Статья

Efficient Uranium Capture by Polysulfide/Layered Double Hydroxide Composites

Shulan MaBeijing Key Laboratory of Energy Conversion and Storage Materials, College of Chemistry, Beijing Normal University, Beijing 100875, ChinaLu HuangBeijing Key Laboratory of Energy Conversion and Storage Materials, College of Chemistry, Beijing Normal University, Beijing 100875, ChinaLijiao MaBeijing Key Laboratory of Energy Conversion and Storage Materials, College of Chemistry, Beijing Normal University, Beijing 100875, ChinaYurina ShimDepartment of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United StatesSaiful M. IslamDepartment of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United StatesPengli WangDepartment of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United StatesLi‐Dong ZhaoDepartment of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United StatesShichao WangDepartment of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United StatesGenban SunBeijing Key Laboratory of Energy Conversion and Storage Materials, College of Chemistry, Beijing Normal University, Beijing 100875, ChinaXiaojing YangBeijing Key Laboratory of Energy Conversion and Storage Materials, College of Chemistry, Beijing Normal University, Beijing 100875, ChinaMercouri G. KanatzidisDepartment of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States

2015en

ABI

Аннотация

There is a need to develop highly selective and efficient materials for capturing uranium (normally as UO2(2+)) from nuclear waste and from seawater. We demonstrate the promising adsorption performance of S(x)-LDH composites (LDH is Mg/Al layered double hydroxide, [S(x)](2-) is polysulfide with x = 2, 4) for uranyl ions from a variety of aqueous solutions including seawater. We report high removal capacities (q(m) = 330 mg/g), large K(d)(U) values (10(4)-10(6) mL/g at 1-300 ppm U concentration), and high % removals (>95% at 1-100 ppm, or ∼80% for ppb level seawater) for UO2(2+) species. The S(x)-LDHs are exceptionally efficient for selectively and rapidly capturing UO2(2+) both at high (ppm) and trace (ppb) quantities from the U-containing water including seawater. The maximum adsorption coeffcient value K(d)(U) of 3.4 × 10(6) mL/g (using a V/m ratio of 1000 mL/g) observed is among the highest reported for U adsorbents. In the presence of very high concentrations of competitive ions such as Ca(2+)/Na(+), S(x)-LDH exhibits superior selectivity for UO2(2+), over previously reported sorbents. Under low U concentrations, (S4)(2-) coordinates to UO2(2+) forming anionic complexes retaining in the LDH gallery. At high U concentrations, (S4)(2-) binds to UO2(2+) to generate neutral UO2S4 salts outside the gallery, with NO3(-) entering the interlayer to form NO3-LDH. In the presence of high Cl(-) concentration, Cl(-) preferentially replaces [S4](2-) and intercalates into LDH. Detailed comparison of U removal efficiency of S(x)-LDH with various known sorbents is reported. The excellent uranium adsorption ability along with the environmentally safe, low-cost constituents points to the high potential of S(x)-LDH materials for selective uranium capture.

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Идентификаторы

DOI: 10.1021/jacs.5b00762

Цитирования и источники

Цитирований: 2Использованных источников: 0

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