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Title: Atomically Dispersed Iron–Nitrogen Sites on Hierarchically Mesoporous Carbon Nanotube and Graphene Nanoribbon Networks for CO2 Reduction

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-N-4 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 supportmore » architecture in single-atom electrocatalysis.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [2];  [3];  [5];  [4]; ORCiD logo [1]; ORCiD logo [1]
  1. Texas A & M Univ., College Station, TX (United States)
  2. Univ. of Pittsburgh, PA (United States)
  3. Northern Illinois Univ., DeKalb, IL (United States)
  4. Michigan Technological Univ., Houghton, MI (United States)
  5. Northern Illinois Univ., DeKalb, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); American Chemical Society - Petroleum Research Fund; USDOE Office of Science (SC); Northern Illinois Univ., DeKalb, IL (United States)
OSTI Identifier:
1670108
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 14; Journal Issue: 5; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 reduction; carbon architecture; nanoribbons; nanotubes; single-atom catalyst

Citation Formats

Pan, Fuping, Li, Boyang, Sarnello, Erik, Fei, Yuhuan, Gang, Yang, Xiang, Xianmei, Du, Zichen, Zhang, Peng, Wang, Guofeng, Nguyen, Hoai T., Li, Tao, Hu, Yun Hang, Zhou, Hong-Cai, and Li, Ying. Atomically Dispersed Iron–Nitrogen Sites on Hierarchically Mesoporous Carbon Nanotube and Graphene Nanoribbon Networks for CO2 Reduction. United States: N. p., 2020. Web. doi:10.1021/acsnano.9b09658.
Pan, Fuping, Li, Boyang, Sarnello, Erik, Fei, Yuhuan, Gang, Yang, Xiang, Xianmei, Du, Zichen, Zhang, Peng, Wang, Guofeng, Nguyen, Hoai T., Li, Tao, Hu, Yun Hang, Zhou, Hong-Cai, & Li, Ying. Atomically Dispersed Iron–Nitrogen Sites on Hierarchically Mesoporous Carbon Nanotube and Graphene Nanoribbon Networks for CO2 Reduction. United States. doi:10.1021/acsnano.9b09658.
Pan, Fuping, Li, Boyang, Sarnello, Erik, Fei, Yuhuan, Gang, Yang, Xiang, Xianmei, Du, Zichen, Zhang, Peng, Wang, Guofeng, Nguyen, Hoai T., Li, Tao, Hu, Yun Hang, Zhou, Hong-Cai, and Li, Ying. Fri . "Atomically Dispersed Iron–Nitrogen Sites on Hierarchically Mesoporous Carbon Nanotube and Graphene Nanoribbon Networks for CO2 Reduction". United States. doi:10.1021/acsnano.9b09658.
@article{osti_1670108,
title = {Atomically Dispersed Iron–Nitrogen Sites on Hierarchically Mesoporous Carbon Nanotube and Graphene Nanoribbon Networks for CO2 Reduction},
author = {Pan, Fuping and Li, Boyang and Sarnello, Erik and Fei, Yuhuan and Gang, Yang and Xiang, Xianmei and Du, Zichen and Zhang, Peng and Wang, Guofeng and Nguyen, Hoai T. and Li, Tao and Hu, Yun Hang and Zhou, Hong-Cai and Li, Ying},
abstractNote = {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-N-4 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.},
doi = {10.1021/acsnano.9b09658},
journal = {ACS Nano},
number = 5,
volume = 14,
place = {United States},
year = {2020},
month = {4}
}

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