Insight into the Role of Defect CN Layer in Enhanced Catalysis of Peroxymonosulfate on Magnetic Cobalt Carbocatalyst for Phenol Degradation

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2025-03-18 DOI:10.1007/s10562-025-04986-x

Haoyi Xu, Wen Huang, Lu Yang, Yifan Ji, Wei Xiong, Derong R. Liu

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Abstract

Phenolic wastewaters possess high toxicity and poor biodegradation and persist in ecosystem for longer periods, causing severe harm to living organisms. Thus, developing highly effective catalysis-oxidation system for phenolic wastewater treatment is highly needed. In this work, a high-performance magnetic cobalt carbocatalyst (M-Co/CN) was prepared via thermal pyrolysis of the amorphous cobalt-aspartic acid complex. It was further applied for activation of peroxymonosulfate (PMS) to degrade phenolic wastewaters. Related characterization results revealed that the compositions, structures, properties of the catalyst mainly depended on pyrolysis temperature. The formed porous CN layer at 600 ℃ could enhance adsorption and catalysis through improving mass transfer, restricting Co aggregation, and exposing more active sites. Therefore, the catalyst we prepared could show high catalytic performance in process of phenol wastewater treatment. Besides, reaction conditions (catalyst dosage, PMS dosage, phenol concentration, pH, and anion type, etc.) were further studied and optimized. Under the optimized conditions, a degradation efficiency of 95.0% was achieved for 100 ppm phenol within 1 h. Furthermore, radical quenching experiments and electron paramagnetic resonance spectroscopy jointly displayed that phenol degradation mechanism in the M-Co/CN-600-PMS system primarily involves the generation of singlet oxygen (¹O₂) with Co⁰ serving as active reaction sites. Besides, recycling experiment also demonstrated that M-Co/CN catalyst had high structure stability and better reusability after tests.

Graphical abstract

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缺陷CN层在过氧单硫酸盐强化催化磁性钴碳催化剂降解苯酚中的作用

酚类废水毒性高，生物降解性差，在生态系统中存留时间长，对生物造成严重危害。因此，迫切需要开发高效的催化氧化系统来处理含酚废水。本文采用热裂解法制备了一种高性能的磁性钴碳催化剂（M-Co/CN）。并进一步应用于活化过氧单硫酸盐（PMS）降解含酚废水。相关表征结果表明，催化剂的组成、结构和性能主要取决于热解温度。600℃下形成的多孔CN层可以通过改善传质、限制Co聚集、暴露更多活性位点等方式增强吸附和催化作用。因此，所制备的催化剂在苯酚废水处理过程中具有较高的催化性能。并对反应条件（催化剂用量、PMS用量、苯酚浓度、pH、阴离子类型等）进行了进一步研究和优化。在优化条件下，对100 ppm苯酚的降解效率在1 h内达到95.0%。此外，自由基猝灭实验和电子顺磁共振波谱分析共同表明，M-Co/CN-600-PMS体系中苯酚的降解机制主要涉及以Co0为活性反应位点的单线态氧（1O2）的生成。此外，回收实验也证明了M-Co/CN催化剂具有较高的结构稳定性和较好的可重复使用性。图形抽象

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.