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Structure-performance relationship in mesoporous CuO/SBA-15 type SOx adsorbents: evolution of copper-based species under different regenerative treatments

Abstract

Sulphur oxides (SOx) represent a major air pollutant, controlled by national/international regulations. CuO/SiO2 materials are known as SOx trap materials. However, a large-scale development is still hampered by the sintering of the active phase over multiple adsorption/regeneration cycles, leading to the progressive decrease in SOx adsorption capacities of the adsorbent. In this work, SBA-15 Organised Mesoporous Silica was functionalized with highly dispersed Cu2+-based species. The as-obtained adsorbent was then assessed as a regenerable SOX trap material. An extended characterisation was performed along adsorption/regeneration cycles to correlate the evolution of the copper species with the performance of the adsorbent under different regenerative treatments. A thermal regeneration at 600°C under pure N2 leads to the formation of Cu+-based species enabling a significant increase in the SOX chemisorption efficiency which nevertheless decreases during the subsequent cycles due to a progressive sintering of the active phase, leading to bulky copper (II) oxide particles. The regeneration under “reductive” conditions (0.5 vol.% of H2 in N2) was then investigated as a way to decrease the regeneration temperature, to limit this sintering process. It was found that the general behaviour of the copper-based species was very sensitive to the regeneration temperature. At 600°C, the active phase was completely converted into large metallic copper particles, giving rise to a fast decrease in SOX adsorption capacities of the adsorbent due to a partial obstruction of the SBA-15 silica porosity. Conversely, when this regeneration was performed at 280°C, no decrease in performances was noticed and the copper species remained as a highly-dispersed phase on the silica support.

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Publication details

The article was received on 18 May 2017, accepted on 24 Jul 2017 and first published on 24 Jul 2017


Article type: Paper
DOI: 10.1039/C7CY01010A
Citation: Catal. Sci. Technol., 2017, Accepted Manuscript
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    Structure-performance relationship in mesoporous CuO/SBA-15 type SOx adsorbents: evolution of copper-based species under different regenerative treatments

    M. BERGER, P. Fioux, S. DORGE, H. Nouali, D. Habermacher, E. Fiani, M. Vierling, M. Moliere, J. Brilhac and J. Patarin, Catal. Sci. Technol., 2017, Accepted Manuscript , DOI: 10.1039/C7CY01010A

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