Shailesh S. Sable , Anett Georgi , Sandra Contreras , Francesc Medina
{"title":"原位生成过氧化氢和Pd/ fe分子筛催化剂对苯酚类fenton氧化的影响","authors":"Shailesh S. Sable , Anett Georgi , Sandra Contreras , Francesc Medina","doi":"10.1016/j.wen.2021.06.001","DOIUrl":null,"url":null,"abstract":"<div><p>Two types of iron-containing zeolites with different surface hydrophobicity, Fe-ZSM5 (SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> = 26) and Fe-ZSM5 (SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> = 236) were studied as adsorbents and catalysts for oxidation of phenol by means of a Fenton-like process at ambient conditions and nearly neutral pH, with and without in-situ generation of H<sub>2</sub>O<sub>2</sub>. Adsorption of phenol is more favorable on high silica Fe-ZSM5 (236) zeolite due to its higher surface hydrophobicity. Palladium (Pd) immobilization on Fe-ZSM5 zeolites has a positive impact on phenol degradation with a synergistic role of Pd and Fe (II)/(III) for activation of H<sub>2</sub>O<sub>2</sub>. The best result for phenol conversion and mineralization was observed over both hydrophilic and hydrophobic 0.1 wt.% Pd/Fe-ZSM5 with commercial H<sub>2</sub>O<sub>2</sub> achieving ≥ 90% conversion of phenol (100 mg/L) in 4 h and 60–63% mineralization in 6 h with 5 g/L catalyst and 5 g/L H<sub>2</sub>O<sub>2</sub>. In addition, Pd/Fe-ZSM5 can be used for in-situ formation of H<sub>2</sub>O<sub>2</sub> using formic acid as H-source and externally supplied oxygen. The combination of these processes provided by this adsorbent/catalyst material is exploitable for on-site oxidative regeneration of zeolite adsorbents. This study shows that Fe-containing zeolites are promising catalysts for a combined approach of adsorption/oxidative degradation of phenol by commercial or in-situ produced H<sub>2</sub>O<sub>2</sub>.</p></div>","PeriodicalId":101279,"journal":{"name":"Water-Energy Nexus","volume":"4 ","pages":"Pages 95-102"},"PeriodicalIF":0.0000,"publicationDate":"2021-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.wen.2021.06.001","citationCount":"4","resultStr":"{\"title\":\"Fenton-like oxidation of phenol with in-situ generated hydrogen peroxide and Pd/Fe-zeolite catalysts\",\"authors\":\"Shailesh S. Sable , Anett Georgi , Sandra Contreras , Francesc Medina\",\"doi\":\"10.1016/j.wen.2021.06.001\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Two types of iron-containing zeolites with different surface hydrophobicity, Fe-ZSM5 (SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> = 26) and Fe-ZSM5 (SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> = 236) were studied as adsorbents and catalysts for oxidation of phenol by means of a Fenton-like process at ambient conditions and nearly neutral pH, with and without in-situ generation of H<sub>2</sub>O<sub>2</sub>. Adsorption of phenol is more favorable on high silica Fe-ZSM5 (236) zeolite due to its higher surface hydrophobicity. Palladium (Pd) immobilization on Fe-ZSM5 zeolites has a positive impact on phenol degradation with a synergistic role of Pd and Fe (II)/(III) for activation of H<sub>2</sub>O<sub>2</sub>. The best result for phenol conversion and mineralization was observed over both hydrophilic and hydrophobic 0.1 wt.% Pd/Fe-ZSM5 with commercial H<sub>2</sub>O<sub>2</sub> achieving ≥ 90% conversion of phenol (100 mg/L) in 4 h and 60–63% mineralization in 6 h with 5 g/L catalyst and 5 g/L H<sub>2</sub>O<sub>2</sub>. In addition, Pd/Fe-ZSM5 can be used for in-situ formation of H<sub>2</sub>O<sub>2</sub> using formic acid as H-source and externally supplied oxygen. The combination of these processes provided by this adsorbent/catalyst material is exploitable for on-site oxidative regeneration of zeolite adsorbents. This study shows that Fe-containing zeolites are promising catalysts for a combined approach of adsorption/oxidative degradation of phenol by commercial or in-situ produced H<sub>2</sub>O<sub>2</sub>.</p></div>\",\"PeriodicalId\":101279,\"journal\":{\"name\":\"Water-Energy Nexus\",\"volume\":\"4 \",\"pages\":\"Pages 95-102\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2021-01-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://sci-hub-pdf.com/10.1016/j.wen.2021.06.001\",\"citationCount\":\"4\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Water-Energy Nexus\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2588912521000084\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Water-Energy Nexus","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2588912521000084","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Fenton-like oxidation of phenol with in-situ generated hydrogen peroxide and Pd/Fe-zeolite catalysts
Two types of iron-containing zeolites with different surface hydrophobicity, Fe-ZSM5 (SiO2/Al2O3 = 26) and Fe-ZSM5 (SiO2/Al2O3 = 236) were studied as adsorbents and catalysts for oxidation of phenol by means of a Fenton-like process at ambient conditions and nearly neutral pH, with and without in-situ generation of H2O2. Adsorption of phenol is more favorable on high silica Fe-ZSM5 (236) zeolite due to its higher surface hydrophobicity. Palladium (Pd) immobilization on Fe-ZSM5 zeolites has a positive impact on phenol degradation with a synergistic role of Pd and Fe (II)/(III) for activation of H2O2. The best result for phenol conversion and mineralization was observed over both hydrophilic and hydrophobic 0.1 wt.% Pd/Fe-ZSM5 with commercial H2O2 achieving ≥ 90% conversion of phenol (100 mg/L) in 4 h and 60–63% mineralization in 6 h with 5 g/L catalyst and 5 g/L H2O2. In addition, Pd/Fe-ZSM5 can be used for in-situ formation of H2O2 using formic acid as H-source and externally supplied oxygen. The combination of these processes provided by this adsorbent/catalyst material is exploitable for on-site oxidative regeneration of zeolite adsorbents. This study shows that Fe-containing zeolites are promising catalysts for a combined approach of adsorption/oxidative degradation of phenol by commercial or in-situ produced H2O2.