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Fe3C@C/C for catalytic ozonation of silicon-containing wastewater: Dual improvement of silicon resistance and catalytic effect
Journal of Materials Science & Technology ( IF 10.9 ) Pub Date : 2022-08-11 , DOI: 10.1016/j.jmst.2022.07.015
Shengzhe Wang , Lei Ma , Rui Wang , Chengyu Jin , Ying Zhao , Xuefei Tan , Yanan Zhang , Mengyang Liu , Chenxing Yao , Huangzhao Wei , Chenglin Sun

The improvement of catalysts’ stability under harsh reaction conditions is vital for their practical applicability. Herein, iron carbide (Fe3C) nanoparticles were encapsulated in graphitic carbon in situ and a carbon ball served as the carrier. The synthesized Fe3C@C/C was first utilized to treat an m-cresol wastewater containing Si via catalytic ozonation. Compared with the commercial Fe/Al2O3 catalyst, the resistance to Si of the Fe3C@C/C was improved 22.68 times, while the TOC removal rate increased by a factor of 2.9, and it remained stable during 10 cycles and 12000 min of continuous reaction, which further demonstrated its potential for diverse applications. The catalyst exhibits improved resistance to Si because of the dual protection from the carbon-encapsulated structure and carbon carrier. Density functional theory calculations show that the encapsulation of Fe3C using carbon significantly increases the resistance to adsorption of Si on its active sites. In addition, the activation of O3 is unimpeded on the Fe3C adsorption sites by the protection from C, thus the generation of reactive oxygen species (ROS) by ozone is largely promoted. The mechanism associated with the resistance of the Fe3C@C/C catalyst to Si and its elevated activity are also elucidated.



中文翻译:

Fe3C@C/C催化臭氧化含硅废水:耐硅性和催化效果的双重提升

提高催化剂在苛刻反应条件下的稳定性对其实际应用至关重要。在此,碳化铁(Fe 3 C)纳米颗粒被原位封装在石墨碳中,并且碳球作为载体。合成的 Fe 3 C@C/C 首次用于通过催化臭氧化处理含硅的间甲酚废水。与市售的Fe/Al 2 O 3催化剂相比,Fe 3的耐SiC@C/C 提高了 22.68 倍,TOC 去除率提高了 2.9 倍,并且在 10 个循环和 12000 分钟的连续反应中保持稳定,进一步展示了其在多种应用中的潜力。由于碳包封结构和碳载体的双重保护,该催化剂表现出更高的抗硅性能。密度泛函理论计算表明,使用碳包封 Fe 3 C 显着增加了 Si 在其活性位点上的吸附阻力。此外,O 3的活化对 Fe 3没有阻碍。C 吸附位点受到 C 的保护,从而大大促进了臭氧产生的活性氧 (ROS)。还阐明了与 Fe 3 C@C/C 催化剂对 Si 的抗性及其提高的活性相关的机制。

更新日期:2022-08-11
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