Nickel and nickel oxide are widely used as heterogeneous catalysts in various processes involving the hydrogenation or reduction of organic compounds, and also as excellent methanation catalysts in the hydrogenation of CO2. As heterogeneous catalysis is a surface-dependent process, nickel compounds in the form of microparticles (MPs), and particularly nanoparticles (NPs), improve the catalytic activity of Ni-based catalysts due to their high specific surface area. Solvothermal synthesis, which has so far been neglected for the synthesis of Ni-based methanation catalysts, was used in this study to synthesize nickel and nickel oxide MPs and NPs with a narrow size distribution. Solvothermal synthesis allows for the control of both the chemical composition of the resulting Ni catalysts and their physical structure by simply changing the reaction conditions (solvent, temperature, or concentration of reactants). Only non-toxic substances were used for synthesis in this study, meaning that the whole synthesis process can be described as environmentally friendly. Solvothermally prepared Ni compounds were subsequently transformed into nickel oxide by means of high-temperature decomposition, and all of the prepared Ni-based compounds were tested as catalysts for CO2 methanation. The best catalysts prepared in this study exhibited a CO2 conversion rate of nearly 95% and a selectivity for methane close to 100%, which represent thermodynamic limits for this reaction at the used temperature. These results are commonly achieved with much more complex catalytic composites containing precious metals, while here we worked with pure nickel and its oxides, in the form of micro- or nanoparticles, only.

Center for Innovations in the Field of Nanomaterials and Nanotechnologies J Heyrovský Institute of Physical Chemistry Czech Academy of Sciences Dolejskova 2155 3 18223 Prague Czech Republic

Czech Advanced Technology and Research Institute CATRIN Regional Centrum of Advanced Technologies and Materials Palacký University Olomouc Slechtitelu 27 78371 Olomouc Czech Republic

Department of Biophysics Faculty of Science Palacký University Olomouc Slechtitelu 27 78371 Olomouc Czech Republic

Department of Chemistry University of Milan Via Golgi 19 20133 Milano Italy

Department of Civil Energy Environmental and Material Engineering Mediterranea University of Reggio Calabria 89124 Reggio Calabria Italy

Department of Low Dimensional Systems J Heyrovský Institute of Physical Chemistry Czech Academy of Sciences Dolejskova 2155 3 18223 Prague Czech Republic

Department of Nanocatalysis J Heyrovský Institute of Physical Chemistry Czech Academy of Sciences Dolejskova 2155 3 18223 Prague Czech Republic

Department of Physical Chemistry Faculty of Science Palacký University Olomouc 17 Listopadu 12 77900 Olomouc Czech Republic

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