Tunable Syngas Formation at Industrially Relevant Current Densities via CO2 Electroreduction and Hydrogen Evolution over Ni and Fe‐derived Catalysts obtained via One‐Step Pyrolysis of Polybenzoxazine Based Composites

Author:

Sanjuán Ignacio1,Kumbhar Vaibhav1,Chanda Vimanshu1,Machado Raíssa R. L.1,Jaato Bright N.1,Braun Michael1,Mahbub Muhammad A. A.2,Bendt Georg3,Hagemann Ulrich4,Heidelmann Markus4,Schuhmann Wolfgang2,Andronescu Corina1ORCID

Affiliation:

1. Chemical Technology III; Faculty of Chemistry and CENIDE Center for Nanointegration University of Duisburg‐Essen Carl‐Benz‐Straße 199 47057 Duisburg Germany

2. Analytical Chemistry‐Center for Electrochemical Sciences (CES) Faculty of Chemistry and Biochemistry Ruhr University Bochum Universitätsstrasse 150 44780 Bochum Germany

3. Institute of Inorganic Chemistry; Faculty of Chemistry and CENIDE Center for Nanointegration University of Duisburg‐Essen Universitätsstaße 7 45141 Essen Germany

4. ICAN – Interdisciplinary Center for Analytics on the Nanoscale University of Duisburg‐Essen Carl‐Benz‐Straße 199 47057 Duisburg Germany

Abstract

AbstractSimultaneous electroreduction of CO2 and H2O to syngas can provide a sustainable feed for established processes used to synthesize carbon‐based chemicals. The synthesis of MOx/M‐N‐Cs (M = Ni, Fe) electrocatalysts reported via one‐step pyrolysis that shows increased performance during syngas electrosynthesis at high current densities with adaptable H2/CO ratios, e.g., for the Fischer–Tropsch process. When embedded in gas diffusion electrodes (GDEs) with optimized hydrophobicity, the NiOx/Ni‐N‐C catalyst produces syngas (H2/CO = 0.67) at −200 mA cm−2 while for the FeOx/Fe‐N‐C syngas production occurs at ≈−150 mA cm−2. By tuning the electrocatalyst's microenvironment, stable operation for >3 h at −200 mA cm−2 is achieved with the NiOx/Ni‐N‐C GDE. Post‐electrolysis characterization revealed that the restructuring of the catalyst via reduction of NiOx to metallic Ni NPs still enables stable operation of the electrode at −200 mA cm−2, when embedded in an optimized microenvironment. The ionomer and additives used in the catalyst layer are important for the observed stable operation. Operando Raman measurements confirm the presence of NiOx during CO formation and indicate weak adsorption of CO on the catalyst surface.

Funder

Universität Duisburg-Essen

Bundesministerium für Bildung und Forschung

Publisher

Wiley

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