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2. Large-scale synthesis of metal/nitrogen Co-doped carbon catalysts for CO2 electroreduction

Author

Xiang Lyu, Dimitra Anastasiadou, Jithu Raj, Jingjie Wu, Yaocai Bai, Jianlin Li, David A. Cullen, Jun Yang, Liliana P.L. Gonçalves, Oleg I. Lebedev, Yury V. Kolen'ko, Marta Costa Figueiredo, Alexey Serov, Inorganic Materials & Catalysis, and EIRES Chem. for Sustainable Energy Systems

Subjects
Nickel, General Chemical Engineering, Large-scale synthesis, Electrochemistry, CO valorization, M–N–C catalysts, Microstructure, Single-atom catalysts
Abstract

Here, we report a facile approach for synthesizing M–N–C catalysts (M = Co, Fe, Ni) at a commercial scale without employing organic solvents. Our characterization efforts indicate that single atomic catalysts with high surface areas were successfully obtained. Electrochemical measurements demonstrate that, among the three synthesized catalysts, Ni–N–C exhibits the highest performance in the electrochemical CO2 reduction reaction (CO2RR) to carbon monoxide (CO), affording 80% Faradaic efficiency (FE) of CO production at –0.49 VRHE with a turnover frequency (TOF) of 57,379 h–1. Large-scale synthesis coupled with high performance allows moving forward with the practical implementation of M–N–C catalysts for industrially relevant CO2RR.

Published
2023

4. In situ investigation of the CO2 methanation on carbon/ceria-supported Ni catalysts using modulation-excitation DRIFTS

Author

Liliana P.L. Gonçalves, Jerrik Mielby, O. Salomé G.P. Soares, Juliana P.S. Sousa, Dmitri Y. Petrovykh, Oleg I. Lebedev, M. Fernando R. Pereira, Søren Kegnæs, Yury V. Kolen’ko, Laboratoire de cristallographie et sciences des matériaux (CRISMAT), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Laboratory of Separation and Reaction Engineering - Laboratory of Catalysis and Materials (LSRE-LCM), Faculdade de Engenharia (LSRE-LCM), Universidade do Porto = University of Porto, and International Iberian Nanotechnology Laboratory (INL)

Subjects
Heterogeneous catalysis, In situ DRIFTS, Carbon dioxide, Process Chemistry and Technology, [CHIM]Chemical Sciences, Methane, Catalysis, Reaction mechanism, General Environmental Science
Abstract

The development of novel cost-efficient, high-performing catalysts for CO2 methanation that are active at low temperatures can be optimized through the understanding of the reaction mechanism on different materials. A series of Ni-based catalysts supported on CeO2 and carbon/CeO2 composites was investigated, showing that Ni nanoparticles supported on a carbon/CeO2 composite with a 50:50 weight ratio and on pure CeO2 have excellent low-temperature activity and achieve up to 87% CO2 conversion with full selectivity towards CH4 at 370 °C. Importantly, meaningful insights on the reaction mechanism were gathered for the different types of materials by using the emerging ME−PSD−DRIFTS technique. The study of the rate of formation/consumption of the various intermediates showed that the CO2 methanation reaction follows a combination of the CO and formate pathways in the case of Ni on pure CeO2; however, in the case of Ni on the carbon/CeO2 composite, it follows only the formate pathway.

Published
2022

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