Carbon-supported iron complexes as electrocatalysts for the cogeneration of hydroxylamine and electricity in a NO-H2 fuel cell: A combined electrochemical and density functional theory study

Autor: Annick Hubin, Xia Sheng, Ivo F.J. Vankelecom, Kristine Pierloot, Yolanda Alvarez-Gallego, Tzvetan Mihaylov, Xochitl Dominguez-Benetton, Hailiang Zhao, Kitty Baert, Paolo P. Pescarmona
Přispěvatelé: Vrije Universiteit Brussel, Electrochemical and Surface Engineering, Materials and Chemistry, Earth System Sciences, Product Technology
Rok vydání: 2018
Předmět:
OXYGEN REDUCTION
Materials science
Activated carbon
Inorganic chemistry
Energy Engineering and Power Technology
chemistry.chemical_element
GAS-DIFFUSION ELECTRODES
Hydroxylamine
02 engineering and technology
OXIDATION
010402 general chemistry
Electrochemistry
Electrocatalyst
01 natural sciences
NITRIC-OXIDE REDUCTION
NITROGEN-COMPOUNDS
chemistry.chemical_compound
METAL-ELECTRODES
medicine
SCHIFF-BASE COMPLEXES
EXCHANGE-ENERGY
Electrical and Electronic Engineering
Physical and Theoretical Chemistry
FeSalen
Cogeneration of chemical products and electricity
Gas diffusion electrode
Renewable Energy
Sustainability and the Environment
POROUS PLATINUM
021001 nanoscience & nanotechnology
0104 chemical sciences
NO-H-2 fuel cell
chemistry
Linear sweep voltammetry
Phthalocyanine
Electrocatalysis
0210 nano-technology
Carbon
NO-H fuel cell
medicine.drug
Zdroj: Journal of Power Sources, 390, 249-260. ELSEVIER SCIENCE BV
ISSN: 0378-7753
DOI: 10.1016/j.jpowsour.2018.04.040
Popis: Carbon-supported iron complexes were investigated as electrocatalysts for the reduction of nitric oxide (NO) in a H-2-NO fuel cell conceived for the production of hydroxylamine (NH2OH) with concomitant generation of electricity. Two types of iron complexes with tetradentate ligands, namely bis(salicylidene)ethylenediimine (Salen) and phthalocyanine (Pc), supported on activated carbon or graphite were prepared and evaluated as electrocatalysts, either without further treatment or after pyrolysis at 700 degrees C. The performance in the reduction of NO of gas diffusion cathodes based on these electrocatalysts was investigated in an electrochemical half cell (3-electrode configuration) using linear sweep voltammetry (LSV). The most promising electrocatalysts were studied further by chronoamperometric experiments in a H-2-NO fuel cell, which allowed comparison in terms of power output and hydroxylamine production. Depending on the concentration of the NO feed (6 or 18%), the best electrocatalytic performance was delivered either by FePc or FeSalen. The gas diffusion electrode based on FeSalen supported on activated carbon with 0.3 wt% Fe-loading provided the highest current density (86 A/m(2)) and the best current efficiency (43%) towards the desired NH2OH when operating at the higher NO concentration (18%). Moreover, FeSalen offers the advantage of being cheaper than FePc. The experimental work was complemented by density functional theory (DFT) calculations, which allowed to shed more light on the reaction mechanism for the reduction of nitric oxide at the atomistic level.
Databáze: OpenAIRE
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