title: Highly Sensitive and Selective Uranium Detection in Natural Water Systems Using a Luminescent Mesoporous Metal-Organic Framework Equipped with Abundant Lewis Basic Sites: A Combined Batch, X-ray Absorption Spectroscopy, and First Principles Simulation Investigation.
abstract: Uranium is not only a strategic resource for the nuclear industry but also a global contaminant with high toxicity. Although several strategies have been established for detecting uranyl ions in water, searching for new uranium sensor material with great sensitivity, selectivity, and stability remains a challenge. We introduce here a hydrolytically stable mesoporous terbium(III)-based MOF material compound 1, whose channels are as large as 27 Å × 23 Å and are equipped with abundant exposed Lewis basic sites, the luminescence intensity of which can be efficiently and selectively quenched by uranyl ions. The detection limit in deionized water reaches 0.9 μg/L, far below the maximum contamination standard of 30 μg/L in drinking water defined by the United States Environmental Protection Agency, making compound 1 currently the only MOF material that can achieve this goal. More importantly, this material exhibits great capability in detecting uranyl ions in natural water systems such as lake water and seawater with pH being adjusted to 4, where huge excesses of competing ions are present. The uranyl detection limits in Dushu Lake water and in seawater were calculated to be 14.0 and 3.5 μg/L, respectively. This great detection capability originates from the selective binding of uranyl ions onto the Lewis basic sites of the MOF material, as demonstrated by synchrotron radiation extended X-ray adsorption fine structure, X-ray adsorption near edge structure, and first principles calculations, further leading to an effective energy transfer between the uranyl ions and the MOF skeleton.
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , 199 Ren'ai Road, Suzhou 215123, P. R. China.
authors.forename: Wei
authors.initials: W
authors.lastname: Liu
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , 199 Ren'ai Road, Suzhou 215123, P. R. China.
authors.forename: Xing
authors.initials: X
authors.lastname: Dai
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , 199 Ren'ai Road, Suzhou 215123, P. R. China.
authors.forename: Zhuanling
authors.initials: Z
authors.lastname: Bai
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , 199 Ren'ai Road, Suzhou 215123, P. R. China.
authors.forename: Yanlong
authors.initials: Y
authors.lastname: Wang
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , 199 Ren'ai Road, Suzhou 215123, P. R. China.
authors.forename: Zaixing
authors.identifier: 0000-0003-3521-6867
authors.initials: Z
authors.lastname: Yang
authors.affiliation: Shanghai Institute of Applied Physics and Key Laboratory of Nuclear Radiation and Nuclear Energy Technology, Chinese Academy of Sciences , Shanghai 201800, P. R. China.
authors.forename: Linjuan
authors.initials: L
authors.lastname: Zhang
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , 199 Ren'ai Road, Suzhou 215123, P. R. China.
authors.forename: Lin
authors.initials: L
authors.lastname: Xu
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , 199 Ren'ai Road, Suzhou 215123, P. R. China.
authors.forename: Lanhua
authors.initials: L
authors.lastname: Chen
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , 199 Ren'ai Road, Suzhou 215123, P. R. China.
authors.forename: Yuxiang
authors.initials: Y
authors.lastname: Li
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , 199 Ren'ai Road, Suzhou 215123, P. R. China.
authors.forename: Daxiang
authors.initials: D
authors.lastname: Gui
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , 199 Ren'ai Road, Suzhou 215123, P. R. China.
authors.forename: Juan
authors.initials: J
authors.lastname: Diwu
authors.affiliation: Shanghai Institute of Applied Physics and Key Laboratory of Nuclear Radiation and Nuclear Energy Technology, Chinese Academy of Sciences , Shanghai 201800, P. R. China.
authors.forename: Jianqiang
authors.initials: J
authors.lastname: Wang
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , 199 Ren'ai Road, Suzhou 215123, P. R. China.|Computational Biology Center, IBM Thomas J Watson Research Center , Yorktown Heights, New York 10598, United States.|Department of Chemistry, Columbia University , New York, New York 10027, United States.
authors.forename: Ruhong
authors.identifier: 0000-0001-8624-5591
authors.initials: R
authors.lastname: Zhou
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , 199 Ren'ai Road, Suzhou 215123, P. R. China.
authors.forename: Zhifang
authors.initials: Z
authors.lastname: Chai
authors.affiliation: School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University , 199 Ren'ai Road, Suzhou 215123, P. R. China.
authors.forename: Shuao
authors.identifier: 0000-0002-1526-1102
authors.initials: S
authors.lastname: Wang
mesh_terms: D058115:Lewis Bases; D049449:Luminescence; D014501:Uranium / Q000737:chemistry*; D014867:Water / Q000737:chemistry; D056928:X-Ray Absorption Spectroscopy
chemical_list: D058115:Lewis Bases; D014867:Water; D014501:Uranium