ methods, there is still a lack of understanding of the behavior of the active center in non-precious metal Fe–N/C catalysts under operating conditions. Utilizing nitrite, nitric oxide, and hydroxylamine as molecular probes, we show that the active site for the oxygen reduction reaction (ORR) is different under acidic and alkaline conditions. An in-depth investigation of the ORR in acid reveals a behavior which is similar to that of iron macrocyclic complexes and suggests a contribution of the metal center in the catalytic cycle. We also show that this catalyst is highly active toward nitrite and nitric oxide electroreduction under various pH values with ammonia as a significant byproduct. This study offers fundamental insight into the chemical behavior of the active site and demonstrates a possible use of these materials for nitrite and nitric oxide sensing applications or environmental nitrite destruction.
Date Issued
2016-12-14
Date Acceptance
2016-11-13
Citation
Journal of the American Chemical Society, 2016, 138 (49), pp.16056-16068
ISSN
1520-5126
Publisher
American Chemical Society
Start Page
16056
End Page
16068
Journal / Book Title
Journal of the American Chemical Society
Volume
138
Issue
49
Copyright Statement
© 2016 American Chemical Society. ACS AuthorChoice - This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.
Sponsor
Engineering & Physical Science Research Council (EPSRC)
Grant Number
EP/J016454/1
Subjects
Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
Chemistry
MEMBRANE FUEL-CELLS
ACID ELECTROLYTE
CATHODE CATALYST
FE/N/C-CATALYSTS
ELECTROCHEMICAL REDUCTION
METAL ELECTROCATALYST
DISK ELECTRODE
O-2 REDUCTION
OXIDE
CARBON
General Chemistry
03 Chemical Sciences
Publication Status
Published
Date Publish Online
2016-11-13