Atomically Dispersed Iron-Nitrogen Sites on Hierarchically Mesoporous Carbon Nanotube and Graphene Nanoribbon Networks for CO2 Reduction
Document Type
Article
Publication Date
5-26-2020
Department
Department of Materials Science and Engineering
Abstract
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.
Publication Title
ACS Nano
Recommended Citation
Pan, F.,
Li, B.,
Sarnello, E.,
Fei, Y.,
Gang, Y.,
Xiang, X.,
Du, Z.,
Zhang, P.,
Wang, G.,
Nguyen, H.,
Li, T.,
Hu, Y. H.,
Zhou, H.,
&
Li, Y.
(2020).
Atomically Dispersed Iron-Nitrogen Sites on Hierarchically Mesoporous Carbon Nanotube and Graphene Nanoribbon Networks for CO2 Reduction.
ACS Nano,
14(5), 5506-5516.
http://doi.org/10.1021/acsnano.9b09658
Retrieved from: https://digitalcommons.mtu.edu/michigantech-p/2014
Publisher's Statement
© 2020 American Chemical Society. Publisher’s version of record: https://doi.org/10.1021/acsnano.9b09658