TY - JOUR
T1 - Removal of CrO42-, a Nonradioactive Surrogate of 99TcO4-, Using LDH-Mo3S13Nanosheets
AU - Celik, Ahmet
AU - Li, Dien
AU - Quintero, Michael A.
AU - Taylor-Pashow, Kathryn M.L.
AU - Zhu, Xianchun
AU - Shakouri, Mohsen
AU - Roy, Subrata Chandra
AU - Kanatzidis, Mercouri G.
AU - Arslan, Zikri
AU - Blanton, Alicia
AU - Nie, Jing
AU - Ma, Shulan
AU - Han, Fengxiang X.
AU - Islam, Saiful M.
N1 - Funding Information:
This work was partially supported by the US Department of Energy Minority Serving Institution Partnership Program (MSIPP) managed by the Savannah River National Laboratory under SRNS contract (RFP No. 0000542525 and 0000458357). S.C.R. is thankful to the NSF Division of Chemistry (NSF-2100797). All of the ICP-MS analysis was conducted at JSU’s core research centers supported by RCMI (NIH grant: 1U54MD015929). X-ray Absorption Spectroscopy was performed at the SXRMB beamline of the Canadian Light Source, a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), the Natural Sciences and Engineering Research Council (NSERC), the National Research Council (NRC), the Canadian Institutes of Health Research (CIHR), the Government of Saskatchewan, and the University of Saskatchewan. This work made use of the Keck-II facility of Northwestern University’s NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-2025633), the IIN, and Northwestern’s MRSEC program (NSF DMR-1720139).
Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.
PY - 2022/6/21
Y1 - 2022/6/21
N2 - Removal of chromate (CrO42-) and pertechnetate (TcO4-) from the Hanford Low Activity Waste (LAW) is beneficial as it impacts the cost, life cycle, operational complexity of the Waste Treatment and Immobilization Plant (WTP), and integrity of vitrified glass for nuclear waste disposal. Here, we report the application of [MoIV3S13]2-intercalated layer double hydroxides (LDH-Mo3S13) for the removal of CrO42-as a surrogate for TcO4-, from ppm to ppb levels from water and a simulated LAW off-gas condensate of Hanford's WTP. LDH-Mo3S13removes CrO42-from the LAW condensate stream, having a pH of 7.5, from ppm (∼9.086 × 104ppb of Cr6+) to below 1 ppb levels with distribution constant (Kd) values of up to ∼107mL/g. Analysis of postadsorbed solids indicates that CrO42-removal mainly proceeds by reduction of Cr6+to Cr3+. This study sets the first example of a metal sulfide intercalated LDH for the removal of CrO42-, as relevant to TcO4-, from the simulated off-gas condensate streams of Hanford's LAW melter which contains highly concentrated competitive anions, namely F-, Cl-, CO32-, NO3-, BO33-, NO2-, SO42-, and B4O72-. LDH-Mo3S13's remarkable removal efficiency makes it a promising sorbent to remediate CrO42-/TcO4-from surface water and an off-gas condensate of nuclear waste.
AB - Removal of chromate (CrO42-) and pertechnetate (TcO4-) from the Hanford Low Activity Waste (LAW) is beneficial as it impacts the cost, life cycle, operational complexity of the Waste Treatment and Immobilization Plant (WTP), and integrity of vitrified glass for nuclear waste disposal. Here, we report the application of [MoIV3S13]2-intercalated layer double hydroxides (LDH-Mo3S13) for the removal of CrO42-as a surrogate for TcO4-, from ppm to ppb levels from water and a simulated LAW off-gas condensate of Hanford's WTP. LDH-Mo3S13removes CrO42-from the LAW condensate stream, having a pH of 7.5, from ppm (∼9.086 × 104ppb of Cr6+) to below 1 ppb levels with distribution constant (Kd) values of up to ∼107mL/g. Analysis of postadsorbed solids indicates that CrO42-removal mainly proceeds by reduction of Cr6+to Cr3+. This study sets the first example of a metal sulfide intercalated LDH for the removal of CrO42-, as relevant to TcO4-, from the simulated off-gas condensate streams of Hanford's LAW melter which contains highly concentrated competitive anions, namely F-, Cl-, CO32-, NO3-, BO33-, NO2-, SO42-, and B4O72-. LDH-Mo3S13's remarkable removal efficiency makes it a promising sorbent to remediate CrO42-/TcO4-from surface water and an off-gas condensate of nuclear waste.
KW - Hanford's radioactive waste
KW - chromate
KW - low activity waste
KW - nuclear waste
KW - off-gas condensate stream
KW - pertechnetate
UR - http://www.scopus.com/inward/record.url?scp=85132037852&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85132037852&partnerID=8YFLogxK
U2 - 10.1021/acs.est.1c08766
DO - 10.1021/acs.est.1c08766
M3 - Article
C2 - 35647805
AN - SCOPUS:85132037852
SN - 0013-936X
VL - 56
SP - 8590
EP - 8598
JO - Environmental Science & Technology
JF - Environmental Science & Technology
IS - 12
ER -