富缺陷二氧化锰活化过氧乙酸降解磺胺乙胺的机理研究

IF 7.4 Q1 ENGINEERING, ENVIRONMENTAL
Jie Dong, Long Li, Chang Zhang, Daofen Huang, Xing Li, Mengxi Zhao, Guangfu Wang, Irene M. C. Lo, Xiaohong Guan and Haoran Dong*, 
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引用次数: 0

摘要

锰(Mn)基氧化物,主要是二氧化锰,由于其优异的氧化还原性能和结构灵活性,在催化应用中引起了极大的关注。然而,它们饱和的协调结构给实现性能增强带来了挑战。本文构建了一种缺陷MnO2催化剂(MnO2- d),并首次证明了该催化剂能有效激活过氧乙酸(PAA)完全降解磺胺乙嘧啶(SMT)。与具有饱和配位结构的MnO2(即完美MnO2- p结构)相比,MnO2- d催化剂表现出更高的表面电子密度和丰富的表面氧空位(OVs),显著提高了其催化活性。实验结果表明,MnO2-D表面的OVs和Mn3+被认为是主要的活性位点,MnO2-D/PAA体系遵循单线态氧(1O2)主导的非自由基途径。MnO2-D催化剂可以在无机阴离子、腐植酸、不同pH值和真实水环境的干扰下保持活性。此外,MnO2-D/PAA体系在减轻SMT毒性和消除多种微污染物方面效果显著。本工作提出了构建富缺陷金属氧化物催化剂的改进策略,以推进未来的水处理技术。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Mechanistic Insights into Sulfamethazine Degradation by Defect-Rich MnO2-Activated Peracetic Acid

Mechanistic Insights into Sulfamethazine Degradation by Defect-Rich MnO2-Activated Peracetic Acid

Manganese (Mn)-based oxides, mainly MnO2, have garnered significant attention in catalytic applications due to their superior redox properties and structural flexibility. However, their saturated coordination structure presents challenges in achieving an enhanced performance. Herein, a defective MnO2 catalyst (MnO2-D) was constructed, and for the first time, it was proven to effectively activate peracetic acid (PAA) for the complete degradation of sulfamethazine (SMT). Compared to MnO2 with a saturated coordination structure (i.e., the perfect MnO2 structure, MnO2-P), the MnO2-D catalyst exhibited a higher surface electron density and abundant surface oxygen vacancies (OVs), significantly improving its catalytic activity. Experimental evidence revealed that the OVs and Mn3+ on the surface of MnO2-D were considered as the primary active sites and that the MnO2-D/PAA system followed a singlet oxygen (1O2)-dominated nonradical pathway. The MnO2-D catalyst can maintain its activity with minimal interference from inorganic anions, humic acid, varying pH levels, and real water environments. In addition, the MnO2-D/PAA system was efficient in mitigating the toxicity of SMT and eliminating diverse micropollutants. This work presents an enhancement strategy for constructing defect-rich metal oxide catalysts to advance future water treatment technologies.

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来源期刊
ACS ES&T engineering
ACS ES&T engineering ENGINEERING, ENVIRONMENTAL-
CiteScore
8.50
自引率
0.00%
发文量
0
期刊介绍: ACS ES&T Engineering publishes impactful research and review articles across all realms of environmental technology and engineering, employing a rigorous peer-review process. As a specialized journal, it aims to provide an international platform for research and innovation, inviting contributions on materials technologies, processes, data analytics, and engineering systems that can effectively manage, protect, and remediate air, water, and soil quality, as well as treat wastes and recover resources. The journal encourages research that supports informed decision-making within complex engineered systems and is grounded in mechanistic science and analytics, describing intricate environmental engineering systems. It considers papers presenting novel advancements, spanning from laboratory discovery to field-based application. However, case or demonstration studies lacking significant scientific advancements and technological innovations are not within its scope. Contributions containing experimental and/or theoretical methods, rooted in engineering principles and integrated with knowledge from other disciplines, are welcomed.
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