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Title: Aryl Diazonium-Assisted Amidoximation of MXene for Boosting Water Stability and Uranyl Sequestration via Electrochemical Sorption

Abstract

Despite that two-dimensional transition metal carbides and carbonitrides (MXenes) are burgeoning candidates for remediation of environmental pollutants, the construction of robust functionalized MXene nanosheets with a high affinity for target heavy metal ions and radionuclides remains a challenge. Here we report the successful placement of amidoxime chelating groups on Ti3C2Tx MXene surface by diazonium salt grafting. The introduction of amidoxime functional groups significantly enhances the selectivity of Ti3C2Tx nanosheets for uranyl ions and also greatly improves their stability in aqueous solution, enabling efficient, rapid, and recyclable uranium extraction from aqueous solutions containing competitive metal ions. Benefiting from the excellent conductivity of MXenes, the amidoxime functionalized Ti3C2Tx nanosheets show outstanding electrochemical performance such that when loaded on carbon cloth the application of an electric field increases the uranium adsorption capacity from 294 to 626 mg/g, outperforming all organic electrochemical sorption materials reported previously. Finally, the present work provides an effective strategy to functionalize MXene nanosheets with fundamental implications for the design of MXene-based selective electrosorption electrode materials.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [2];  [2];  [2];  [2];  [2]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2];  [2];  [4];  [2]; ORCiD logo [2]
+ Show Author Affiliations
  1. Chinese Academy of Sciences (CAS), Beijing (China); Univ. of South China, Hengyang (China)
  2. Chinese Academy of Sciences (CAS), Beijing (China)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Univ. of South China, Hengyang (China)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES), Chemical Sciences, Geosciences & Biosciences Division; National Natural Science Foundation of China (NSFC); National Science Fund for Distinguished Young Scholars
OSTI Identifier:
1642684
Grant/Contract Number:  
AC02-05CH11231; 11675192; 21836001; 21777161; 21577144; 21925603; TZ
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 12; Journal Issue: 13; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; MXene; amidoxime group; diazonium salt; uranium capture

Citation Formats

Zhang, Pengcheng, Wang, Lin, Huang, Zhiwei, Yu, Jipan, Li, Zijie, Deng, Hao, Yin, Taiqi, Yuan, Liyong, Gibson, John K., Mei, Lei, Zheng, Lirong, Wang, Hongqing, Chai, Zhifang, and Shi, Weiqun. Aryl Diazonium-Assisted Amidoximation of MXene for Boosting Water Stability and Uranyl Sequestration via Electrochemical Sorption. United States: N. p., 2020. Web. doi:10.1021/acsami.0c00861.
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Zhang, Pengcheng, Wang, Lin, Huang, Zhiwei, Yu, Jipan, Li, Zijie, Deng, Hao, Yin, Taiqi, Yuan, Liyong, Gibson, John K., Mei, Lei, Zheng, Lirong, Wang, Hongqing, Chai, Zhifang, & Shi, Weiqun. Aryl Diazonium-Assisted Amidoximation of MXene for Boosting Water Stability and Uranyl Sequestration via Electrochemical Sorption. United States. https://doi.org/10.1021/acsami.0c00861
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Zhang, Pengcheng, Wang, Lin, Huang, Zhiwei, Yu, Jipan, Li, Zijie, Deng, Hao, Yin, Taiqi, Yuan, Liyong, Gibson, John K., Mei, Lei, Zheng, Lirong, Wang, Hongqing, Chai, Zhifang, and Shi, Weiqun. Mon . "Aryl Diazonium-Assisted Amidoximation of MXene for Boosting Water Stability and Uranyl Sequestration via Electrochemical Sorption". United States. https://doi.org/10.1021/acsami.0c00861. https://www.osti.gov/servlets/purl/1642684.
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@article{osti_1642684,
title = {Aryl Diazonium-Assisted Amidoximation of MXene for Boosting Water Stability and Uranyl Sequestration via Electrochemical Sorption},
author = {Zhang, Pengcheng and Wang, Lin and Huang, Zhiwei and Yu, Jipan and Li, Zijie and Deng, Hao and Yin, Taiqi and Yuan, Liyong and Gibson, John K. and Mei, Lei and Zheng, Lirong and Wang, Hongqing and Chai, Zhifang and Shi, Weiqun},
abstractNote = {Despite that two-dimensional transition metal carbides and carbonitrides (MXenes) are burgeoning candidates for remediation of environmental pollutants, the construction of robust functionalized MXene nanosheets with a high affinity for target heavy metal ions and radionuclides remains a challenge. Here we report the successful placement of amidoxime chelating groups on Ti3C2Tx MXene surface by diazonium salt grafting. The introduction of amidoxime functional groups significantly enhances the selectivity of Ti3C2Tx nanosheets for uranyl ions and also greatly improves their stability in aqueous solution, enabling efficient, rapid, and recyclable uranium extraction from aqueous solutions containing competitive metal ions. Benefiting from the excellent conductivity of MXenes, the amidoxime functionalized Ti3C2Tx nanosheets show outstanding electrochemical performance such that when loaded on carbon cloth the application of an electric field increases the uranium adsorption capacity from 294 to 626 mg/g, outperforming all organic electrochemical sorption materials reported previously. Finally, the present work provides an effective strategy to functionalize MXene nanosheets with fundamental implications for the design of MXene-based selective electrosorption electrode materials.},
doi = {10.1021/acsami.0c00861},
journal = {ACS Applied Materials and Interfaces},
number = 13,
volume = 12,
place = {United States},
year = {Mon Mar 09 00:00:00 EDT 2020},
month = {Mon Mar 09 00:00:00 EDT 2020}
}
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https://doi.org/10.1021/acsami.0c00861
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