Ultrastable Zirconium-Based Cationic Metal-Organic Frameworks for Perrhenate Removal from Wastewater

TY - JOUR

T1 - Ultrastable Zirconium-Based Cationic Metal-Organic Frameworks for Perrhenate Removal from Wastewater

AU - Zhang, Guoyu

AU - Tan, Kui

AU - Xian, Shikai

AU - Xing, Kai

AU - Sun, Hongbing

AU - Hall, Gene

AU - Li, Liangying

AU - Li, Jing

N1 - Funding Information: We are grateful for financial support from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award DE-SC0019902. Publisher Copyright: ©

PY - 2021/8/16

Y1 - 2021/8/16

N2 - The effective removal of radioactive 99TcO4- anion from nuclear wastewater remains a very difficult unsolved problem. Functional adsorbent materials with high stability, anion-exchange capacity, excellent selectivity, and recyclability are much needed to solve this problem. In this work, we designed two stable cationic metal-organic frameworks (MOFs)-Zr-tcbp-Me and Zr-tcpp-Me-for possible use as adsorbent materials to remove 99TcO4-. Both compounds were synthesized by solvothermal reactions of the tetracarboxylate ligand with zirconium salt, followed by postsynthetic modification (N-methylation). The crystallinity of both zirconium-based MOFs can be well retained under harsh conditions, and they exhibit high adsorption capacity and selectivity toward ReO4- anion, a nonradioactive analogue of 99TcO4-. Zr-tcbp-Me and Zr-tcpp-Me demonstrate the highest framework stability toward acidity among all previously reported cationic MOFs that have been tested for perrhenate removal from wastewater.

AB - The effective removal of radioactive 99TcO4- anion from nuclear wastewater remains a very difficult unsolved problem. Functional adsorbent materials with high stability, anion-exchange capacity, excellent selectivity, and recyclability are much needed to solve this problem. In this work, we designed two stable cationic metal-organic frameworks (MOFs)-Zr-tcbp-Me and Zr-tcpp-Me-for possible use as adsorbent materials to remove 99TcO4-. Both compounds were synthesized by solvothermal reactions of the tetracarboxylate ligand with zirconium salt, followed by postsynthetic modification (N-methylation). The crystallinity of both zirconium-based MOFs can be well retained under harsh conditions, and they exhibit high adsorption capacity and selectivity toward ReO4- anion, a nonradioactive analogue of 99TcO4-. Zr-tcbp-Me and Zr-tcpp-Me demonstrate the highest framework stability toward acidity among all previously reported cationic MOFs that have been tested for perrhenate removal from wastewater.

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U2 - 10.1021/acs.inorgchem.1c00512

DO - 10.1021/acs.inorgchem.1c00512

M3 - Article

C2 - 33872495

SN - 0020-1669

VL - 60

SP - 11730

EP - 11738

JO - Inorganic Chemistry

JF - Inorganic Chemistry

IS - 16

ER -