Adjusting oxidation pathways via fine-tuning atomic ratios in window-opening MOF membranes for efficient self-cleaning

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

Water Research Pub Date : 2024-11-10 DOI:10.1016/j.watres.2024.122783

Hui Zhang, Junjie Yang, Zhiyu Sun, Yinkun Sun, Guanjin Liu, Dongwei Lu, Jun Ma

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引用次数: 0

Abstract

Peroxymonosulfate (PMS) can be used as a green oxidant to mitigate catalytic membranes fouling and restore filtration performance through advanced oxidation processes (AOP). However, the adjustment of oxidation pathways and the understanding of underlying mechanisms for efficient cleaning without sacrificing the filtration performance need to be studied systematically. We optimized the membranes microenvironment via thermal modification from 25 °C to 400 °C below the catalyst ZIF-8 framework's decomposition temperature. The modified membranes have a doubled pure water flux (158.3 LMH bar⁻¹) and remain rejection rates due to intact ZIF-8 framework structure with “window-opening” effect. The methyl dissociation and self-catalyzed graphitization were regulated by changing temperature, resulting in adjustable nonradical pathway proportion (correlated with the C/Zn atomic ratio at 0.96). The enhanced nonradical pathway targeted attacks on electron-rich regions of organic compounds, resulting in efficient cleaning and almost complete flux recovery (99.3 %). The theoretical simulations revealed that methyl groups dissociation and graphitization significantly influence the electron density and adsorption energy at active sites for tunable oxidation pathways and enhanced catalytic performance. Our work offers a rational strategy to improve both filtration and catalytic performance in catalytic membranes. The enhanced understanding of oxidation mechanisms guides the design of designing efficient AOP membrane cleaning systems.

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通过微调开窗 MO0F 膜中的原子比来调整氧化途径，实现高效自清洁

过一硫酸盐（PMS）可用作绿色氧化剂，通过高级氧化过程（AOP）减轻催化膜污垢并恢复过滤性能。然而，如何调整氧化途径并了解其基本机制，以便在不牺牲过滤性能的情况下实现高效清洁，还需要进行系统研究。我们通过热改性优化了膜的微环境，改性温度从 25 °C 至 400 °C 不等，低于催化剂 ZIF-8 框架的分解温度。由于具有 "开窗 "效应的完整 ZIF-8 框架结构，改性后的膜纯水通量翻了一番（158.3 LMH bar-1），排斥率保持不变。甲基解离和自催化石墨化受温度变化的调节，从而产生了可调节的非辐射途径比例（与 0.96 的 C/Zn 原子比相关）。增强的非辐射途径针对有机化合物的富电子区域进行攻击，从而实现了高效清洁和几乎完全的通量回收（99.3%）。理论模拟显示，甲基解离和石墨化会显著影响活性位点的电子密度和吸附能，从而实现可调的氧化途径并提高催化性能。我们的工作为提高催化膜的过滤和催化性能提供了合理的策略。加深对氧化机制的理解有助于设计高效的 AOP 膜清洁系统。

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

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.