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Electric field-enhanced heterogeneous catalytic ozonation (EHCO) process for sulfadiazine removal: The role of cathodic reduction
Chemosphere ( IF 8.1 ) Pub Date : 2024-01-14 , DOI: 10.1016/j.chemosphere.2024.141226
Xu Yin 1 , Jie Zhang 1 , Siru Chen 1 , Wei Li 1 , Hongwei Zhu 1 , Kajia Wei 1 , Yonghao Zhang 2 , Haoming Chen 1 , Weiqing Han 1
Chemosphere ( IF 8.1 ) Pub Date : 2024-01-14 , DOI: 10.1016/j.chemosphere.2024.141226
Xu Yin 1 , Jie Zhang 1 , Siru Chen 1 , Wei Li 1 , Hongwei Zhu 1 , Kajia Wei 1 , Yonghao Zhang 2 , Haoming Chen 1 , Weiqing Han 1
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In this work, an electric field-enhanced heterogeneous catalytic ozonation (EHCO) was systematically investigated using a prepared FeOx/PAC catalyst. The EHCO process exhibited high sulfadiazine (SDZ) and TOC removal efficiency compared with electrocatalysis (EC) and heterogeneous catalytic ozonation (HCO) process. Almost 100% of SDZ was removed within 2 min, and the TOC removal reached approximately 85% within 60 min. Quenching experiments and EPR analysis suggested that the prominent SDZ and TOC removal performance is supported by the enhanced ·OH generation ability. Further study proved that HO formed by O electrochemical reduction, peroxone reaction and electrochemical reduction of ozone contributed to improving ·OH generation. Furthermore, the EHCO system showed satisfactory stability and recyclability compared to conventional HCO systems, and the SDZ and TOC removal rates were maintained at ≥95% and ≥70% in 16 consecutive recycles, respectively. Meanwhile, XPS analysis and Boehm's titration for the FeOx/PAC catalyst used in HCO and EHCO process confirmed that the external electron supply could restrain the oxidation of surface functional groups of PAC and maintain a balance of the Fe(II)/Fe(III) ratio, which proved the critical role of cathode reduction in catalyst in situ regeneration during long consecutive recycles. In addition, the EHCO system could achieve more than 80% SDZ removal within 2 min in different water matrices. These results confirmed that the EHCO process has a wide application perspective for refractory organics removal in actual wastewater.
中文翻译：
去除磺胺嘧啶的电场增强非均相催化臭氧化 (EHCO) 工艺：阴极还原的作用
在这项工作中，使用制备的 FeOx/PAC 催化剂系统地研究了电场增强非均相催化臭氧化 (EHCO)。与电催化（EC）和非均相催化臭氧化（HCO）工艺相比，EHCO工艺表现出较高的磺胺嘧啶（SDZ）和TOC去除效率。 2分钟内SDZ几乎100%被去除，60分钟内TOC去除率达到约85%。淬火实验和 EPR 分析表明，突出的 SDZ 和 TOC 去除性能是由增强的·OH 生成能力支持的。进一步的研究证明，O电化学还原、过氧酮反应和臭氧电化学还原形成的H2O有助于提高·OH的生成。此外，与传统的HCO系统相比，EHCO系统表现出令人满意的稳定性和可回收性，并且在连续16次回收中SDZ和TOC去除率分别保持在≥95%和≥70%。同时，对HCO和EHCO过程中使用的FeOx/PAC催化剂的XPS分析和Boehm滴定证实，外部电子供应可以抑制PAC表面官能团的氧化并维持Fe(II)/Fe(III)的平衡比，这证明了阴极还原在长时间连续循环过程中催化剂原位再生中的关键作用。此外，EHCO系统在不同的水基质中可以在2分钟内实现超过80%的SDZ去除率。这些结果证实了EHCO工艺在去除实际废水中的难降解有机物方面具有广泛的应用前景。
更新日期：2024-01-14
中文翻译：
去除磺胺嘧啶的电场增强非均相催化臭氧化 (EHCO) 工艺：阴极还原的作用
在这项工作中，使用制备的 FeOx/PAC 催化剂系统地研究了电场增强非均相催化臭氧化 (EHCO)。与电催化（EC）和非均相催化臭氧化（HCO）工艺相比，EHCO工艺表现出较高的磺胺嘧啶（SDZ）和TOC去除效率。 2分钟内SDZ几乎100%被去除，60分钟内TOC去除率达到约85%。淬火实验和 EPR 分析表明，突出的 SDZ 和 TOC 去除性能是由增强的·OH 生成能力支持的。进一步的研究证明，O电化学还原、过氧酮反应和臭氧电化学还原形成的H2O有助于提高·OH的生成。此外，与传统的HCO系统相比，EHCO系统表现出令人满意的稳定性和可回收性，并且在连续16次回收中SDZ和TOC去除率分别保持在≥95%和≥70%。同时，对HCO和EHCO过程中使用的FeOx/PAC催化剂的XPS分析和Boehm滴定证实，外部电子供应可以抑制PAC表面官能团的氧化并维持Fe(II)/Fe(III)的平衡比，这证明了阴极还原在长时间连续循环过程中催化剂原位再生中的关键作用。此外，EHCO系统在不同的水基质中可以在2分钟内实现超过80%的SDZ去除率。这些结果证实了EHCO工艺在去除实际废水中的难降解有机物方面具有广泛的应用前景。
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