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Title:Efficient electrochemical nitrogen fixation at iron phosphide (Fe_2P) catalyst in alkaline medium
Authors:ID Rytelewska, Beata (Author)
ID Chmielnicka, Anna (Author)
ID Chouki, Takwa (Author)
ID Skunik-Nuckowka, Magdalena (Author)
ID Naghdi, Shaghayegh (Author)
ID Eder, Dominik (Author)
ID Michalowska, Aleksandra (Author)
ID Ratajczyk, Tomasz (Author)
ID Pavlica, Egon (Author)
ID Emin, Saim (Author)
Files:.pdf Manuscript_Fe2P_NO3RR_ElectrochimActa_2023.pdf (2,67 MB)
MD5: 69E9202ADC77562347C28F23ECF00843
Work type:Unknown
Typology:1.01 - Original Scientific Article
Organization:UNG - University of Nova Gorica
Abstract:A catalytic system based on iron phosphide (Fe2P) has exhibited electrocatalytic activity toward N2-reduction reaction in alkaline medium (0.5 mol dm−3 NaOH). Based on voltammetric stripping-type electroanalytical measurements, Raman spectroscopic and spectrophotometric data, it can be stated that the Fe2P catalyst facilitates conversion of N2 to NH3, and the process is fairly selective with respect to the competing hydrogen evolution. A series of diagnostic electrocatalytic experiments (utilizing platinum nanoparticles and HKUST-1) have been proposed and performed to control purity of nitrogen gas and to probe presence of potential contaminants such as ammonia, nitrogen oxo-species and oxygen. On the whole, the results are consistent with the view that the interfacial reduced-iron (Fe0) centers, while existing within the network of P sites, induce activation and reduction of nitrogen, parallel to the water splitting (reduction) to hydrogen. It is apparent from Tafel plots and impedance measurements that mechanism and dynamics of nitrogen reduction depends on the applied electroreduction potential. The catalytic system exhibits certain tolerance with respect to the competitive hydrogen evolution and gives (during electrolysis at -0.4 V vs. RHE) the Faradaic efficiency, namely, the selectivity (molar) efficiency, toward production of NH3 on the level of 60%. Under such conditions, the NH3-yield rate has been found to be equal to 7.5 µmol cm−2 h−1 (21 µmol m−2 s−1). By referring to classic concepts of electrochemical kinetic analysis, the rate constant in heterogeneous units has been found to be on the moderate level of 1-2*10−4 cm s−1 (at -0.4 V). The above mentioned iron-phosphorous active sites, which are generated on surfaces of Fe2P particles, have also been demonstrated to exhibit strong catalytic properties during reductions of other electrochemically inert reactants, such as oxygen, nitrites and nitrates.
Keywords:nitrogen reduction, alkaline medium, iron phosphide catalyst, ammonia, electrochemical determinations
Publication status:Published
Publication version:Version of Record
Publication date:01.01.2023
Year of publishing:2023
Number of pages:str. 1-13
Numbering:Vol. 471, [article no.] 143360
PID:20.500.12556/RUNG-8664-230d8384-4c0d-cbeb-9562-81ba4eb2f488 New window
COBISS.SI-ID:174266371 New window
ISSN on article:0013-4686
DOI:10.1016/j.electacta.2023.143360 New window
Publication date in RUNG:30.11.2023
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Record is a part of a journal

Title:Electrochimica Acta
Shortened title:Electrochim. acta
Publisher:Pergamon Press
COBISS.SI-ID:1106959 New window

Document is financed by a project

Funder:ARIS - Slovenian Research and Innovation Agency
Project number:N2-0221
Name:Večnamenski elektrokatalizatorji za čisto energijsko pretvorbo


License:CC BY 4.0, Creative Commons Attribution 4.0 International
Description:This is the standard Creative Commons license that gives others maximum freedom to do what they want with the work as long as they credit the author.