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Nitrogen-rich carbon nitride inducing electron delocalization of Co-N4 site to enhance electrocatalytic carbon dioxide reduction by Jofrey Jackson Masana; Jiayong Xiao; Hui Zhang; Xiaoying Lu; Ming Qiu; Ying Yu is a Energy article available to read on EtoBox.

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Cobalt phthalocyanine (CoPc) is an appealing electrocatalyst for CO 2 reduction. However, its catalytic performance is limited by instability and low conductivity. Herein, theoretical calculations reveal that nitrogen-rich carbon nitride, as a promising Supporting material, can help to tune the electronic structure of CoPc and then enhance its stability and conductivity by inducing electron delocalization of Co-N 4 sites for the formation of Co-N 5 , achieving a superior electrochemical reduction of CO 2 . Inspired by this prediction, we prepared nitrogen-rich carbon nitride that coordinated with Co-N 4 through axial N coordination under 400 oC, forming an atomically dispersed Co-N 5 catalytic site. The synthesized catalyst demonstrates excellent performance in CO 2 conversion to CO with >99 % selectivity at a current density of -5.3 mA cm -2 , which can remain for 40 h. These findings provide a strategy for regulating catalytic sites and shed light on expanding the applications of low-cost carbon nitride materials at mild heat-treatment temperatures.

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Author

Jofrey Jackson Masana; Jiayong Xiao; Hui Zhang; Xiaoying Lu; Ming Qiu; Ying Yu

Publisher

Elsevier BV

Published

2023

Language

EN

Field

Energy (Physical Sciences)