竹硫酸盐木质素单原子催化过氧单硫酸盐活化高效降解双酚A

IF 12.1 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Small Pub Date : 2025-01-19 DOI:10.1002/smll.202409803
Jianfeng Ma, Shumin Zhang, Xin Shi, Linxin Dai, Zhenzhen Liu, Xinge Liu, Xihong Lu, Zehui Jiang
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引用次数: 0

摘要

以竹硫酸盐木质素为碳源,采用均相乙醇溶解体系合成了氮配位铁单原子催化剂(SA Fe‐N/C)。通过X射线吸收光谱分析和HAADF - STEM图像,发现SA Fe - N/C结构中均匀分布着原子间距离小于2 Å的铁原子,其铁负载量高达2.69%。在5 min内双酚A (BPA)的降解率接近99%,观察到的速率常数(kobs)从0.070 min−1显著提高到0.615 min−1。催化剂介导的电子转移途径被认为是BPA降解的主要机制。氮配体的实验数据和DFT分析表明,吡啶N配位的铁单原子是主要的活性位点,这是由于电子密度的增强和铁位周围的离域集中。这些发现极大地阐明了氮配体在设计高效木质素衍生碳单原子环境催化剂中的作用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Highly Efficient Degradation of Bisphenol A by Peroxymonosulfate Activation Using Bamboo Kraft Lignin Single-Atom Catalyst

Highly Efficient Degradation of Bisphenol A by Peroxymonosulfate Activation Using Bamboo Kraft Lignin Single-Atom Catalyst

A nitrogen-coordinated Fe single-atom catalyst (SA Fe-N/C) is synthesized using a homogeneous ethanol-based dissolution system with bamboo kraft lignin serving as the carbon source. Uniformly dispersed Fe atoms with an interatomic distance of less than 2 Å throughout the SA Fe-N/C structure are revealed through X-ray absorption spectral analysis and HAADF-STEM images, which possessed a high Fe loading of 2.69%. The degradation rate of bisphenol A (BPA) approached 99% within 5 min, with the observed rate constant (kobs) of the catalysts markedly increasing from 0.070 to 0.615 min−1. The catalyst-mediated electron transfer pathway is identified as the predominant mechanism for BPA degradation. Both experimental data and DFT analysis of the nitrogen ligands demonstrated that pyridinic N-coordinated Fe single atoms are the principal active sites, attributed to the enhanced electron density and delocalization concentrated around the Fe sites. These findings significantly elucidate the role of nitrogen ligands in designing efficient lignin-derived carbon single-atom catalysts for environmental applications.

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来源期刊
Small
Small 工程技术-材料科学:综合
CiteScore
17.70
自引率
3.80%
发文量
1830
审稿时长
2.1 months
期刊介绍: Small serves as an exceptional platform for both experimental and theoretical studies in fundamental and applied interdisciplinary research at the nano- and microscale. The journal offers a compelling mix of peer-reviewed Research Articles, Reviews, Perspectives, and Comments. With a remarkable 2022 Journal Impact Factor of 13.3 (Journal Citation Reports from Clarivate Analytics, 2023), Small remains among the top multidisciplinary journals, covering a wide range of topics at the interface of materials science, chemistry, physics, engineering, medicine, and biology. Small's readership includes biochemists, biologists, biomedical scientists, chemists, engineers, information technologists, materials scientists, physicists, and theoreticians alike.
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