Silver Sulfide and Silver Sulfate as Aging Byproducts and Adsorbents for Gaseous Iodine Capture in Spent Nuclear Fuel Reprocessing

Ziheng Shen; Alexander I. Wiechert; Seungrag Choi; Lawrence L. Tavlarides; Costas Tsouris; Sotira Yiacoumi

doi:10.1021/acs.iecr.2c02024

Silver Sulfide and Silver Sulfate as Aging Byproducts and Adsorbents for Gaseous Iodine Capture in Spent Nuclear Fuel Reprocessing

Ziheng Shen, Alexander I. Wiechert, Seungrag Choi, Lawrence L. Tavlarides, Costas Tsouris, Sotira Yiacoumi

Chemical Process Scale Up

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Abstract

While it is considered a promising adsorbent for radioiodine capture in spent nuclear fuel reprocessing off-gas, silver functionalized silica aerogel (Ag⁰-aerogel) experiences a capacity loss when exposed to other off-gas components (O₂, H₂O, NO, and NO₂) through a process known as aging. Ag₂S and Ag₂SO₄were identified as major byproducts of aging, but their impact on iodine adsorption remains unclear. Thus, to further investigate aging, we loaded Ag₂S and Ag₂SO₄powders with molecular iodine (I₂) at 150 °C and characterized their properties. The I₂adsorption capacity of Ag₂SO₄was 0.12 wt % after 72 h, suggesting its formation directly reduces the capacity of the Ag⁰-aerogel. Conversely, Ag₂S had an iodine capacity of 86.8 wt % and near total Ag utilization after 240 h. Given its high capacity and availability, we evaluated the feasibility of Ag₂S as an I₂adsorbent in future applications. Several drawbacks need to be overcome, including the relatively slow uptake rate, potential emission of another hazardous byproduct (SO₂), and potential aging effects (e.g., Ag₂S conversion to Ag₂SO₄) before Ag₂S can be applied for the radioiodine capture process.

Original language	English
Pages (from-to)	14393-14401
Number of pages	9
Journal	Industrial and Engineering Chemistry Research
Volume	61
Issue number	38
DOIs	https://doi.org/10.1021/acs.iecr.2c02024
State	Published - Sep 28 2022

Funding

This research was supported by the Nuclear Energy University Program, Office of Nuclear Energy, U.S. Department of Energy (grant number 18-15596). The authors are thankful to Dr. Greaney Allison (Oak Ridge National Laboratory) for providing the I-loaded AgZ samples used for elemental analysis in this study. This work was performed in part at the Materials Characterization Facility (MCF) at Georgia Tech. The MCF is jointly supported by the GT Institute for Materials (IMat) and the Institute for Electronics and Nanotechnology (IEN), which is a member of the National Nanotechnology Coordinated Infrastructure supported by the National Science Foundation (Grant ECCS-2025462). 2 0

Funders	Funder number
GT Institute for Materials
IMat
National Science Foundation	ECCS-2025462
U.S. Department of Energy	18-15596
Office of Nuclear Energy
Nuclear Energy University Program

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title = "Silver Sulfide and Silver Sulfate as Aging Byproducts and Adsorbents for Gaseous Iodine Capture in Spent Nuclear Fuel Reprocessing",

abstract = "While it is considered a promising adsorbent for radioiodine capture in spent nuclear fuel reprocessing off-gas, silver functionalized silica aerogel (Ag0-aerogel) experiences a capacity loss when exposed to other off-gas components (O2, H2O, NO, and NO2) through a process known as aging. Ag2S and Ag2SO4were identified as major byproducts of aging, but their impact on iodine adsorption remains unclear. Thus, to further investigate aging, we loaded Ag2S and Ag2SO4powders with molecular iodine (I2) at 150 °C and characterized their properties. The I2adsorption capacity of Ag2SO4was 0.12 wt % after 72 h, suggesting its formation directly reduces the capacity of the Ag0-aerogel. Conversely, Ag2S had an iodine capacity of 86.8 wt % and near total Ag utilization after 240 h. Given its high capacity and availability, we evaluated the feasibility of Ag2S as an I2adsorbent in future applications. Several drawbacks need to be overcome, including the relatively slow uptake rate, potential emission of another hazardous byproduct (SO2), and potential aging effects (e.g., Ag2S conversion to Ag2SO4) before Ag2S can be applied for the radioiodine capture process.",

author = "Ziheng Shen and Wiechert, {Alexander I.} and Seungrag Choi and Tavlarides, {Lawrence L.} and Costas Tsouris and Sotira Yiacoumi",

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AU - Shen, Ziheng

AU - Wiechert, Alexander I.

AU - Choi, Seungrag

AU - Tavlarides, Lawrence L.

AU - Tsouris, Costas

AU - Yiacoumi, Sotira

PY - 2022/9/28

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N2 - While it is considered a promising adsorbent for radioiodine capture in spent nuclear fuel reprocessing off-gas, silver functionalized silica aerogel (Ag0-aerogel) experiences a capacity loss when exposed to other off-gas components (O2, H2O, NO, and NO2) through a process known as aging. Ag2S and Ag2SO4were identified as major byproducts of aging, but their impact on iodine adsorption remains unclear. Thus, to further investigate aging, we loaded Ag2S and Ag2SO4powders with molecular iodine (I2) at 150 °C and characterized their properties. The I2adsorption capacity of Ag2SO4was 0.12 wt % after 72 h, suggesting its formation directly reduces the capacity of the Ag0-aerogel. Conversely, Ag2S had an iodine capacity of 86.8 wt % and near total Ag utilization after 240 h. Given its high capacity and availability, we evaluated the feasibility of Ag2S as an I2adsorbent in future applications. Several drawbacks need to be overcome, including the relatively slow uptake rate, potential emission of another hazardous byproduct (SO2), and potential aging effects (e.g., Ag2S conversion to Ag2SO4) before Ag2S can be applied for the radioiodine capture process.

AB - While it is considered a promising adsorbent for radioiodine capture in spent nuclear fuel reprocessing off-gas, silver functionalized silica aerogel (Ag0-aerogel) experiences a capacity loss when exposed to other off-gas components (O2, H2O, NO, and NO2) through a process known as aging. Ag2S and Ag2SO4were identified as major byproducts of aging, but their impact on iodine adsorption remains unclear. Thus, to further investigate aging, we loaded Ag2S and Ag2SO4powders with molecular iodine (I2) at 150 °C and characterized their properties. The I2adsorption capacity of Ag2SO4was 0.12 wt % after 72 h, suggesting its formation directly reduces the capacity of the Ag0-aerogel. Conversely, Ag2S had an iodine capacity of 86.8 wt % and near total Ag utilization after 240 h. Given its high capacity and availability, we evaluated the feasibility of Ag2S as an I2adsorbent in future applications. Several drawbacks need to be overcome, including the relatively slow uptake rate, potential emission of another hazardous byproduct (SO2), and potential aging effects (e.g., Ag2S conversion to Ag2SO4) before Ag2S can be applied for the radioiodine capture process.

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Silver Sulfide and Silver Sulfate as Aging Byproducts and Adsorbents for Gaseous Iodine Capture in Spent Nuclear Fuel Reprocessing

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