Covalent Organic Frameworks as a Decorating Platform for Utilization and Affinity Enhancement of Chelating Sites for Radionuclide Sequestration

Advanced Materials - Tập 30 Số 20 - 2018
Qi Sun1, Briana Aguila1, Lyndsey D. Earl2, Carter W. Abney2, Łukasz Wojtas1, Praveen K. Thallapally3, Shengqian Ma1
1Department of Chemistry, University of South Florida, 4202 E. Fowler Avenue, Tampa, FL, 33620, USA
2Chemical Sciences Division, Oak Ridge National Laboratory, P.O. Box 2008, Oak Ridge, TN 37831, USA
3Physical and Computational Science Directorate, Pacific Northwest National Laboratory, Richland, WA 99352, USA

Tóm tắt

AbstractThe potential consequences of nuclear events and the complexity of nuclear waste management motivate the development of selective solid‐phase sorbents to provide enhanced protection. Herein, it is shown that 2D covalent organic frameworks (COFs) with unique structures possess all the traits to be well suited as a platform for the deployment of highly efficient sorbents such that they exhibit remarkable performance, as demonstrated by uranium capture. The chelating groups laced on the open 1D channels exhibit exceptional accessibility, allowing significantly higher utilization efficiency. In addition, the 2D extended polygons packed closely in an eclipsed fashion bring chelating groups in adjacent layers parallel to each other, which may facilitate their cooperation, thereby leading to high affinity toward specific ions. As a result, the amidoxime‐functionalized COFs far outperform their corresponding amorphous analogs in terms of adsorption capacities, kinetics, and affinities. Specifically, COF‐TpAb‐AO is able to reduce various uranium contaminated water samples from 1 ppm to less than 0.1 ppb within several minutes, well below the drinking water limit (30 ppb), as well as mine uranium from spiked seawater with an exceptionally high uptake capacity of 127 mg g−1. These results delineate important synthetic advances toward the implementation of COFs in environmental remediation.

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Tài liệu tham khảo

10.1038/532435a

10.1038/nchem.1880

10.1002/anie.201307825

10.1038/nenergy.2017.7

10.1002/anie.201700919

10.1021/acs.chemrev.7b00355

10.1039/C5CS00330J

10.1021/cr990114x

10.1002/adma.200702055

10.1021/es202816c

10.1021/jacs.6b03106

10.1002/anie.200906397

10.1002/anie.201510712

10.1038/35071173

10.1021/es049201j

10.1021/jacs.5b00762

10.1021/ja510488r

10.1002/adma.201401376

10.1021/acs.chemmater.6b04273

10.1021/cm501894h

10.1039/C6DT01318J

10.1016/j.jcis.2005.09.045

10.1039/C6RA06807C

10.1021/am201204r

10.1021/acsami.7b01711

10.1039/C6TA10824E

10.1039/c3sc50230a

10.1039/c3cc44983a

10.1039/C4TA04878D

10.1021/acsami.6b11332

10.1126/science.1120411

10.1039/c2cs35157a

10.1039/C2CS35072F

10.1038/s41570-017-0056

10.1021/jacs.6b01244

10.1021/jacs.6b12005

10.1021/jacs.6b00652

10.1021/acscentsci.7b00127

10.1126/science.aaa8075

10.1021/acs.chemrev.6b00439

10.1021/jacs.6b12885

10.1021/jacs.6b12328

10.1021/jacs.5b04147

10.1021/jacs.7b04096

10.1002/adma.201603006

10.1021/jacs.7b02648

10.1021/jacs.7b00925

10.1021/jacs.7b03204

10.1002/anie.201509014

10.1002/adma.201505004

10.1021/jacs.6b10316

10.1021/jacs.6b08803

10.1126/science.aac8343

10.1038/nchem.2352

10.1021/ja206846p

10.1021/jacs.6b10629

10.1021/jacs.6b07714

10.1073/pnas.1221824110

10.1021/ja509551m

10.1021/jacs.6b07351

10.1021/acsami.6b09681

10.1021/ja5087563

10.1021/jp408460x

10.1039/C5EE02913A

10.1021/ja308278w

10.1039/C6QM00363J

10.1016/j.cej.2016.04.013

10.1021/ic300062s

10.1039/C4CC06370H

10.1021/ja308028n

10.1103/PhysRevB.71.094110

10.1016/j.cpc.2008.12.020

10.1016/j.cpc.2012.02.002

10.1088/0953-8984/26/5/055401

10.1063/1.4978500

10.1016/j.cpc.2008.12.020

10.1038/nchem.1856

10.1021/acsami.6b15968

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Advanced Materials

Tập 30 Số 20

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