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Mechanistic insight into the active centers of single/dual-atom Ni/Fe-based oxygen electrocatalysts
DOI:
10.1038/s41467-021-25811-0
Authors:
Wenchao
Wan
(University of Zurich)
,
Yonggui
Zhao
(University of Zurich)
,
Shiqian
Wei
(Leshan Normal University)
,
Carlos A.
Triana
(University of Zurich)
,
Jingguo
Li
(University of Zurich)
,
Andrea
Arcifa
(Empa, Swiss Federal Institute for Materials Science and Technology)
,
Christopher
Allen
(Diamond Light Source; University of Oxford)
,
Rui
Cao
(Stanford Synchrotron Radiation Lightsource)
,
Greta R.
Patzke
(University of Zurich)
Co-authored by industrial partner:
No
Type:
Journal Paper
Journal:
Nature Communications
, VOL 12
State:
Published (Approved)
Published:
September 2021
Diamond Proposal Number(s):
16967

Abstract: Single-atom catalysts with maximum metal utilization efficiency show great potential for sustainable catalytic applications and fundamental mechanistic studies. We here provide a convenient molecular tailoring strategy based on graphitic carbon nitride as support for the rational design of single-site and dual-site single-atom catalysts. Catalysts with single Fe sites exhibit impressive oxygen reduction reaction activity with a half-wave potential of 0.89 V vs. RHE. We find that the single Ni sites are favorable to promote the key structural reconstruction into bridging Ni-O-Fe bonds in dual-site NiFe SAC. Meanwhile, the newly formed Ni-O-Fe bonds create spin channels for electron transfer, resulting in a significant improvement of the oxygen evolution reaction activity with an overpotential of 270 mV at 10 mA cm−2. We further reveal that the water oxidation reaction follows a dual-site pathway through the deprotonation of *OH at both Ni and Fe sites, leading to the formation of bridging O2 atop the Ni-O-Fe sites.
Journal Keywords: Catalysis; Catalytic mechanisms; Chemistry
Subject Areas:
Chemistry,
Energy
Diamond Offline Facilities:
Electron Physical Sciences Imaging Centre (ePSIC)
Instruments:
E02-JEM ARM 300CF
Added On:
27/09/2021 14:04
Documents:
s41467-021-25811-0.pdf
Discipline Tags:
Earth Sciences & Environment
Sustainable Energy Systems
Energy
Climate Change
Physical Chemistry
Catalysis
Chemistry
Technical Tags:
Microscopy
Electron Microscopy (EM)
Transmission Electron Microscopy (TEM)