Synergistic enhancement of Cobalt-Based catalysts for Peroxymonosulfate Activation: Polyoxometalate-Modified MOF-derived C/Co for efficient Acetaminophen degradation

IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Xiuding Shi , Zhengyi Lu , Qian Zhang , Jiefeng Xiao , Han Feng , Junming Hong , Hongyi Yang
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引用次数: 0

Abstract

As an emerging aquatic pollutant, acetaminophen (APAP) poses ecological risks that drive the development of efficient treatment technologies. This study addresses the challenges of active site dispersion and redox cycling efficiency in cobalt-based peroxymonosulfate (PMS) activation systems by innovatively employing a phosphomolybdic acid (PMA) coordination modification strategy to construct a Co-N@PMA multi-metal catalyst. Experimental results show that the catalyst enhances APAP degradation efficiency by 28.45 times compared to the original ZIF-67de system and exhibits exceptional environmental adaptability in complex water parameters (pH 3–9, coexisting anions, and humic acid). Electron paramagnetic resonance (EPR) and quenching experiments characterization confirm that the system primarily follows a non-radical degradation pathway. Experiments and theoretical calculations reveal that the PMA-induced Co-N-Mo ternary synergistic structure optimizes the electron transfer network, facilitating the Co2+/Co3+ redox cycle and thereby enhancing catalytic activity. This study lays a theoretical foundation for the design of multi-metal synergistic catalytic systems and their practical applications in water treatment.

Abstract Image

Abstract Image

钴基催化剂对过氧单硫酸盐活化的协同增强:多金属氧酸修饰mof衍生的C/Co用于对乙酰氨基酚的高效降解
对乙酰氨基酚(APAP)作为一种新兴的水生污染物,其生态风险推动着高效处理技术的发展。本研究通过创新地采用磷酸钼酸(PMA)配位改性策略构建Co-N@PMA多金属催化剂,解决了钴基过氧单硫酸盐(PMS)活化体系中活性位点分散和氧化还原循环效率的挑战。实验结果表明,该催化剂对APAP的降解效率比原来的ZIF-67de体系提高了28.45倍,并且在复杂的水参数(pH 3-9、阴离子共存、腐植酸)中表现出优异的环境适应性。电子顺磁共振(EPR)和淬火实验表征证实了该体系主要遵循非自由基降解途径。实验和理论计算表明,pma诱导的Co-N-Mo三元协同结构优化了电子传递网络,促进了Co2+/Co3+的氧化还原循环,从而提高了催化活性。本研究为多金属协同催化体系的设计及其在水处理中的实际应用奠定了理论基础。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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