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Heterogeneous activation of peroxymonosulfate over porous graphitized carbon-supported CoS catalyst for efficient removal of gaseous chlorobenzene
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2024-02-20 , DOI: 10.1016/j.cej.2024.149831 Cong Pan , Yihui Zhang , Wenyu Wang , Feng Wu , Zhixiong You , Jing Xu , Jinjun Li
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2024-02-20 , DOI: 10.1016/j.cej.2024.149831 Cong Pan , Yihui Zhang , Wenyu Wang , Feng Wu , Zhixiong You , Jing Xu , Jinjun Li
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Chlorobenzene (CB) is a typical example of chlorinated volatile organic compounds (CVOCs) that require pollution control. Using wet scrubbers coupled with advanced oxidation processes (AOPs) has become a promising technique to degrade gaseous CVOCs. Here, a CoS-loaded porous graphitized carbon (PGC) served as an adsorbent for CVOCs and a catalyst to activate peroxymonosulfate (PMS) to construct a wet scrubber for CB degradation. CoS/PGC exhibited excellent catalytic performance at pH 9.0; a 0.1 g/L CoS/PGC dosage and a 10 mM initial PMS concentration achieved 90% CB (25 ppmv) removal within 500 min. Electron spin resonance and quenching experiments identified hydroxyl radicals and sulfate radicals as the main reactive oxygen species that removed CB. In addition, we proposed possible CB degradation pathways by intermediates identified using liquid chromatography-mass spectrometry and density functional theory calculations. Electrochemical experimental results such as cyclic voltammetry and Nyquist proved that CoS/PGC has superior electron transport capacity compared to CoS. A possible catalytic mechanism for CB removal in CoS/PGC + PMS system was proposed by ESR and XPS spectra. By using continuous dosing or pulsed dosing to replenish PMS to maintain its suitable concentration, the system achieves a commendable long-term efficiency. Moreover, this catalyst displayed excellent recyclability and universal applicability to treat various gaseous CVOCs as well as the scrubbing solution replacement with tap water for efficient CB removal. This study may provide new fundamental insights into the PGC-supported catalysts for wet oxidation of CVOCs or other contaminants.
中文翻译:
多孔石墨化碳载 CoS 催化剂上过一硫酸盐的非均相活化有效去除气态氯苯
氯苯(CB)是需要污染控制的氯化挥发性有机化合物(CVOC)的典型例子。使用湿式洗涤器与高级氧化工艺 (AOP) 相结合已成为一种有前途的降解气态 CVOC 的技术。在这里,负载 CoS 的多孔石墨化碳 (PGC) 用作 CVOC 的吸附剂和激活过一硫酸盐 (PMS) 的催化剂,以构建用于 CB 降解的湿式洗涤器。 CoS/PGC在pH 9.0时表现出优异的催化性能; 0.1 g/L CoS/PGC 剂量和 10 mM 初始 PMS 浓度可在 500 分钟内实现 90% CB (25 ppmv) 去除。电子自旋共振和猝灭实验确定羟基自由基和硫酸根自由基是去除CB的主要活性氧。此外,我们提出了使用液相色谱-质谱法和密度泛函理论计算确定的中间体可能的CB降解途径。循环伏安、奈奎斯特等电化学实验结果证明,CoS/PGC相比CoS具有更优越的电子传输能力。通过ESR和XPS谱提出了CoS/PGC + PMS系统中去除CB的可能催化机制。通过使用连续加药或脉冲加药来补充PMS以维持其合适的浓度,该系统实现了值得称赞的长期效率。此外,该催化剂表现出优异的可回收性和普遍适用性,可处理各种气态CVOC,以及用自来水替代洗涤液以有效去除CB。这项研究可能为用于 CVOC 或其他污染物湿式氧化的 PGC 支撑催化剂提供新的基本见解。
更新日期:2024-02-20
中文翻译:

多孔石墨化碳载 CoS 催化剂上过一硫酸盐的非均相活化有效去除气态氯苯
氯苯(CB)是需要污染控制的氯化挥发性有机化合物(CVOC)的典型例子。使用湿式洗涤器与高级氧化工艺 (AOP) 相结合已成为一种有前途的降解气态 CVOC 的技术。在这里,负载 CoS 的多孔石墨化碳 (PGC) 用作 CVOC 的吸附剂和激活过一硫酸盐 (PMS) 的催化剂,以构建用于 CB 降解的湿式洗涤器。 CoS/PGC在pH 9.0时表现出优异的催化性能; 0.1 g/L CoS/PGC 剂量和 10 mM 初始 PMS 浓度可在 500 分钟内实现 90% CB (25 ppmv) 去除。电子自旋共振和猝灭实验确定羟基自由基和硫酸根自由基是去除CB的主要活性氧。此外,我们提出了使用液相色谱-质谱法和密度泛函理论计算确定的中间体可能的CB降解途径。循环伏安、奈奎斯特等电化学实验结果证明,CoS/PGC相比CoS具有更优越的电子传输能力。通过ESR和XPS谱提出了CoS/PGC + PMS系统中去除CB的可能催化机制。通过使用连续加药或脉冲加药来补充PMS以维持其合适的浓度,该系统实现了值得称赞的长期效率。此外,该催化剂表现出优异的可回收性和普遍适用性,可处理各种气态CVOC,以及用自来水替代洗涤液以有效去除CB。这项研究可能为用于 CVOC 或其他污染物湿式氧化的 PGC 支撑催化剂提供新的基本见解。