Accelerated Catalytic Ozonation in a Mesoporous Carbon-Supported Atomic Fe-N4 Sites Nanoreactor: Confinement Effect and Resistance to Poisoning

Wei Qu; Manhui Luo; Zhuoyun Tang

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Accelerated Catalytic Ozonation in a Mesoporous Carbon-Supported Atomic Fe-N4 Sites Nanoreactor: Confinement Effect and Resistance to Poisoning

机译：Accelerated Catalytic Ozonation in a Mesoporous Carbon-Supported Atomic Fe-N4 Sites Nanoreactor: Confinement Effect and Resistance to Poisoning

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The design of a micro-/nanoreactor is of great significance for catalytic ozonation, which can achieve effective mass transfer and expose powerful reaction species. Herein, the mesoporous carbon with atomic Fe-N4 sites embedded in the ordered carbon nanochannels (Fe-N4/CMK-3) was synthesized by the hard-template method. Fe-N4/CMK-3 can be employed as nanoreactors with preferred electronic and geometric catalytic microenvironments for the internal catalytic ozonation of CH3SH. During the CH3SH oxidation process, the mass transfer coefficient of the Fe-N4/CMK-3 confined system with sufficient O3 transfer featured a level of at least 1.87 X 1O-5, which is 34.6 times that of the Fe-N4/C—Si unconfined system. Detailed experimental studies and theoretical calculations demonstrated that the anchored atomic Fe-N4 sites and nanoconfinement effects regulated the local electronic structure of the catalyst and promoted the activation of O3 molecules to produce atomic oxygen species (AOS) and reactive oxygen species (ROS), eventually achieving efficient oxidation of CH3SH into C02/S042_. Benefiting from the high diffusion rate and the augmentation of AOS/ROS, Fe-N4/ CMK-3 exhibited an excellent poisoning tolerance, along with high catalytic durability. This contribution provides the proof-of- concept strategy for accelerating catalytic ozonation of sulfur-containing volatile organic compounds (VOCs) by combining confined catalysis and atomic catalysts and can be extended to the purification of other gaseous pollutants.

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《Environmental Science & Technology: ES&T》 |2023年第35期|13205-13216|共12页
作者
Wei Qu; Manhui Luo; Zhuoyun Tang;
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作者单位

School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275, China;

School of Environmental Science and Engineering Sun Yat-Sen University, Guangzhou 510275, China;

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收录信息美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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正文语种英语
中图分类环境科学、安全科学;
关键词
catalytic ozonation; nanoconfinement effect; poisoning resistance; single-atom catalysis; sulfur-containing VOCs;

Accelerated Catalytic Ozonation in a Mesoporous Carbon-Supported Atomic Fe-N4 Sites Nanoreactor: Confinement Effect and Resistance to Poisoning

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