Facile, Electrochemical Chlorination of Graphene from an Aqueous NaCl Solution.
basic_science · Level V
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- Record sourced from PubMed, PMID 33448861.
- Also identified by DOI 10.1021/acs.nanolett.0c04641.
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Abstract
We report a facile approach to directly chlorinate graphene from an aqueous sodium chloride solution under ambient conditions. By applying a moderate anodic voltage to substrate-supported monolayer graphene, the resultant chlorine radicals generated at the graphene surface enable efficient chlorination: X-ray photoelectron spectrum confirms the formation of C-Cl bonds, and reaction voltage-tunable Cl:C atomic ratios of up to 17% are achieved. In comparison, we find the corresponding electrochemical graphene bromination and iodination reactions much less viable. Electrical and Raman characterizations show substantial <i>p</i>-doping for the chlorinated graphene, yet good basal-plane integrity and electrical properties are maintained. Interference reflection microscopy and pH-dependent experiments next help elucidate the competition between the radical-mediated electrochemical chlorination and oxidation in the process, and rationalize acidic conditions for optimal chlorination. Reaction in a mixed NaCl-NaN<sub>3</sub> solution shows the electrochemical chlorination to be fully suppressed by azidation, yet a sequential, two-step chlorination-azidation approach permits facile bifunctionalization.