title: Zirconium-Based Metal-Organic Framework for Removal of Perrhenate from Water.
abstract: The efficient removal of pertechnetate (TcO4(-)) anions from liquid waste or melter off-gas solution for an alternative treatment is one of the promising options to manage (99)Tc in legacy nuclear waste. Safe immobilization of (99)Tc is of major importance because of its long half-life (t1/2 = 2.13 × 10(5) yrs) and environmental mobility. Different types of inorganic and solid-state ion-exchange materials have been shown to absorb TcO4(-) anions from water. However, both high capacity and selectivity have yet to be achieved in a single material. Herein, we show that a protonated version of an ultrastable zirconium-based metal-organic framework can adsorb perrhenate (ReO4(-)) anions, a nonradioactive surrogate for TcO4(-), from water even in the presence of other common anions. Synchrotron-based powder X-ray diffraction and molecular simulations were used to identify the position of the adsorbed ReO4(-) (surrogate for TcO4(-)) molecule within the framework.
authors: Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
authors: Debasis
authors: D
authors: Banerjee
authors: X-ray Science Division, Advanced Photon Source, Argonne National Laboratory , Argonne, Illinois 60439, United States.
authors: Wenqian
authors: W
authors: Xu
authors: Energy and Environment Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
authors: Zimin
authors: Z
authors: Nie
authors: Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
authors: Lewis E V
authors: LE
authors: Johnson
authors: Department of Chemistry, The University of Adelaide , Adelaide, South Australia 5005, Australia.
authors: Campbell
authors: C
authors: Coghlan
authors: Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
authors: Maria L
authors: ML
authors: Sushko
authors: Energy and Environment Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
authors: Dongsang
authors: D
authors: Kim
authors: Energy and Environment Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
authors: Michael J
authors: MJ
authors: Schweiger
authors: Office of River Protection, U.S. Department of Energy , Richland, Washington 99352, United States.
authors: Albert A
authors: AA
authors: Kruger
authors: Department of Chemistry, The University of Adelaide , Adelaide, South Australia 5005, Australia.
authors: Christian J
authors: CJ
authors: Doonan
authors: Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
authors: Praveen K
authors: PK
authors: Thallapally