Silver-functionalized silica aerogel: towards an understanding of aging on iodine sorption performance
The silver-functionalized silica aerogel (Ag 0 -aerogel) is being developed for the removal and sequestration of iodine compounds from the off-gas of a nuclear fuel reprocessing plant. This material shows high selectivity and sorption capacity for iodine. However, its sorption performance decreases...
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| Published in | RSC advances Vol. 8; no. 56; pp. 31843 - 31852 |
|---|---|
| Main Authors | , , |
| Format | Journal Article |
| Language | English |
| Published |
England
Royal Society of Chemistry
12.09.2018
The Royal Society of Chemistry |
| Subjects | |
| Online Access | Get full text |
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| Abstract | The silver-functionalized silica aerogel (Ag
0
-aerogel) is being developed for the removal and sequestration of iodine compounds from the off-gas of a nuclear fuel reprocessing plant. This material shows high selectivity and sorption capacity for iodine. However, its sorption performance decreases when exposed to air containing H
2
O and NO
x
at 150 °C for extended periods of time. This phenomenon is referred to as "aging" and simulates exposure of the sorbent during plant idling. This extensive study of unaged and aged samples of Ag
0
-aerogel with and without iodine revealed that decreased efficiency of I capture after NO-aging can be attributed to an increase in size of silver nanoparticles and by the formation of free sulfate on their surfaces from oxidized thiol groups. The smaller reactive surface areas of bigger particles and thin sulfate layer on particle surfaces prevented a complete utilization of the silver. By contrast, formation of silver sulfate appears to be the main factor in decreasing the sorption capacity for samples aged in dry or humid air. It is hypothesized that a short period exposure of the Ag
0
-aerogel to a reducing gas stream would reduce oxidized silver back to metal and sulfate to sulfide. This may recover the sorption performance of Ag
0
-aerogel close to original levels.
This manuscript elucidates the mechanism responsible for a decrease of iodine-sorption performance for Ag
0
-functionalized silica aerogel in the reprocessing off-gas streams. |
|---|---|
| AbstractList | The silver-functionalized silica aerogel (Ag
0
-aerogel) is being developed for the removal and sequestration of iodine compounds from the off-gas of a nuclear fuel reprocessing plant. This material shows high selectivity and sorption capacity for iodine. However, its sorption performance decreases when exposed to air containing H
2
O and NO
x
at 150 °C for extended periods of time. This phenomenon is referred to as “aging” and simulates exposure of the sorbent during plant idling. This extensive study of unaged and aged samples of Ag
0
-aerogel with and without iodine revealed that decreased efficiency of I capture after NO-aging can be attributed to an increase in size of silver nanoparticles and by the formation of free sulfate on their surfaces from oxidized thiol groups. The smaller reactive surface areas of bigger particles and thin sulfate layer on particle surfaces prevented a complete utilization of the silver. By contrast, formation of silver sulfate appears to be the main factor in decreasing the sorption capacity for samples aged in dry or humid air. It is hypothesized that a short period exposure of the Ag
0
-aerogel to a reducing gas stream would reduce oxidized silver back to metal and sulfate to sulfide. This may recover the sorption performance of Ag
0
-aerogel close to original levels.
This manuscript elucidates the mechanism responsible for a decrease of iodine-sorption performance for Ag
0
-functionalized silica aerogel in the reprocessing off-gas streams. The silver-functionalized silica aerogel (Ag0-aerogel) is being developed for the removal and sequestration of iodine compounds from the off-gas of a nuclear fuel reprocessing plant. This material shows high selectivity and sorption capacity for iodine. However, its sorption performance decreases when exposed to air containing H2O and NO x at 150 °C for extended periods of time. This phenomenon is referred to as "aging" and simulates exposure of the sorbent during plant idling. This extensive study of unaged and aged samples of Ag0-aerogel with and without iodine revealed that decreased efficiency of I capture after NO-aging can be attributed to an increase in size of silver nanoparticles and by the formation of free sulfate on their surfaces from oxidized thiol groups. The smaller reactive surface areas of bigger particles and thin sulfate layer on particle surfaces prevented a complete utilization of the silver. By contrast, formation of silver sulfate appears to be the main factor in decreasing the sorption capacity for samples aged in dry or humid air. It is hypothesized that a short period exposure of the Ag0-aerogel to a reducing gas stream would reduce oxidized silver back to metal and sulfate to sulfide. This may recover the sorption performance of Ag0-aerogel close to original levels.The silver-functionalized silica aerogel (Ag0-aerogel) is being developed for the removal and sequestration of iodine compounds from the off-gas of a nuclear fuel reprocessing plant. This material shows high selectivity and sorption capacity for iodine. However, its sorption performance decreases when exposed to air containing H2O and NO x at 150 °C for extended periods of time. This phenomenon is referred to as "aging" and simulates exposure of the sorbent during plant idling. This extensive study of unaged and aged samples of Ag0-aerogel with and without iodine revealed that decreased efficiency of I capture after NO-aging can be attributed to an increase in size of silver nanoparticles and by the formation of free sulfate on their surfaces from oxidized thiol groups. The smaller reactive surface areas of bigger particles and thin sulfate layer on particle surfaces prevented a complete utilization of the silver. By contrast, formation of silver sulfate appears to be the main factor in decreasing the sorption capacity for samples aged in dry or humid air. It is hypothesized that a short period exposure of the Ag0-aerogel to a reducing gas stream would reduce oxidized silver back to metal and sulfate to sulfide. This may recover the sorption performance of Ag0-aerogel close to original levels. The silver-functionalized silica aerogel (Ag -aerogel) is being developed for the removal and sequestration of iodine compounds from the off-gas of a nuclear fuel reprocessing