Efficient Activation of PMS by EDTA-CeCoO3 Composite: Effect of Ce/Co Doping Ratio, Structural Property and Degradation Mechanism

IF 3 4区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES
Junlin Peng, Dihao Bai, Lei Sun, Xiangjuan Yuan
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引用次数: 0

Abstract

The perovskite CeCoO3 composites were synthesized through the sol–gel method with two complexing agents (citric acid and EDTA) with different Ce/Co molar rations and further applied for peroxymonosulfate (PMS) activation. The physicochemical properties and morphology of CeCoO3 were characterized using BET, XRD, FT-IR, SEM, TEM, and XPS techniques. When the CeCoO3 prepared with EDTA as the complexing agent at 600°C and Ce/Co ratio of 1:1, the EDTA-CeCoO3 exhibited superior physicochemical properties, including a high specific surface area (7.69 m2/g) and pore volume, abundant oxygen vacancies, and optimal exposure of active sites, which is most conducive to activating PMS. The effects of catalyst dosage, PMS dosage, initial pH, natural organic matter, and common anions on CeCoO3/PMS system for bisphenol A (BPA) degradation were systematically evaluated. The results revealed that CeCoO3 prepared with EDTA at 600°C Demonstrated excellent catalytic activity for PMS Degradation of BPA, achieving over 97% Degradation efficiency of BPA within 15 min, with a pseudo-first-order reaction rate constant (k) of 0.2909 min⁻1. Furthermore, CeCoO3 showed outstanding stability in multiple cyclic experiments. Furthermore, radical quenching experiments confirmed that SO4•−, OH, and O2•− were the dominant active radicals in the CeCoO3/PMS system for BPA degradation, and a plausible reaction mechanism was proposed. This study provides new insights into the development of PMS activating catalysts, specifically low-cobalt-content yet highly efficient cobalt-based catalysts.

EDTA-CeCoO3复合材料对PMS的高效活化:Ce/Co掺杂比、结构性能和降解机理的影响
以不同Ce/Co摩尔比的两种络合剂(柠檬酸和EDTA)为原料,采用溶胶-凝胶法制备了钙钛矿型CeCoO3复合材料,并将其应用于过氧单硫酸盐(PMS)活化。采用BET、XRD、FT-IR、SEM、TEM和XPS等技术对CeCoO3的理化性质和形貌进行了表征。以EDTA为络合剂,在600℃、Ce/Co比为1:1条件下制备的CeCoO3具有较高的比表面积(7.69 m2/g)和孔容、丰富的氧空位、最佳的活性位点暴露等优越的物理化学性能,最有利于活化PMS。系统评价了催化剂用量、PMS用量、初始pH、天然有机物和常见阴离子对CeCoO3/PMS体系降解双酚A (BPA)的影响。结果表明,EDTA在600℃下制备的CeCoO3对PMS降解BPA具有良好的催化活性,在15 min内达到97%以上的降解效率,准一级反应速率常数(k)为0.2909 min⁻1。此外,CeCoO3在多次循环实验中表现出优异的稳定性。此外,自由基猝灭实验证实了SO4•−、•OH和O2•−是CeCoO3/PMS体系降解BPA的主要活性自由基,并提出了一种合理的反应机理。本研究为PMS活化催化剂,特别是低钴含量高效钴基催化剂的开发提供了新的思路。
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来源期刊
Water, Air, & Soil Pollution
Water, Air, & Soil Pollution 环境科学-环境科学
CiteScore
4.50
自引率
6.90%
发文量
448
审稿时长
2.6 months
期刊介绍: Water, Air, & Soil Pollution is an international, interdisciplinary journal on all aspects of pollution and solutions to pollution in the biosphere. This includes chemical, physical and biological processes affecting flora, fauna, water, air and soil in relation to environmental pollution. Because of its scope, the subject areas are diverse and include all aspects of pollution sources, transport, deposition, accumulation, acid precipitation, atmospheric pollution, metals, aquatic pollution including marine pollution and ground water, waste water, pesticides, soil pollution, sewage, sediment pollution, forestry pollution, effects of pollutants on humans, vegetation, fish, aquatic species, micro-organisms, and animals, environmental and molecular toxicology applied to pollution research, biosensors, global and climate change, ecological implications of pollution and pollution models. Water, Air, & Soil Pollution also publishes manuscripts on novel methods used in the study of environmental pollutants, environmental toxicology, environmental biology, novel environmental engineering related to pollution, biodiversity as influenced by pollution, novel environmental biotechnology as applied to pollution (e.g. bioremediation), environmental modelling and biorestoration of polluted environments. Articles should not be submitted that are of local interest only and do not advance international knowledge in environmental pollution and solutions to pollution. Articles that simply replicate known knowledge or techniques while researching a local pollution problem will normally be rejected without review. Submitted articles must have up-to-date references, employ the correct experimental replication and statistical analysis, where needed and contain a significant contribution to new knowledge. The publishing and editorial team sincerely appreciate your cooperation. Water, Air, & Soil Pollution publishes research papers; review articles; mini-reviews; and book reviews.
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