Asymmetric Activation of the Nitro Group over a Ag/Graphene Heterointerface to Boost Highly Selective Electrocatalytic Reduction of Nitrobenzene.

ACS Appl Mater Interfaces

Shanghai Electrochemical Energy Devices Research Center, School of Chemistry and Chemical Engineering and State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University Shanghai, Shanghai 200240, P. R. China.

Published: June 2022

The electrocatalytic reduction of nitrobenzene to aniline normally faces high overpotential and poor selectivity because of its six-electron redox nature. Herein, a Ag nanoparticles/laser-induced-graphene (LIG) heterointerface was fabricated on polyimide films and employed as an electrode material for an efficient nitrobenzene reduction reaction (NBRR) via a one-step laser direct writing technology. The first-principles calculations reveal that Ag/LIG shows the lowest activation barriers for the NBRR, which could be attributed to the optimum adsorption of the H atom realized by the appropriate interaction between Ag/LIG heterointerfaces and nitrobenzene. As a result, the overpotential of the NBRR is reduced by 217 mV after silver loading, and Ag/LIG shows a high aniline selectivity of 93%. Furthermore, an electrochemical reduction of nitrobenzene in tandem with an electrochemical oxidative polymerization of aniline was designed to serve as an alternative method to remove nitrobenzene from the aqueous solution. This strategy highlights the significance of heterointerfaces for efficient electrocatalysts, which may stimulate the development of novel electrocatalysts to boost the electrocatalytic activity.

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http://dx.doi.org/10.1021/acsami.2c04533DOI Listing

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