plant. This material shows high selectivity and sorption capacity for iodine. However, its sorption performance decreases when exposed to air containing H O and NO at 150 °C for extended periods of time. This phenomenon is referred to as "aging" and simulates exposure of the sorbent during plant idling. This extensive study of unaged and aged samples of Ag -aerogel with and without iodine revealed that decreased efficiency of I capture after NO-aging can be attributed to an increase in size of silver nanoparticles and by the formation of free sulfate on their surfaces from oxidized thiol groups. The smaller reactive surface areas of bigger particles and thin sulfate layer on particle surfaces prevented a complete utilization of the silver. By contrast, formation of silver sulfate appears to be the main factor in decreasing the sorption capacity for samples aged in dry or humid air. It is hypothesized that a short period exposure of the Ag -aerogel to a reducing gas stream would reduce oxidized silver back to metal and sulfate to sulfide. This may recover the sorption performance of Ag -aerogel close to original levels. The silver-functionalized silica aerogel (Ag0-aerogel) is being developed for the removal and sequestration of iodine compounds from the off-gas of a nuclear fuel reprocessing plant. This material shows high selectivity and sorption capacity for iodine. However, its sorption performance decreases when exposed to air containing H2O and NOx at 150 °C for extended periods of time. This phenomenon is referred to as “aging” and simulates exposure of the sorbent during plant idling. This extensive study of unaged and aged samples of Ag0-aerogel with and without iodine revealed that decreased efficiency of I capture after NO-aging can be attributed to an increase in size of silver nanoparticles and by the formation of free sulfate on their surfaces from oxidized thiol groups. The smaller reactive surface areas of bigger particles and thin sulfate layer on particle surfaces prevented a complete utilization of the silver. By contrast, formation of silver sulfate appears to be the main factor in decreasing the sorption capacity for samples aged in dry or humid air. It is hypothesized that a short period exposure of the Ag0-aerogel to a reducing gas stream would reduce oxidized silver back to metal and sulfate to sulfide. This may recover the sorption performance of Ag0-aerogel close to original levels. The silver-functionalized silica aerogel (Ag 0 -aerogel) is being developed for the removal and sequestration of iodine compounds from the off-gas of a nuclear fuel reprocessing plant. This material shows high selectivity and sorption capacity for iodine. However, its sorption performance decreases when exposed to air containing H 2 O and NO x at 150 °C for extended periods of time. This phenomenon is referred to as “aging” and simulates exposure of the sorbent during plant idling. This extensive study of unaged and aged samples of Ag 0 -aerogel with and without iodine revealed that decreased efficiency of I capture after NO-aging can be attributed to an increase in size of silver nanoparticles and by the formation of free sulfate on their surfaces from oxidized thiol groups. The smaller reactive surface areas of bigger particles and thin sulfate layer on particle surfaces prevented a complete utilization of the silver. By contrast, formation of silver sulfate appears to be the main factor in decreasing the sorption capacity for samples aged in dry or humid air. It is hypothesized that a short period exposure of the Ag 0 -aerogel to a reducing gas stream would reduce oxidized silver back to metal and sulfate to sulfide. This may recover the sorption performance of Ag 0 -aerogel close to original levels. The silver-functionalized silica aerogel (Ag⁰-aerogel) is being developed for the removal and sequestration of iodine compounds from the off-gas of a nuclear fuel reprocessing plant. This material shows high selectivity and sorption capacity for iodine. However, its sorption performance decreases when exposed to air containing H₂O and NOₓ at 150 °C for extended periods of time. This phenomenon is referred to as “aging” and simulates exposure of the sorbent during plant idling. This extensive study of unaged and aged samples of Ag⁰-aerogel with and without iodine revealed that decreased efficiency of I capture after NO-aging can be attributed to an increase in size of silver nanoparticles and by the formation of free sulfate on their surfaces from oxidized thiol groups. The smaller reactive surface areas of bigger particles and thin sulfate layer on particle surfaces prevented a complete utilization of the silver. By contrast, formation of silver sulfate appears to be the main factor in decreasing the sorption capacity for samples aged in dry or humid air. It is hypothesized that a short period exposure of the Ag⁰-aerogel to a reducing gas stream would reduce oxidized silver back to metal and sulfate to sulfide. This may recover the sorption performance of Ag⁰-aerogel close to original levels. |
| Author | Kova ík, Libor Ilton, Eugene S Matyáš, Josef |
| AuthorAffiliation | Pacific Northwest National Laboratory |
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| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/35547510$$D View this record in MEDLINE/PubMed https://www.osti.gov/biblio/1469722$$D View this record in Osti.gov |
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| Snippet | The silver-functionalized silica aerogel (Ag
0
-aerogel) is being developed for the removal and sequestration of iodine compounds from the off-gas of a nuclear... The silver-functionalized silica aerogel (Ag -aerogel) is being developed for the removal and sequestration of iodine compounds from the off-gas of a nuclear... The silver-functionalized silica aerogel (Ag0-aerogel) is being developed for the removal and sequestration of iodine compounds from the off-gas of a nuclear... The silver-functionalized silica aerogel (Ag⁰-aerogel) is being developed for the removal and sequestration of iodine compounds from the off-gas of a nuclear... |
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| SubjectTerms | Aerogels Aging air Chemistry Exposure INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Iodine Iodine compounds Nanoparticles nanosilver nitrogen oxides Nuclear fuel reprocessing nuclear fuels oxidation silica Silicon dioxide Silver sorbents Sorption sulfates thiols |
| Title | Silver-functionalized silica aerogel: towards an understanding of aging on iodine sorption performance |
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