Magneto-voltaic activity of single-atom iron on reduced graphene oxide for magneto-catalytic conversion of H2O2into O2
Journal
Chemical Science
Journal Volume
17
Journal Issue
2
Start Page
1073
End Page
1097
ISSN
20416520
Date Issued
2026-01-14
Author(s)
Chung, Chieh-Wei
Huang, Jyun-Yau
Liang, Jing-Guan
Iffland, Linda
Dayao, Loise Ann
Dhanthala Chittibabu, Dinesh Kumar
Chi, Chong-Chi
Chen, Jeng-Lung
Chan, Ting-Shan
Chen, Chi-Liang
Lu, Ying-Rui
Huang, Chieh-Cheng
Chou, Ho-Hsiu
Chen, Ying-Chieh
Lu, Ming-Yen
Chen, Hsin-Tsung
Apfel, Ulf-Peter
Lai, Yei-Chen
Lu, Tsai-Te
Abstract
Recent advances in magnetically enhanced (electro)catalysis have disclosed the potential of magnetic fields to modulate reaction kinetics and catalytic performance. Herein, a combination of alternating magnetic field (AMF) as a physical stimulus, reduced graphene oxide (rGO) as a magneto-sensitizer, single-atom Fe on rGO (FeSA:rGO) as the catalytic active site, and H2O2 as a dual reductant and oxidant demonstrated a proof-of-concept magneto-catalytic process that is thermodynamically driven solely by magneto-voltaic activity. Upon application of an AMF to electroconductive FeSA:rGO, AMF-induced charge separation led to formation of low-lying electron holes (EHOMO = 2.41/2.43 eV) and excited electrons (ELUMO = −0.65/−0.57 eV), which triggered AMF power-dependent magneto-voltaic and magneto-electric activity (0.19–1.56 V and 0.15–0.62 mA). In the presence of H2O2, these AMF-induced low-lying electron holes in FeSA:rGO promoted oxidation of the Fe3+ resting state leading to transient formation of a high-valent Fe4+ species, which served as a critical intermediate for magneto-catalytic oxidation of H2O2 and evolution of O2. Furthermore, a kinetic study unveiled that FeSA:rGO concentration, H2O2 concentration, and AMF power played key roles in controlling the rates for FeSA:rGO-mediated magneto-catalytic oxygen evolution reaction. Consequently, these investigations established a mechanistic foundation for the future development of magneto-catalytic systems by integrating AMF-responsive magneto-sensitizers with diverse catalytic active sites.
Publisher
Royal Society of Chemistry
Type
journal article