文献类型：期刊文献

英文题名：Successful Coupling of a Bis-Amidoxime Uranophile with a Hydrophilic Backbone for Selective Uranium Sequestration

作者：Piechowicz, Marek[1];Abney, Carter W.[2];Thacker, Nathan C.[1];Gilhula, James C.[1];Wang, Youfu[1,3];Veroneau, Samuel S.[1];Hu, Aiguo[3];Lin, Wenbin[1]

机构：[1]Univ Chicago, Dept Chem, 929 E 57th St, Chicago, IL 60637 USA;[2]Oak Ridge Natl Lab, POB 2008,MS-6201, Oak Ridge, TN 37831 USA;[3]East China Univ Sci & Technol, Sch Mat Sci & Engn, Shanghai Key Lab Adv Polymer Mat, Shanghai 200237, Peoples R China

年份：2017

卷号：9

期号：33

起止页码：27894

外文期刊名：ACS APPLIED MATERIALS & INTERFACES

收录：;EI(收录号：20173504087648);WOS:【SCI-EXPANDED(收录号:WOS:000408518800062)】；

基金：This work was supported by the DOE Office of Nuclear Energy's Nuclear Energy University Program (Sub-Contract-20 No. 120427, Project No. 3151). Work at Oak Ridge National Laboratory was sponsored by the U.S. DOE, Office of Nuclear Energy. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. The authors also thank Dan Micheroni, Zekai Lin, and Chris Poon for experimental assistance; Keene Zhang for stimulating discussion; and Isabel Piechowicz for graphic design. We acknowledge the University of Chicago Research Computing Center, the Nuclear Magnetic Resonance Facility, and NSF instrumentation grant CHE-1048528 in conjunction with the Mass Spectrometry Facility for support of this work. The United States Government retains, and by accepting the article for publication the publisher acknowledges that the United States Government retains, a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript or allow others to do so, for the United States Government Purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).

语种：英文

外文关键词：amidoxime; uranium extraction; seawater; cooperative binding; DFT

摘要：The amidoxime group (-RNH2NOH) has long been used to extract uranium from seawater on account of its high affinity toward uranium. The development of tunable sorbent materials for uranium sequestration remains a research priority as well as a significant challenge. Herein, we report the design, synthesis, and uranium sorption properties of bis-amidoxime-functionalized polymeric materials (BAP 1-3). Bifunctional amidoxime monomers were copolymerized with an acrylamide cross-linker to obtain bis-amidoxime incorporation as high as 2 mmol g(-1) after five synthetic steps. The resulting sorbents were able to uptake nearly 600 mg of uranium per gram of polymer after 37 days of contact with a seawater simulant containing 8 ppm uranium. Moreover, the polymeric materials exhibited low vanadium uptake with a maximum capacity of 128 mg of vanadium per gram of polymer. This computationally predicted and experimentally realized selectivity of uranium over vanadium, nearly 5 to 1 w/w, is one of the highest reported to date and represents an advancement in the rational design of sorbent materials with high uptake capacity and selectivity.