High-Efficiency Electrosynthesis of Hydrogen Peroxide from Oxygen Reduction Enabled by a Tungsten Single Atom Catalyst with Unique Terdentate N1O2 Coordination
Author(s)
Zhang, Feifei
Zhu, Yinlong
Tang, Cheng
Chen, Yu
Qian, Binbin
Hu, Zhiwei
Chang, Yu-Chung
Pao, Chih-Wen
Lin, Qian
Kazemi, Seyedeh Alieh
Wang, Yun
Zhang, Lian
Zhang, Xiwang
Wang, Huanting
Griffith University Author(s)
Year published
2021
Metadata
Show full item recordAbstract
Single-atom catalysts (SACs) have shown great potential in the electrochemical oxygen reduction reaction (ORR) toward hydrogen peroxide (H2O2) production. However, current studies are mainly focused on 3d transition-metal SACs, and very little attention has been paid to 5d SACs. Here, a new kind of W SAC anchored on a porous O, N-doped carbon nanosheet (W1/NO-C) is designed and prepared via a simple coordination polymer-pyrolysis method. A unique local structure of W SAC, terdentate W1N1O2 with the coordination of two O atoms and one N atom, is identified by the combination of aberration-corrected scanning transmission ...
View more >Single-atom catalysts (SACs) have shown great potential in the electrochemical oxygen reduction reaction (ORR) toward hydrogen peroxide (H2O2) production. However, current studies are mainly focused on 3d transition-metal SACs, and very little attention has been paid to 5d SACs. Here, a new kind of W SAC anchored on a porous O, N-doped carbon nanosheet (W1/NO-C) is designed and prepared via a simple coordination polymer-pyrolysis method. A unique local structure of W SAC, terdentate W1N1O2 with the coordination of two O atoms and one N atom, is identified by the combination of aberration-corrected scanning transmission electron microscopy, X-ray photoelectron spectroscopy and X-ray absorption fine structure spectroscopy. Remarkably, the as-prepared W1/NO-C catalyzes the ORR via a 2e– pathway with high onset potential, high H2O2 selectivity in the wide potential range, and excellent operation durability in 0.1 m KOH solution, superior to most of state-of-the-art H2O2 electrocatalysts ever reported. Theoretical calculations reveal that the C atoms adjacent to O in the W1N1O2-C moiety are the most active sites for the 2e– ORR to H2O2 with the optimal binding energy of the HOO* intermediate. This work opens up a new opportunity for the development of high-performance W-based catalysts for electrochemical H2O2 production.
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View more >Single-atom catalysts (SACs) have shown great potential in the electrochemical oxygen reduction reaction (ORR) toward hydrogen peroxide (H2O2) production. However, current studies are mainly focused on 3d transition-metal SACs, and very little attention has been paid to 5d SACs. Here, a new kind of W SAC anchored on a porous O, N-doped carbon nanosheet (W1/NO-C) is designed and prepared via a simple coordination polymer-pyrolysis method. A unique local structure of W SAC, terdentate W1N1O2 with the coordination of two O atoms and one N atom, is identified by the combination of aberration-corrected scanning transmission electron microscopy, X-ray photoelectron spectroscopy and X-ray absorption fine structure spectroscopy. Remarkably, the as-prepared W1/NO-C catalyzes the ORR via a 2e– pathway with high onset potential, high H2O2 selectivity in the wide potential range, and excellent operation durability in 0.1 m KOH solution, superior to most of state-of-the-art H2O2 electrocatalysts ever reported. Theoretical calculations reveal that the C atoms adjacent to O in the W1N1O2-C moiety are the most active sites for the 2e– ORR to H2O2 with the optimal binding energy of the HOO* intermediate. This work opens up a new opportunity for the development of high-performance W-based catalysts for electrochemical H2O2 production.
View less >
Journal Title
Advanced Functional Materials
Note
This publication has been entered as an advanced online version in Griffith Research Online.
Subject
Physical sciences
Chemical sciences
Engineering
Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
Chemistry, Physical