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Effect of support structure of Pt/silicaite-1 catalyst on non-thermal plasma (NTP) assisted chlorobenzene degradation and PCDD/Fs formation
Chemosphere ( IF 8.1 ) Pub Date : 2024-05-09 , DOI: 10.1016/j.chemosphere.2024.142294
Yibing Mu 1 , Yilai Jiao 2 , Xinrui Wang 3 , Paul T Williams 1
Chemosphere ( IF 8.1 ) Pub Date : 2024-05-09 , DOI: 10.1016/j.chemosphere.2024.142294
Yibing Mu 1 , Yilai Jiao 2 , Xinrui Wang 3 , Paul T Williams 1
Affiliation
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Development of efficient catalysts for non-thermal plasma (NTP) assisted catalysis to mitigate the formation of harmful by-products is a significant challenge in the degradation of chlorinated volatile organic compounds (Cl–VOCs). In this study, catalytically active Pt nanoparticles supported on non-porous SiO2 and silicalite-1 zeolites (S1) with different pore structure were comparatively investigated for catalytic chlorobenzene degradation under NTP condition. It was shown that the pore structure could significantly impact the metal size and metal dispersion rate. Pt supported on modified S1 hierarchical meso-micro-porous silicalite-1 (Pt/D-S1) exhibited the smallest particle size (∼6.19 nm) and the highest dispersion rate (∼1.87). Additionally, Pt/D-S1 demonstrated superior catalytic performance compared to the other catalysts, achieving the highest chlorobenzene conversion and COx selectivity at about 80% and 75%, respectively. Furthermore, the pore structure also affected the formation of by-products according to the findings from GC-MS analysis. Pt/SiO2 generated a total of 18 different species of organic compounds, whereas only 12 species of organic by-products were identified in the Pt/D-S1 system (e.g. polychlorinated compounds like 3,4 dichlorophenol were exclusively identified in Pt/SiO2 ). Moreover, dioxin-like polychlorinated biphenyl and other chlorinated organic compounds, which have potential to form highly toxic dioxins, were detected in the catalysts. HRGC-HRMS confirmed and quantified the 17 different dioxin/furans formed on Pt/SiO2 (25,100 ng TEQ kg−1 ), Pt/S1 (515 ng TEQ kg−1 ) and Pt/D-S1 (367 ng TEQ kg−1 ). The correlation between synthesis-structure-performance in this study provides insights into the design of catalysts for deep oxidation of Cl–VOCs in NTP system.
中文翻译:
Pt/硅酸盐-1 催化剂的支撑结构对非热等离子体 (NTP) 辅助氯苯降解和 PCDD/Fs 形成的影响
开发用于非热等离子体 (NTP) 辅助催化的高效催化剂以减少有害副产物的形成是降解氯化挥发性有机化合物 (Cl-VOC) 的重大挑战。在本研究中,比较研究了负载在具有不同孔结构的无孔 SiO2 和硅石-1 分子筛 (S1) 上的催化活性 Pt 纳米颗粒在 NTP 条件下催化氯苯降解的性能。结果表明,孔结构可以显着影响金属尺寸和金属分散速率。改性 S1 多级介微孔硅石-1 (Pt/D-S1) 上负载的 Pt 表现出最小的粒径 (∼6.19 nm) 和最高的色散速率 (∼1.87)。此外,与其他催化剂相比,Pt/D-S1 表现出优异的催化性能,分别实现了最高的氯苯转化率和 COx 选择性,分别约为 80% 和 75%。此外,根据 GC-MS 分析的结果,孔结构还影响了副产物的形成。Pt/SiO2 共产生 18 种不同种类的有机化合物,而在 Pt/D-S1 系统中仅鉴定出 12 种有机副产物(例如,在 Pt/SiO2 中仅鉴定出 3,4 二氯苯酚等多氯化合物)。此外,在催化剂中检测到类似二恶英的多氯联苯和其他氯化有机化合物,它们有可能形成剧毒的二恶英。HRGC-HRMS 确认并量化了在 Pt/SiO2 (25,100 ng TEQ kg-1)、Pt/S1 (515 ng TEQ kg-1) 和 Pt/D-S1 (367 ng TEQ kg-1) 上形成的 17 种不同的二恶英/呋喃。 本研究中合成-结构-性能之间的相关性为 NTP 体系中 Cl-VOCs 深度氧化催化剂的设计提供了见解。
更新日期:2024-05-09
中文翻译:
![](https://scdn.x-mol.com/jcss/images/paperTranslation.png)
Pt/硅酸盐-1 催化剂的支撑结构对非热等离子体 (NTP) 辅助氯苯降解和 PCDD/Fs 形成的影响
开发用于非热等离子体 (NTP) 辅助催化的高效催化剂以减少有害副产物的形成是降解氯化挥发性有机化合物 (Cl-VOC) 的重大挑战。在本研究中,比较研究了负载在具有不同孔结构的无孔 SiO2 和硅石-1 分子筛 (S1) 上的催化活性 Pt 纳米颗粒在 NTP 条件下催化氯苯降解的性能。结果表明,孔结构可以显着影响金属尺寸和金属分散速率。改性 S1 多级介微孔硅石-1 (Pt/D-S1) 上负载的 Pt 表现出最小的粒径 (∼6.19 nm) 和最高的色散速率 (∼1.87)。此外,与其他催化剂相比,Pt/D-S1 表现出优异的催化性能,分别实现了最高的氯苯转化率和 COx 选择性,分别约为 80% 和 75%。此外,根据 GC-MS 分析的结果,孔结构还影响了副产物的形成。Pt/SiO2 共产生 18 种不同种类的有机化合物,而在 Pt/D-S1 系统中仅鉴定出 12 种有机副产物(例如,在 Pt/SiO2 中仅鉴定出 3,4 二氯苯酚等多氯化合物)。此外,在催化剂中检测到类似二恶英的多氯联苯和其他氯化有机化合物,它们有可能形成剧毒的二恶英。HRGC-HRMS 确认并量化了在 Pt/SiO2 (25,100 ng TEQ kg-1)、Pt/S1 (515 ng TEQ kg-1) 和 Pt/D-S1 (367 ng TEQ kg-1) 上形成的 17 种不同的二恶英/呋喃。 本研究中合成-结构-性能之间的相关性为 NTP 体系中 Cl-VOCs 深度氧化催化剂的设计提供了见解。