Atomically Dispersed Iron Regulating Electronic Structure of Iron Atom Clusters for Electrocatalytic H2O2 Production and Biomass Upgrading
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Zhang, Shengbo
Zhang, Xinyuan
Xu, Min
Han, Miaomiao
Zheng, Li Rong
Zhang, Yunxia
Wang, Guozhong
Zhang, Haimin
Zhao, Huijun
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Abstract
The integration of highly active single atoms (SAs) and atom clusters (ACs) into an electrocatalyst is critically important for high-efficiency two-electron oxygen reduction reaction (2e- ORR) to hydrogen peroxide (H2O2). Here we report a tandem impregnation-pyrolysis-etching strategy to fabricate the oxygen-coordinated Fe SAs and ACs anchored on bacterial cellulose derived carbon (BCC) (FeSAs/ACs-BCC). As the electrocatalyst, FeSAs/ACs-BCC exhibits superior electrocatalytic activity and selectivity toward 2e- ORR, affording an onset potential of 0.78 V (vs. RHE) and a high H2O2 selectivity of 96.5% in 0.1 M KOH. In a flow cell reactor, the FeSAs/ACs-BCC also achieves high-efficiency H2O2 production with a yield rate of 12.51 ± 0.18 mol gcat-1 h-1 and a faradaic efficiency of 89.4% ± 1.3% at 150 mA cm-2. Additionally, the feasibility of coupling the produced H2O2 and electro-Fenton process for the valorization of ethylene glycol was explored in detail. The theoretical calculations uncover that the oxygen-coordinated Fe SAs effectively regulate the electronic structure of Fe ACs which are the 2e- ORR active sites, resulting in the optimal binding strength of *OOH intermediate for high-efficiency H2O2 production.
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Angewandte Chemie International Edition
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This is the peer reviewed version of the following article: Xu, H; Zhang, S; Zhang, X; Xu, M; Han, M; Zheng, LR; Zhang, Y; Wang, G; Zhang, H; Zhao, H, Atomically Dispersed Iron Regulating Electronic Structure of Iron Atom Clusters for Electrocatalytic H2O2 Production and Biomass Upgrading, Angewandte Chemie International Edition, 2023, pp. e202314414, which has been published in final form at https://doi.org/10.1002/anie.202314414. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.
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Chemical sciences
Fe single atoms * Fe atom clusters * two-electron ORR * H2O2 electrosynthesis * electro-Fenton process
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Xu, H; Zhang, S; Zhang, X; Xu, M; Han, M; Zheng, LR; Zhang, Y; Wang, G; Zhang, H; Zhao, H, Atomically Dispersed Iron Regulating Electronic Structure of Iron Atom Clusters for Electrocatalytic H2O2 Production and Biomass Upgrading, Angewandte Chemie International Edition, 2023, pp. e202314414