Analysis of competitive binding of several metal cations by graphene oxide reveals the quantity and spatial distribution of carboxyl groups on its surface

Physical Chemistry Chemical Physics : PCCP
Rustem R AmirovAyrat M Dimiev

Abstract

The sorption capacity of graphene oxide (GO) toward different metal cations has been the subject of several recent studies. However, the reported quantitative data are controversial, and the mechanism of chemical bonding between GO and metal cations is poorly understood. Clarifying these questions can eventually help to reveal the fine chemical structure of GO that remains ambiguous. In this work, we study the binding of Gd3+ and Mn2+ by GO in the presence of several competing metal cations by the 1H NMR relaxation method. As a general trend, the efficiency of the metal cations to bind to GO increases with ionic charge, and depends on their ability to form coordinate-covalent bonds with GO oxygen groups. The efficiency of the competing metal cations to "replace" Gd3+ and Mn2+ increases in the order Na+ < Cs+ < Ca2+ < Sr2+ < Ga3+ < Lu3+. GO contains two different types of binding sites, bonding to which results in either high or low NMR relaxivity of the resulting Gd3+-GO and Mn2+-GO solutions. Gd3+ and Mn2+, being replaced from the high-relaxivity sites by the large excess of competing cations, are not released into the bulk solution, but only migrate to the low-relaxivity sites, remaining covalently bonded to GO. The absolute ...Continue Reading

References

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Jan 14, 2012·Journal of the American Chemical Society·Ayrat DimievJames M Tour
Jul 25, 2012·Proceedings of the National Academy of Sciences of the United States of America·Adriano AmbrosiMartin Pumera
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Jun 1, 2017·Angewandte Chemie·Fabian GroteSiegfried Eigler

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Citations

Mar 31, 2021·Small·Ravishankar G KadamManoj B Gawande
Aug 6, 2021·Physical Chemistry Chemical Physics : PCCP·Julia ShayimovaAyrat M Dimiev
Oct 30, 2018·ACS Applied Materials & Interfaces·Alexander SolodovAyrat M Dimiev
Sep 10, 2019·Langmuir : the ACS Journal of Surfaces and Colloids·Artur KhannanovAyrat M Dimiev
Sep 10, 2020·ACS Applied Materials & Interfaces·Nicolas BoulangerAlexandr V Talyzin
Nov 10, 2021·The Science of the Total Environment·Md Osim AquatarReddithota J Krupadam

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Methods Mentioned

BETA
NMR

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