Atomically dispersed
metal and nitrogen co-doped carbon (M-N/C)
catalysts hold great promise for electrochemical CO2 conversion.
However, there is a lack of cost-effective synthesis approaches to
meet the goal of economic mass production of single-atom M-N/C with
desirable carbon support architecture for efficient CO2 reduction. Herein, we report facile transformation of commercial
carbon nanotube (CNT) into isolated Fe–N4 sites
anchored on carbon nanotube and graphene nanoribbon (GNR) networks
(Fe-N/CNT@GNR). The oxidization-induced partial unzipping of CNT results
in the generation of GNR nanolayers attached to the remaining fibrous
CNT frameworks, which reticulates a hierarchically mesoporous complex
and thus enables a high electrochemical active surface area and smooth
mass transport. The Fe residues originating from CNT growth seeds
serve as Fe sources to form isolated Fe–N4 moieties
located at the CNT and GNR basal plane and edges with high intrinsic
capability of activating CO2 and suppressing hydrogen evolution.
The Fe-N/CNT@GNR delivers a stable CO Faradaic efficiency of 96% with
a partial current density of 22.6 mA cm–2 at a low
overpotential of 650 mV, making it one of the most active M-N/C catalysts
reported. This work presents an effective strategy to fabricate advanced
atomistic catalysts and highlights the key roles of support architecture
in single-atom electrocatalysis.
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