Boosting Hydrogen Production from Formic Acid over Pd Catalysts by Deposition of N-Containing Precursors on the Carbon Support
Formic acid is a promising liquid organic hydrogen carrier (LOHC) since it has relatively high hydrogen content (4.4 wt%), low inflammability, low toxicity and can be obtained from biomass or from CO<sub>2</sub>. The aim of the present research was the creation of efficient 1 wt% Pd cata...
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MDPI AG
2019-10-01
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| Series: | Energies |
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| Online Access: | https://www.mdpi.com/1996-1073/12/20/3885 |
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| author | Fedor S. Golub Sergey Beloshapkin Artem V. Gusel’nikov Vasily A. Bolotov Valentin N. Parmon Dmitri A. Bulushev |
| author_facet | Fedor S. Golub Sergey Beloshapkin Artem V. Gusel’nikov Vasily A. Bolotov Valentin N. Parmon Dmitri A. Bulushev |
| author_sort | Fedor S. Golub |
| collection | DOAJ |
| description | Formic acid is a promising liquid organic hydrogen carrier (LOHC) since it has relatively high hydrogen content (4.4 wt%), low inflammability, low toxicity and can be obtained from biomass or from CO<sub>2</sub>. The aim of the present research was the creation of efficient 1 wt% Pd catalysts supported on mesoporous graphitic carbon (Sibunit) for the hydrogen production from gas-phase formic acid. For this purpose, the carbon support was modified by pyrolysis of deposited precursors containing pyridinic nitrogen such as melamine (Mel), 2,2′-bipyridine (Bpy) or 1,10-phenanthroline (Phen) at 673 K. The following activity trend of the catalysts Pd/Mel/C > Pd/C ~ Pd/Bpy/C > Pd/Phen/C was obtained. The activity of the Pd/Mel/C catalyst was by a factor of 4 higher than the activity of the Pd/C catalyst at about 373 K and the apparent activation energy was significantly lower than those for the other catalysts (32 vs. 42−46 kJ/mol). The high activity of the melamine-based samples was explained by a high dispersion of Pd nanoparticles (~2 nm, HRTEM) and their strong electron-deficient character (XPS) provided by interaction of Pd with pyridinic nitrogen species of the support. The presented results can be used for the development of supported Pd catalysts for hydrogen production from different liquid organic hydrogen carriers. |
| first_indexed | 2024-04-13T06:06:57Z |
| format | Article |
| id | doaj.art-54d1a9d25a9c4403b55b02ed78456481 |
| institution | Directory Open Access Journal |
| issn | 1996-1073 |
| language | English |
| last_indexed | 2024-04-13T06:06:57Z |
| publishDate | 2019-10-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Energies |
| spelling | doaj.art-54d1a9d25a9c4403b55b02ed784564812022-12-22T02:59:12ZengMDPI AGEnergies1996-10732019-10-011220388510.3390/en12203885en12203885Boosting Hydrogen Production from Formic Acid over Pd Catalysts by Deposition of N-Containing Precursors on the Carbon SupportFedor S. Golub0Sergey Beloshapkin1Artem V. Gusel’nikov2Vasily A. Bolotov3Valentin N. Parmon4Dmitri A. Bulushev5Laboratory of Catalytic Methods of Solar Energy Transformation, Boreskov Institute of Catalysis, SB RAS, 630090 Novosibirsk, RussiaBernal Institute, University of Limerick, V94 T9PX Limerick, IrelandLaboratory of Physico-Chemistry of Nanomaterials, Nikolaev Institute of Inorganic Chemistry, SB RAS, 630090 Novosibirsk, RussiaLaboratory of Catalytic Methods of Solar Energy Transformation, Boreskov Institute of Catalysis, SB RAS, 630090 Novosibirsk, RussiaLaboratory of Catalytic Methods of Solar Energy Transformation, Boreskov Institute of Catalysis, SB RAS, 630090 Novosibirsk, RussiaLaboratory of Catalytic Methods of Solar Energy Transformation, Boreskov Institute of Catalysis, SB RAS, 630090 Novosibirsk, RussiaFormic acid is a promising liquid organic hydrogen carrier (LOHC) since it has relatively high hydrogen content (4.4 wt%), low inflammability, low toxicity and can be obtained from biomass or from CO<sub>2</sub>. The aim of the present research was the creation of efficient 1 wt% Pd catalysts supported on mesoporous graphitic carbon (Sibunit) for the hydrogen production from gas-phase formic acid. For this purpose, the carbon support was modified by pyrolysis of deposited precursors containing pyridinic nitrogen such as melamine (Mel), 2,2′-bipyridine (Bpy) or 1,10-phenanthroline (Phen) at 673 K. The following activity trend of the catalysts Pd/Mel/C > Pd/C ~ Pd/Bpy/C > Pd/Phen/C was obtained. The activity of the Pd/Mel/C catalyst was by a factor of 4 higher than the activity of the Pd/C catalyst at about 373 K and the apparent activation energy was significantly lower than those for the other catalysts (32 vs. 42−46 kJ/mol). The high activity of the melamine-based samples was explained by a high dispersion of Pd nanoparticles (~2 nm, HRTEM) and their strong electron-deficient character (XPS) provided by interaction of Pd with pyridinic nitrogen species of the support. The presented results can be used for the development of supported Pd catalysts for hydrogen production from different liquid organic hydrogen carriers.https://www.mdpi.com/1996-1073/12/20/3885hydrogen productionformic acid decompositionpd/cmelamineg-c<sub>3</sub>n<sub>4</sub>bipyridinephenanthrolinen-doped carbon |
| spellingShingle | Fedor S. Golub Sergey Beloshapkin Artem V. Gusel’nikov Vasily A. Bolotov Valentin N. Parmon Dmitri A. Bulushev Boosting Hydrogen Production from Formic Acid over Pd Catalysts by Deposition of N-Containing Precursors on the Carbon Support Energies hydrogen production formic acid decomposition pd/c melamine g-c<sub>3</sub>n<sub>4</sub> bipyridine phenanthroline n-doped carbon |
| title | Boosting Hydrogen Production from Formic Acid over Pd Catalysts by Deposition of N-Containing Precursors on the Carbon Support |
| title_full | Boosting Hydrogen Production from Formic Acid over Pd Catalysts by Deposition of N-Containing Precursors on the Carbon Support |
| title_fullStr | Boosting Hydrogen Production from Formic Acid over Pd Catalysts by Deposition of N-Containing Precursors on the Carbon Support |
| title_full_unstemmed | Boosting Hydrogen Production from Formic Acid over Pd Catalysts by Deposition of N-Containing Precursors on the Carbon Support |
| title_short | Boosting Hydrogen Production from Formic Acid over Pd Catalysts by Deposition of N-Containing Precursors on the Carbon Support |
| title_sort | boosting hydrogen production from formic acid over pd catalysts by deposition of n containing precursors on the carbon support |
| topic | hydrogen production formic acid decomposition pd/c melamine g-c<sub>3</sub>n<sub>4</sub> bipyridine phenanthroline n-doped carbon |
| url | https://www.mdpi.com/1996-1073/12/20/3885 |
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