Nanometric Cu-ZnO Particles Supported on N-Doped Graphitic Carbon as Catalysts for the Selective CO2 Hydrogenation to Methanol

Author:

Peng Lu1,Jurca Bogdan2ORCID,Garcia-Baldovi Alberto1,Tian Liang1ORCID,Sastre German1ORCID,Primo Ana1,Parvulescu Vasile2,Dhakshinamoorthy Amarajothi3ORCID,Garcia Hermenegildo1ORCID

Affiliation:

1. Instituto de Tecnología Química, Consejo Superior de Investigaciones Científicas-Universitat Politecnica de Valencia, Av. De los Naranjos s/n, 46022 Valencia, Spain

2. Department of Organic Chemistry, Biochemistry and Catalysis, University of Bucharest, B-dul Regina Elisabeta 4-12, 030016 Bucharest, Romania

3. Departamento de Química, Universitat Politècnica de València, C/Camino de Vera, s/n, 46022 Valencia, Spain

Abstract

The quest for efficient catalysts based on abundant elements that can promote the selective CO2 hydrogenation to green methanol still continues. Most of the reported catalysts are based on Cu/ZnO supported in inorganic oxides, with not much progress with respect to the benchmark Cu/ZnO/Al2O3 catalyst. The use of carbon supports for Cu/ZnO particles is much less explored in spite of the favorable strong metal support interaction that these doped carbons can establish. This manuscript reports the preparation of a series of Cu-ZnO@(N)C samples consisting of Cu/ZnO particles embedded within a N-doped graphitic carbon with a wide range of Cu/Zn atomic ratio. The preparation procedure relies on the transformation of chitosan, a biomass waste, into N-doped graphitic carbon by pyrolysis, which establishes a strong interaction with Cu nanoparticles (NPs) formed simultaneously by Cu2+ salt reduction during the graphitization. Zn2+ ions are subsequently added to the Cu–graphene material by impregnation. All the Cu/ZnO@(N)C samples promote methanol formation in the CO2 hydrogenation at temperatures from 200 to 300 °C, with the temperature increasing CO2 conversion and decreasing methanol selectivity. The best performing Cu-ZnO@(N)C sample achieves at 300 °C a CO2 conversion of 23% and a methanol selectivity of 21% that is among the highest reported, particularly for a carbon-based support. DFT calculations indicate the role of pyridinic N doping atoms stabilizing the Cu/ZnO NPs and supporting the formate pathway as the most likely reaction mechanism.

Funder

Spanish Ministry of Science and Innovation

Generalitat Valenciana

Advanced Materials programme Graphica

European Union NextGenerationEU

Publisher

MDPI AG

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