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纳米零价钴/氮掺杂碳对高碘酸盐进行电活化以降解磺胺异恶唑:对快速电子转移机制的见解

Electrical activation of periodate by nano-zero-valent cobalt/nitrogen-doped carbon for sulfisoxazole degradation: Insights into rapid electron transfer mechanisms.

作者信息

Liu Yu, Liu Meng, Li Xiaoping, Wen Lanxuan, Chen Xiaobao, Huang Zonghan, Ding Dahu, Yang Shengjiong, Chen Yang, Chen Rongzhi

机构信息

Yanshan Earth Critical Zone and Surface Fluxes Research Station, College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China.

College of Resources and Environmental Sciences, Nanjing Agricultural University, Nanjing 210095, China.

出版信息

J Colloid Interface Sci. 2025 May;685:854-865. doi: 10.1016/j.jcis.2025.01.188. Epub 2025 Jan 21.

Abstract

Periodate (PI) activation via three-dimensional electrochemical (E) is a promising approach for degrading sulfisoxazole (SIZ), while the scarcity of active sites significantly limits the efficient electron-transfer rate. Herein, we synthesized multiple strongly active zero-valent cobalt (Co) nanoparticles encapsulated in nitrogen-doped carbon (NC) shells through Co-potassium chloride (KCl) doping pyrolysis of Zeolitic Imidazolate Framework-8 (ZIF-8) to induce the rapid electron transfer pathways (ETP). Specifically, molten KCl doping provides confined structures for Co with a diameter of 12.57 nm embedded in the NC shell, thereby expanding the active space of Co/NC. The generated Co/NC exhibited an enormous electrochemically active surface area (ECSA, 736.92 cm/mg), low charge transfer resistance (R, 38.50 Ω), and strong adsorption energy (-6.003 eV), which together promote robust electron transfer kinetics. Capitalizing on these properties, the E-Co/NC-PI system achieved 100% SIZ removal at a degradation rate of 1.587 min under near-neutral (pH 5.00-9.00) conditions, with ultra-low energy consumption (0.011 kWh m, $0.125/L). This study highlights a Co/NC-induced rapid ETP for SIZ removal, offering insights into enhanced electrical activation of PI for wastewater treatment.

摘要

通过三维电化学(E)激活高碘酸盐(PI)是降解磺胺异恶唑(SIZ)的一种有前景的方法,然而活性位点的稀缺显著限制了有效的电子转移速率。在此,我们通过对沸石咪唑酯骨架-8(ZIF-8)进行钴-氯化钾(KCl)掺杂热解,合成了多个包裹在氮掺杂碳(NC)壳中的强活性零价钴(Co)纳米颗粒,以诱导快速电子转移途径(ETP)。具体而言,熔融KCl掺杂为嵌入NC壳中的直径为12.57 nm的Co提供了受限结构,从而扩大了Co/NC的活性空间。所生成的Co/NC表现出巨大的电化学活性表面积(ECSA,736.92 cm/mg)、低电荷转移电阻(R,38.50 Ω)和强吸附能(-6.003 eV),这些共同促进了稳健的电子转移动力学。利用这些特性,E-Co/NC-PI系统在近中性(pH 5.00 - 9.00)条件下以1.587 min的降解速率实现了100%的SIZ去除,能耗超低(0.011 kWh m,0.125美元/升)。本研究突出了Co/NC诱导的用于SIZ去除的快速ETP,为增强PI用于废水处理的电激活提供了见解。

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