Facile cascade-anchored synthesis of ultrahigh metal loading single-atom for significantly improved Fenton-like catalysis.

IF 15.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Nature Communications Pub Date : 2025-10-02 DOI:10.1038/s41467-025-63858-5

Shuaishuai Li,Wei Wang,Huizhong Wu,Xuechun Wang,Shihu Ding,Jingyang Liu,Xiuwu Zhang,Jiangli Sun,Chunhong Fu,Minghua Zhou

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Abstract

It is crucial to break the low metal-loading limitation and reveal the intersite synergy-governed catalytic behavior of single-atom catalysts (SACs). Here, a universal synthesis strategy achieves record loadings of transition metals (Fe 41.31 wt%, Mn 35.13 wt%), rare-earth metals (La 28.62 wt%), and noble metals (Ag 27.04 wt%). The strong oxalic acid-metal chelation and concurrent entangled polymer networks enable high-loading SACs. High-density single atoms induce site-intensive effects, modulating electron density and valence states to achieve peroxymonosulfate-based Fenton-like reactions with rate constants 1-2 orders of magnitude higher than conventional SACs. Elevated metal loading boosts Fenton-like potential jumps, facilitates electron transfer, and reduces the rate-limiting energy barrier in 1O2 production. This material is also proven effective in real wastewater treatment, combining high decontamination efficiency with operational stability. It is anticipated that the cascade-anchoring synthesis strategy will take SACs a step closer to practical applications.

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易级联锚定合成超高金属负载单原子，显著改善了类芬顿催化。

突破低金属负载的限制，揭示单原子催化剂（SACs）的场间协同催化行为是至关重要的。在这里，通用合成策略实现了过渡金属（Fe 41.31 wt%, Mn 35.13 wt%），稀土金属（La 28.62 wt%）和贵金属（Ag 27.04 wt%）的创纪录负载。强草酸-金属螯合和并发纠缠的聚合物网络使高负载SACs成为可能。高密度的单原子诱导位点密集效应，调节电子密度和价态，实现速率常数比传统sac高1-2个数量级的过氧单硫酸盐类芬顿反应。升高的金属负载促进了芬顿样电位跳跃，促进了电子转移，并降低了1O2生产中的限速能量势垒。该材料在实际废水处理中也被证明是有效的，结合了高去污效率和运行稳定性。预计级联锚定综合策略将使sac更接近实际应用。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nature Communications Biological Science Disciplines-

CiteScore

24.90

自引率

2.40%

发文量

6928

审稿时长

3.7 months

期刊介绍： Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.