Electron transfer mediated activation of periodate by contaminants to generate 1O2 by charge-confined single-atom catalyst
Qianqian Tang,
Bangxiang Wu,
Xiaowen Huang,
Wei Ren,
Lingling Liu,
Lei Tian,
Ying Chen,
Long-Shuai Zhang (),
Qing Sun,
Zhibing Kang,
Tianyi Ma and
Jian-Ping Zou ()
Additional contact information
Qianqian Tang: Nanchang Hangkong University
Bangxiang Wu: Nanchang Hangkong University
Xiaowen Huang: Nanchang Hangkong University
Wei Ren: Nanchang Hangkong University
Lingling Liu: Nanchang Hangkong University
Lei Tian: Nanchang Hangkong University
Ying Chen: Nanchang Hangkong University
Long-Shuai Zhang: Nanchang Hangkong University
Qing Sun: Nanchang Hangkong University
Zhibing Kang: Nanchang Hangkong University
Tianyi Ma: RMIT University
Jian-Ping Zou: Nanchang Hangkong University
Nature Communications, 2024, vol. 15, issue 1, 1-10
Abstract:
Abstract The electron transfer process (ETP) is able to avoid the redox cycling of catalysts by capturing electrons from contaminants directly. However, the ETP usually leads to the formation of oligomers and the reduction of oxidants to anions. Herein, the charge-confined Fe single-atom catalyst (Fe/SCN) with Fe-N3S1 configuration was designed to achieve ETP-mediated contaminant activation of the oxidant by limiting the number of electrons gained by the oxidant to generate 1O2. The Fe/SCN-activate periodate (PI) system shows excellent contaminant degradation performance due to the combination of ETP and 1O2. Experiments and DFT calculations show that the Fe/SCN-PI* complex with strong oxidizing ability triggers the ETP, while the charge-confined effect allows the single-electronic activation of PI to generate 1O2. In the Fe/SCN + PI system, the 100% selectivity dechlorination of ETP and the ring-opening of 1O2 avoid the generation of oligomers and realize the transformation of large-molecule contaminants into small-molecule biodegradable products. Furthermore, the Fe/SCN + PI system shows excellent anti-interference ability and application potential. This work pioneers the generation of active species using ETP’s electron to activate oxidants, which provides a perspective on the design of single-atom catalysts via the charge-confined effect.
Date: 2024
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-53941-8
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DOI: 10.1038/s41467-024-53941-8
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