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Structure-performance relationship in CuO/SBA-15-type SOx adsorbent: evolution of copper-based species under different regenerative treatmentsElectronic supplementary information (ESI) available. See DOI: 10.1039/c7cy01010a
Sulphur oxides (SO x ) represent a major air pollutant and are controlled by national and international regulations. CuO/SiO 2 materials are known as SO x trap materials. However, their large-scale development is still hampered by the sintering of the active phase over multiple adsorption/regenerati...
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Main Authors: | , , , , , , , , , |
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Format: | Article |
Language: | English |
Online Access: | Get full text |
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Summary: | Sulphur oxides (SO
x
) represent a major air pollutant and are controlled by national and international regulations. CuO/SiO
2
materials are known as SO
x
trap materials. However, their large-scale development is still hampered by the sintering of the active phase over multiple adsorption/regeneration cycles, leading to the progressive decrease in SO
x
adsorption capacities of the adsorbent. In this work, SBA-15 organised mesoporous silica was functionalized with highly dispersed Cu
2+
-based species. The as-obtained adsorbent was then assessed as a regenerable SO
x
trap material. An extended characterisation was performed along with adsorption/regeneration cycles to correlate the evolution of the copper species with the performance of the adsorbent under different regenerative treatments. Thermal regeneration at 600 °C under pure N
2
leads to the formation of Cu
+
-based species, enabling a significant increase in SO
x
chemisorption efficiency, which nevertheless decreases during the subsequent cycles due to progressive sintering of the active phase, leading to bulky copper(
ii
) oxide particles. Regeneration under reductive conditions (0.5 vol% of H
2
in N
2
) was then investigated as a way to decrease the regeneration temperature and 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 SO
x
adsorption capacity of the adsorbent due to 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.
Desulfurization of industrial flue gas stream: characterization of the evolution of copper active sites along SO
x
adsorption/regeneration cycling experiments in CuO/SBA-15-type adsorbent. |
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ISSN: | 2044-4753 2044-4761 |
DOI: | 10.1039/c7cy01010a |