Abstract
The formation of carbon deposits by the pyrolysis of acetonitrile at 600 and 700 °C with the assistance of metals/metal oxides generated in situ from MgCuAl and MgFeAl hydrotalcite-like materials (HTs) is described. The effects of the chemical composition of the supports on the quantity of carbon deposits and their structural ordering, morphology, nitrogen doping, porosity and capacitive properties, as well as their function as catalyst supports, were investigated. Among obtained pyrolytic carbons, that built of platelet-shaped carbon particles (formed at 600 °C with the use of MgCuAl HTs) appeared to be the most effective for charge storage (150 F g−1) as it contained mainly micropores (62%) and slit-shaped mesopores favouring the charge storage in deep parts of the carbon particles. It was revealed that the pyrolytic carbon exhibiting plate-like morphology with high exposure of edge plane surfaces and high specific surface area (1121 m2 g−1) provides the highest dispersion of 12-tungstophosphoric acid (HPW) and as a consequence leads to the highest yield (85%) to the main product (cis-2-butene) of n-butanol conversion achieved for HPW loaded on it.
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This research received funding from National Centre for Research and Development (NCBiR, Poland), agreement number EIG CONCERT-JAPAN/1/2019.
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AP contributed to conception, experimental design, carried out synthesis of the HTs, the composites, the carbon materials and XRD measurements and performed analysis and interpretation of the data obtained by various methods/techniques and manuscript composition. JG carried out XPS measurements. AM-I was involved in conception, carried out preparation of HPW-containing catalysts and measurements via FT-IR spectroscopy and performed catalytic tests. PP carried out measurements via Raman spectroscopy. MR-M carried out nitrogen sorption measurements. BDN carried out nitrogen sorption measurements. DD carried out measurements by means of SEM. GC carried out measurements by means of STEM.
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Details of the measurements (XRD, EA, N2 sorption, Raman, FT-IR, XPS, SEM, EDS, TEM) are provided. Additional graphs and micrographs include: XRD patterns of the HTs, the composites, the carbon materials, H3PW12O40·19H2O (HPW) and HPW deposited on the carbon materials; the stick patterns for references: MgO (PDF 00-045-0946), Cu (PDF 04-009-2090), graphite (PDF 040-014-0362), H3PW12O40·6H2O (PDF 00-050-0304) and H3PW12O40·14H2O (PDF 00-050-0656); SEM, BF-STEM and HAADT-STEM images of the carbon materials; the Raman spectra of the carbon materials and their fittings with D1, D2, D3, D4 and G components; nitrogen sorption isotherms of the carbon materials; CV curves recorded for the carbon materials deposited on glassy carbon electrode; BSE micrographs of HPW deposited on the carbon materials; FT-IR and XPS spectra of unsupported HPW and HPW deposited on the carbon materials; the comparison of PSD, pore volume and specific surface area for the carbon materials and the catalysts; and selectivity profiles for pure HPW and HPW deposited on various carbon materials in catalytic conversion of n-butanol. The data on physicochemical features of additional carbon materials: C-MgMnAl-600 and C-MgMnAl-700, determined by elemental analysis, Raman spectroscopy, nitrogen sorption are also provided. The parameters of W 4f7/2 line determined by XPS for HPW and the catalysts containing HPW deposited on various carbon materials are listed.
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Pacuła, A., Gurgul, J., Micek-Ilnicka, A. et al. Capacitors and catalyst supports based on pyrolytic carbon deposited on metals/metal oxides derived from hydrotalcite-like materials. J Mater Sci 59, 2788–2813 (2024). https://doi.org/10.1007/s10853-024-09361-6
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DOI: https://doi.org/10.1007/s10853-024-09361-6