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An in situ proton filter covalent organic framework catalyst for highly efficient aqueous electrochemical ammonia production
Kayaramkodath C. Ranjeesh, Sukhjot Kaur, Abdul K. Mohammed, Safa Gaber, Divyani Gupta, Khaled Badawy, Mohamed Aslam, Nirpendra Singh, Tina Škorjanc, Matjaž Finšgar, 2023, izvirni znanstveni članek

Opis: The electrocatalytic nitrogen reduction reaction (NRR) driven by renewable electricity provides a green synthesis route for ammonia (NH3) production under ambient conditions but suffers from a low conversion yield and poor Faradaic efficiency (F.E.) because of strong competition from hydrogen evolution reaction (HER) and the poor solubility of N2 in aqueous systems. Herein, an in situ proton filter covalent organic framework catalyst (Ru-Tta-Dfp) is reported with inherent Ruthenium (Ru) sites where the framework controls reactant diffusion by suppressing proton supply and enhancing N2 flux, causing highly selective and efficient catalysis. The smart catalyst design results in a remarkable ammonia production yield rate of 2.03 mg h−1 mgcat−1 with an excellent F.E. of ≈52.9%. The findings are further endorsed with the help of molecular dynamics simulations and control COF systems without in situ proton filter feasibility. The results point to a paradigm shift in engineering high-performance NRR electrocatalysts for more feasible green NH3 production.
Ključne besede: covalent organic frameworks, ammonia, electrochemical synthesis, electrochemistry, nitrogen reduction reaction, ruthenium
Objavljeno v RUNG: 11.12.2023; Ogledov: 664; Prenosov: 6
.pdf Celotno besedilo (2,77 MB)
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Efficient electrochemical nitrogen fixation at iron phosphide (Fe_2P) catalyst in alkaline medium
Beata Rytelewska, Anna Chmielnicka, Takwa Chouki, Magdalena Skunik-Nuckowka, Shaghayegh Naghdi, Dominik Eder, Aleksandra Michalowska, Tomasz Ratajczyk, Egon Pavlica, Saim Emin, 2023, izvirni znanstveni članek

Opis: 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.
Ključne besede: nitrogen reduction, alkaline medium, iron phosphide catalyst, ammonia, electrochemical determinations
Objavljeno v RUNG: 30.11.2023; Ogledov: 762; Prenosov: 4
.pdf Celotno besedilo (2,67 MB)
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