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用于稳定合成碱土金属过氧化物的自清洁电极。

Self-cleaning electrode for stable synthesis of alkaline-earth metal peroxides.

作者信息

Wang Minli, Cheng Jinhuan, Xu Wenwen, Zhu Dandan, Zhang Wuyong, Wen Yingjie, Guan Wanbing, Jia Jinping, Lu Zhiyi

机构信息

Key Laboratory of Marine Materials and Related Technologies, Zhejiang Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, China.

School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, China.

出版信息

Nat Nanotechnol. 2025 Jan;20(1):67-74. doi: 10.1038/s41565-024-01815-x. Epub 2024 Oct 28.

DOI:10.1038/s41565-024-01815-x
PMID:39468360
Abstract

Alkaline-earth metal peroxides (MO, M = Ca, Sr, Ba) represent a category of versatile and clean solid oxidizers, while the synthesis process usually consumes excessive hydrogen peroxide (HO). Here we discover that HO synthesized via two-electron electrochemical oxygen reduction (2e ORR) on the electrode surface can be efficiently and durably consumed to produce high-purity MO in an alkaline environment. The crucial factor lies in the in-time detachment of in situ-generated MO from the self-cleaning electrode, where the solid products spontaneously detach from the electrode to solve the block issue. The self-cleaning electrode is achieved by constructing micro-/nanostructure of a highly active catalyst with appropriate surface modification. In experiments, an unprecedented accumulated selectivity (~99%) and durability (>1,000 h, 50 mA cm) are achieved for electrochemical synthesis of MO. Moreover, the comparability of CaO and HO for tetracycline degradation with hydrodynamic cavitation is validated in terms of their close efficacies (degradation efficiency of 87.9% and 93.6% for HO and CaO, respectively).

摘要

碱土金属过氧化物(MO,M = Ca、Sr、Ba)是一类用途广泛且清洁的固体氧化剂,但其合成过程通常会消耗过量的过氧化氢(HO)。在此,我们发现通过电极表面的两电子电化学氧还原(2e ORR)合成的HO在碱性环境中能够被高效且持久地消耗,从而生成高纯度的MO。关键因素在于原位生成的MO能及时从自清洁电极上脱离,在该电极上固体产物会自发地从电极上脱离,从而解决了堵塞问题。自清洁电极是通过构建具有适当表面修饰的高活性催化剂的微/纳米结构来实现的。在实验中,MO的电化学合成实现了前所未有的累积选择性(约99%)和耐久性(>1000小时,50 mA cm)。此外,通过水力空化作用,验证了CaO和HO在四环素降解方面的可比性,因为它们的降解效果相近(HO和CaO的降解效率分别为87.9%和93.6%)。

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