Electrochemical CO2 Reduction with Atomic Iron‐Dispersed on Nitrogen‐Doped Graphene
Abstract
Electrochemical reduction of CO2 provides an opportunity to reach a carbon‐neutral energy recycling regime, in which CO2 emissions from fuel use are collected and converted back to fuels. The reduction of CO2 to CO is the first step toward the synthesis of more complex carbon‐based fuels and chemicals. Therefore, understanding this step is crucial for the development of high‐performance electrocatalyst for CO2 conversion to higher order products such as hydrocarbons. Here, atomic iron dispersed on nitrogen‐doped graphene (Fe/NG) is synthesized as an efficient electrocatalyst for CO2 reduction to CO. Fe/NG has a low reduction overpotential with high Faradic efficiency up to 80%. The existence of nitrogen‐confined atomic Fe moieties on the nitrogen‐doped graphene layer is confirmed by aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy and X‐ray absorption fine structure analysis. The Fe/NG catalysts provide an ideal platform for comparative studies of the effect of the catalytic center on the electrocatalytic performance. The CO2 reduction reaction mechanism on atomic Fe surrounded by four N atoms (Fe–N4) embedded in nitrogen‐doped graphene is further investigated through density functional theory calculations, revealing a possible promotional effect of nitrogen doping on graphene.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Mar 25, 2018
- Source ID
- 10.1002/aenm.201703487
Entities
People
- Almaz S. Jalilov
- Boris I Yakobson
- Chenhao Zhang
- Emilie Ringe
- Huaming Li
- Hui Xu
- James Tour
- Jingjie Wu
- Jun Zhong
- Junwei Sha
- Kaiqi Nie
- Mingjie Liu
- Muqing Ren
- Pulickel Ajayan
- Qin Wu
- Sadegh Yazdi
- Shize Yang
- Zhenyuan Li
Organizations
- Air Force Office of Scientific Research
- American Chemical Society Petroleum Research Fund
- Brookhaven National Laboratory
- Jiangsu University
- Oak Ridge National Laboratory
- Rice University
- Soochow University
- United States Department of Energy