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Three Mechanisms in One Material: Uranium Capture by a Polyoxometalate–Organic Framework through Combined Complexation, Chemical Reduction, and Photocatalytic Reduction
Author(s) -
Zhang Hailong,
Liu Wei,
Li Ao,
Zhang Duo,
Li Xiaoyan,
Zhai Fuwan,
Chen Lanhua,
Chen Long,
Wang Yanlong,
Wang Shuao
Publication year - 2019
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201909718
Subject(s) - sorbent , uranium , sorption , polyoxometalate , x ray photoelectron spectroscopy , xanes , photocatalysis , adsorption , chemical stability , chemistry , uranyl , inorganic chemistry , nuclear chemistry , ligand (biochemistry) , selectivity , materials science , chemical engineering , catalysis , spectroscopy , organic chemistry , biochemistry , physics , receptor , quantum mechanics , engineering , metallurgy
Abstract The design and synthesis of uranium sorbent materials with high uptake efficiency, capacity and selectivity, as well as excellent hydrolytic stability and radiation resistance remains a challenge. Herein, a polyoxometalate (POM)–organic framework material ( SCU‐19 ) with a rare inclined polycatenation structure was designed, synthesized through a solvothermal method, and tested for uranium separation. Under dark conditions, SCU‐19 can efficiently capture uranium through ligand complexation using its exposed oxo atoms and partial chemical reduction from U VI to U IV by the low‐valent Mo atoms in the POM. An additional U VI photocatalytic reduction mechanism can occur under visible light irradiation, leading to a higher uranium removal without saturation and faster sorption kinetics. SCU‐19 is the only uranium sorbent material with three distinct sorption mechanisms, as further demonstrated by X‐ray photoelectron spectroscopy (XPS) and X‐ray absorption near edge structure (XANES) analysis.