Atomically Dispersed Iron–Nitrogen Sites on Hierarchically Mesoporous Carbon Nanotube and Graphene Nanoribbon Networks for CO2 Reduction
| Autor: | Boyang Li, Erik Sarnello, Hong-Cai Zhou, Zichen Du, Peng Zhang, Ying Li, Xianmei Xiang, Yun Hang Hu, Fuping Pan, Yang Gang, Guofeng Wang, Hoai T. Nguyen, Yuhuan Fei, Tao Li |
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| Rok vydání: | 2020 |
| Předmět: |
Nanotube
Materials science Graphene General Engineering General Physics and Astronomy chemistry.chemical_element 02 engineering and technology Carbon nanotube Overpotential 010402 general chemistry 021001 nanoscience & nanotechnology Electrocatalyst 01 natural sciences 0104 chemical sciences law.invention chemistry Chemical engineering law General Materials Science 0210 nano-technology Mesoporous material Carbon Faraday efficiency |
| Zdroj: | ACS Nano. 14:5506-5516 |
| ISSN: | 1936-086X 1936-0851 |
| DOI: | 10.1021/acsnano.9b09658 |
| Popis: | 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. |
| Databáze: | OpenAIRE |
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