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Electrochemical CO 2 Reduction with Atomic Iron‐Dispersed on Nitrogen‐Doped Graphene
Author(s) -
Zhang Chenhao,
Yang Shize,
Wu Jingjie,
Liu Mingjie,
Yazdi Sadegh,
Ren Muqing,
Sha Junwei,
Zhong Jun,
Nie Kaiqi,
Jalilov Almaz S.,
Li Zhenyuan,
Li Huaming,
Yakobson Boris I.,
Wu Qin,
Ringe Emilie,
Xu Hui,
Ajayan Pulickel M.,
Tour James M.
Publication year - 2018
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.201703487
Subject(s) - graphene , overpotential , electrocatalyst , materials science , catalysis , electrochemistry , carbon fibers , nitrogen , inorganic chemistry , chemical engineering , doping , density functional theory , electrochemical energy conversion , nanotechnology , electrode , chemistry , composite number , composite material , organic chemistry , computational chemistry , optoelectronics , engineering
Abstract Electrochemical reduction of CO 2 provides an opportunity to reach a carbon‐neutral energy recycling regime, in which CO 2 emissions from fuel use are collected and converted back to fuels. The reduction of CO 2 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 CO 2 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 CO 2 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 CO 2 reduction reaction mechanism on atomic Fe surrounded by four N atoms (Fe–N 4 ) embedded in nitrogen‐doped graphene is further investigated through density functional theory calculations, revealing a possible promotional effect of nitrogen doping on graphene.