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Metal-Free Catalytic Wet Oxidation: From Powder to Structured Catalyst Using N-Doped Carbon Nanotubes

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Abstract

This work shows a promising N-doped carbon catalyst for the oxidation of oxalic acid by catalytic wet oxidation, which is able to compete with the traditional noble metal and metal oxide catalysts used in the process. After preliminary studies conducted in batch mode, the catalytic performance of the metal-free carbon nanotubes, both in powder form and supported on a macrostructured carrier (a cordierite monolith), was evaluated under continuous operating conditions. The ability of the N-functionalities to promote activation and chemisorption of oxygen led not only to fast oxalic acid mineralization under batch mode (5 min of reaction to reach full mineralization), but also to good performance under continuous operation (more than 90% conversion of oxalic acid in the steady state, using the powder and around 55% using the catalyst immobilized on a honeycomb cordierite monolith).

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Acknowledgements

This work is a result of project “AIProcMat@N2020—Advanced Industrial Processes and Materials for a Sustainable Northern Region of Portugal 2020”, with the reference NORTE-01-0145-FEDER-000006, supported by Norte Portugal Regional Operational Programme (NORTE 2020), under the Portugal 2020 Partnership Agreement, through the European Regional Development Fund (ERDF) and of Project POCI-01-0145-FEDER-006984—Associate Laboratory LSRE-LCM funded by ERDF through COMPETE2020—Programa Operacional Competitividade e Internacionalização (POCI)—and by national funds through FCT—Fundação para a Ciência e a Tecnologia. D. Santos and R.P. Rocha acknowledge grants received from FCT (PD/BD/105983/2014 and SFRH/BD/95411/2013, respectively). The authors are indebted to Dr. Carlos M. Sá (CEMUP) for assistance with XPS analyses.

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  1. Laboratory of Separation and Reaction Engineering-Laboratory of Catalysis and Materials (LSRE-LCM), Faculty of Engineering, University of Porto, Rua Dr. Roberto Frias s/n, 4200-465, Porto, Portugal

    Raquel P. Rocha, Diogo F. M. Santos, Olívia Salomé M. P. Soares, Adrián M. T. Silva, Manuel Fernando R. Pereira & José L. Figueiredo

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  1. Raquel P. Rocha
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  2. Diogo F. M. Santos
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  3. Olívia Salomé M. P. Soares
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  4. Adrián M. T. Silva
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  5. Manuel Fernando R. Pereira
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  6. José L. Figueiredo
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Correspondence to Raquel P. Rocha.

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Rocha, R.P., Santos, D.F.M., Soares, O.S.M.P. et al. Metal-Free Catalytic Wet Oxidation: From Powder to Structured Catalyst Using N-Doped Carbon Nanotubes. Top Catal 61, 1957–1966 (2018). https://doi.org/10.1007/s11244-018-1029-8

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