Xiao Huiji, Wang Yun, Lv Kewei, Zhu Chenxi, Guan Xiaohong, Xie Bing, Zou Xiaoming, Luo Xubiao, Zhou Yanbo
School of Life Sciences, Key Laboratory of Jiangxi Province for Functional Biology and Pollution Control in Red Soil Regions, Jinggangshan University, Ji'an 343009, China.
State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, Shanghai 200237, China.
Water Res. 2025 Jun 15;278:123399. doi: 10.1016/j.watres.2025.123399. Epub 2025 Mar 1.
Emerging contaminants (ECs) are characterized by their widespread environmental distribution and low concentrations, posing significant challenges for their effective removal from source wastewater. To better deal with the problems associated with ECs, we developed a robust Fe-Mn bimetallic catalyst supported on N-doped biochar (FM@NBC-8) for peroxymonosulfate (PMS)-mediated advanced oxidation system, in which bisphenol A (BPA) was investigated as a typical EC. Particularly, complete degradation of BPA in the FM@NBC-8/PMS system was achieved within 5 min, accompanying with a high TOC removal. The degradation rate of BPA with FM@NBC-8 was 143 times that of the initial biochar (BC-8), 20 and 91 times that of single metal-doped catalysts Fe (F@NBC-8) and Mn (M@NBC-8), respectively. The degradation rate of BPA was enhanced to 1.7337 min with 0.6 g L FM@NBC-8 utilized to activate PMS, achieving a superior performance in BPA degradation compared to most reported results in the literature (0.081∼1.43 min). The introduction of Fe, Mn, and N elements dramatically enhanced the specific surface area (from 46.285 to 218.541 m g) of the catalyst, thereby enhancing the adsorption capacity of PMS and pollutants on the catalyst. Moreover, the accelerated electron transfer between the catalyst and PMS favored the formation of low-valent metal intermediates (Fe(II)-O-O-SO and Mn(II)-O-O-SO), responsible for the generation of SOand OH. And O was generated mainly via the decomposition of SO in FM@NBC-8/PMS system, thereby collectively enhancing the pollutant degradation. The stability of the catalyst was attributed to the synergistic effects of nitrogen doping and biochar encapsulation, which ensured effective operation of the FM@NBC-8/PMS system across a broad pH range of 3 to 10, while also providing resistance to interference from ubiquitous anions. This study indicates that the bimetal biochar-based materials for catalytic PMS activation have significant potential for practical application in green environmental remediation.
新兴污染物(ECs)的特点是在环境中广泛分布且浓度较低,这给从源废水中有效去除它们带来了重大挑战。为了更好地应对与新兴污染物相关的问题,我们开发了一种负载在氮掺杂生物炭上的稳健的铁 - 锰双金属催化剂(FM@NBC - 8)用于过一硫酸盐(PMS)介导的高级氧化系统,其中双酚A(BPA)被作为一种典型的新兴污染物进行研究。特别地,在FM@NBC - 8/PMS系统中,BPA在5分钟内实现了完全降解,同时总有机碳(TOC)去除率很高。FM@NBC - 8对BPA的降解速率是初始生物炭(BC - 8)的143倍,分别是单金属掺杂催化剂铁(F@NBC - 8)和锰(M@NBC - 8)的20倍和91倍。当使用0.6 g/L的FM@NBC - 8来活化PMS时,BPA的降解速率提高到1.7337 min,与文献中大多数报道的结果(0.081∼1.43 min)相比,在BPA降解方面表现出优异的性能。铁、锰和氮元素的引入显著提高了催化剂的比表面积(从46.285增加到218.541 m²/g),从而增强了PMS和污染物在催化剂上的吸附能力。此外,催化剂与PMS之间加速的电子转移有利于低价金属中间体(Fe(II)-O-O-SO和Mn(II)-O-O-SO)的形成,这些中间体负责生成SO₄⁻和·OH。并且O₂主要通过FM@NBC - 8/PMS系统中SO₄⁻的分解产生,从而共同增强了污染物的降解。催化剂的稳定性归因于氮掺杂和生物炭封装的协同作用,这确保了FM@NBC - 8/PMS系统在3至10的宽pH范围内有效运行,同时还能抵抗常见阴离子的干扰。这项研究表明,基于双金属生物炭的材料用于催化PMS活化在绿色环境修复中具有显著的实际应用潜力。