Nonradical-dominated nanoconfined iron single-atom catalytic membrane to enhance peroxymonosulfate activation for efficient water decontamination

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research Pub Date : 2025-06-24 DOI:10.1016/j.watres.2025.124106

Peijie Li , Daliang Xu , Xiaoxiang Cheng , Peng Liu , Xinsheng Luo , Jiaxuan Yang , Heng Liang

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Abstract

Catalytic membrane reactors (CMRs) exhibit significant advantages in the removal of contaminants of emerging concern. However, the impairment inflicted on polymer membranes by radicals and the radical scavenging induced by natural organic matter constrain the advancement of CMRs. Herein, we designed an iron single-atom catalyst (FePc-O-CNT) dominated by nonradical oxidation mechanisms and combined it with peroxymonosulfate (PMS) to develop a CMR system (FePc-O-CNT membrane/PMS). The system exhibited superior degradation activity to multiple pollutants via nonradical pathways. The nanoconfined membrane space facilitated PMS activation and enhanced singlet oxygen generation and mass transfer, resulting in a 9513-fold enhancement for bisphenol A (BPA) degradation kinetics over the heterogeneous suspensions. Moreover, the system performed robustly in complex water matrices even under severe membrane fouling (60 % or 80 % flux declines). Unlike radical-based processes, the FePc-O-CNT membrane/PMS system maintained excellent permeability, with only a 7.4 % flux loss after 84 h filtration. For engineering validation, the FePc-O-CNT membrane was also fabricated through non-solvent induced phase separation, which achieved ∼100 % BPA removal and minimal iron leaching over 48 h operation. This research introduces a nonradical-dominated CMR system that addresses the limitations of radical-dominated catalytic degradation, providing foundational insights for advanced membrane-based water purification processes.

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非自由基主导的纳米约束铁单原子催化膜增强过氧单硫酸盐活化高效水净化

催化膜反应器（CMRs）在去除新出现的污染物方面表现出显著的优势。然而，自由基对聚合物膜的损伤和天然有机物对自由基的清除作用制约了cmr的发展。本文设计了一种以非自由基氧化机制为主的铁单原子催化剂（FePc-O-CNT），并将其与过氧单硫酸盐（PMS）结合，形成了一种CMR体系（FePc-O-CNT膜/PMS）。该系统通过非自由基途径对多种污染物表现出优异的降解活性。纳米膜空间促进了PMS的活化，增强了单线态氧生成和传质，导致双酚a （BPA）的降解动力学比非均相悬浮液提高了9513倍。此外，即使在严重的膜污染（60%或80%的通量下降）下，该系统在复杂的水基质中也表现良好。与基于自由基的工艺不同，FePc-O-CNT膜/PMS系统保持了良好的渗透性，过滤84小时后通量损失仅为7.4%。为了进行工程验证，还通过非溶剂诱导相分离制备了FePc-O-CNT膜，该膜在48小时的操作中实现了~ 100%的BPA去除和最小的铁浸出。本研究介绍了一种非自由基主导的CMR系统，该系统解决了自由基主导的催化降解的局限性，为先进的膜基水净化工艺提供了基础见解。

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来源期刊

Water Research 环境科学-工程：环境

CiteScore

20.80

自引率

9.40%

发文量

1307

审稿时长

38 days

期刊介绍： Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.