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Title: Enrichment and Distribution of Pb 2+ Ions in Zwitterionic Poly(cysteine methacrylate) Brushes at the Solid–Liquid Interface

Abstract

Cysteine-based polyzwitterionic brushes have been prepared via a two-step route. First, poly(allyl methacrylate) (PAMA) brushes have been grown from the surface of silicon substrates using surface-initiated atom transfer radical polymerization. The obtained PAMA brushes with free pendant vinyl groups were further modified via radical thiol-ene addition reaction to attach L-cysteine moieties. Surface zeta potential investigations on pH-responsiveness of these poly(cysteine methacrylate) (PCysMA) brushes confirm their zwitterionic character at intermediate pH range, while at pH values either below pH 3.50 or above pH 8.59, they exhibit polyelectrolyte character. Under acid (pH < 3.50) or base (pH > 8.59) conditions, they possess either cationic or anionic character, respectively. In the zwitterionic region, these PCysMA brushes show positive surface $$\zeta$$ potential in the presence of Pb(CH 3COO) 2 solutions of various concentrations. The results are in line with microscopic investigations using anomalous X-ray reflectivity (AXRR) carried out along the absorption edge of Pb 2+ ions. When the photon energies were varied around the absorption L3 edge of lead (13037 eV), the Pb 2+ concentration normal to the silicon substrates, as a function of depth inside PCysMA brushes, could be revealed at the nanoscale. Both zeta potential and AXRR measurements confirm the enrichment of Pb 2+ ions inside PCysMA brushes, indicating the potential of PCysMA to be used as a water purification material.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [2];  [2];  [2];  [3]; ORCiD logo [2]; ORCiD logo [1];  [1]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Org.:
Energy Frontier Research Center (EFRC)
OSTI Identifier:
1595945
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Langmuir
Additional Journal Information:
Journal Volume: 35; Journal Issue: 52; Journal ID: ISSN 0743-7463
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

He, Qiming, Qiao, Yijun, Mandia, David J., Gan, Shenglong, Zhang, Huiru, Zhou, Hua, Elam, Jeffrey W., Darling, Seth B., Tirrell, Matthew V., and Chen, Wei. Enrichment and Distribution of Pb2+ Ions in Zwitterionic Poly(cysteine methacrylate) Brushes at the Solid–Liquid Interface. United States: N. p., 2019. Web. doi:10.1021/acs.langmuir.9b02770.
He, Qiming, Qiao, Yijun, Mandia, David J., Gan, Shenglong, Zhang, Huiru, Zhou, Hua, Elam, Jeffrey W., Darling, Seth B., Tirrell, Matthew V., & Chen, Wei. Enrichment and Distribution of Pb2+ Ions in Zwitterionic Poly(cysteine methacrylate) Brushes at the Solid–Liquid Interface. United States. doi:10.1021/acs.langmuir.9b02770.
He, Qiming, Qiao, Yijun, Mandia, David J., Gan, Shenglong, Zhang, Huiru, Zhou, Hua, Elam, Jeffrey W., Darling, Seth B., Tirrell, Matthew V., and Chen, Wei. Mon . "Enrichment and Distribution of Pb2+ Ions in Zwitterionic Poly(cysteine methacrylate) Brushes at the Solid–Liquid Interface". United States. doi:10.1021/acs.langmuir.9b02770.
@article{osti_1595945,
title = {Enrichment and Distribution of Pb2+ Ions in Zwitterionic Poly(cysteine methacrylate) Brushes at the Solid–Liquid Interface},
author = {He, Qiming and Qiao, Yijun and Mandia, David J. and Gan, Shenglong and Zhang, Huiru and Zhou, Hua and Elam, Jeffrey W. and Darling, Seth B. and Tirrell, Matthew V. and Chen, Wei},
abstractNote = {Cysteine-based polyzwitterionic brushes have been prepared via a two-step route. First, poly(allyl methacrylate) (PAMA) brushes have been grown from the surface of silicon substrates using surface-initiated atom transfer radical polymerization. The obtained PAMA brushes with free pendant vinyl groups were further modified via radical thiol-ene addition reaction to attach L-cysteine moieties. Surface zeta potential investigations on pH-responsiveness of these poly(cysteine methacrylate) (PCysMA) brushes confirm their zwitterionic character at intermediate pH range, while at pH values either below pH 3.50 or above pH 8.59, they exhibit polyelectrolyte character. Under acid (pH < 3.50) or base (pH > 8.59) conditions, they possess either cationic or anionic character, respectively. In the zwitterionic region, these PCysMA brushes show positive surface $\zeta$ potential in the presence of Pb(CH3COO)2 solutions of various concentrations. The results are in line with microscopic investigations using anomalous X-ray reflectivity (AXRR) carried out along the absorption edge of Pb2+ ions. When the photon energies were varied around the absorption L3 edge of lead (13037 eV), the Pb2+ concentration normal to the silicon substrates, as a function of depth inside PCysMA brushes, could be revealed at the nanoscale. Both zeta potential and AXRR measurements confirm the enrichment of Pb2+ ions inside PCysMA brushes, indicating the potential of PCysMA to be used as a water purification material.},
doi = {10.1021/acs.langmuir.9b02770},
journal = {Langmuir},
number = 52,
volume = 35,
place = {United States},
year = {2019},
month = {12}
}

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This content will become publicly available on December 2, 2020
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