Electronic structure modulation of iron sites with fluorine coordination enables ultra-effective H2O2 activation

Deyou Yu, Licong Xu, Kaixing Fu, Xia Liu, Shanli Wang, Minghua Wu, Wangyang Lu, Chunyu Lv and Jinming Luo ()
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Deyou Yu: Zhejiang Sci-Tech University
Licong Xu: Zhejiang Sci-Tech University
Kaixing Fu: Shanghai Jiao Tong University
Xia Liu: Qingdao University
Shanli Wang: Zhejiang Sci-Tech University
Minghua Wu: Zhejiang Sci-Tech University
Wangyang Lu: Zhejiang Sci-Tech University
Chunyu Lv: Shanghai Jiao Tong University
Jinming Luo: Shanghai Jiao Tong University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Electronic structure modulation of active sites is critical important in Fenton catalysis as it offers a promising strategy for boosting H2O2 activation. However, efficient generation of hydroxyl radicals (•OH) is often limited to the unoptimized coordination environment of active sites. Herein, we report the rational design and synthesis of iron oxyfluoride (FeOF), whose iron sites strongly coordinate with the most electronegative fluorine atoms in a characteristic moiety of F-(Fe(III)O3)-F, for effective H2O2 activation with potent •OH generation. Results demonstrate that the fluorine coordination plays a pivotal role in lowering the local electron density and optimizing the electronic structures of iron sites, thus facilitating the rate-limiting H2O2 adsorption and subsequent peroxyl bond cleavage reactions. Consequently, FeOF exhibits a significant and pH-adaptive •OH yield (~450 µM) with high selectivity, which is 1 ~ 3 orders of magnitude higher than the state-of-the-art iron-based catalysts, leading to excellent degradation activities against various organic pollutants at neutral condition. This work provides fundamental insights into the function of fluorine coordination in boosting Fenton catalysis at atomic level, which may inspire the design of efficient active sites for sustainable environmental remediation.

Date: 2024
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DOI: 10.1038/s41467-024-46653-6

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