Ziyue Zhang, Yi Ding, Xin Hua, Lingli Song, Songqin Liu
{"title":"水界面加速协同光- fenton /光催化反应","authors":"Ziyue Zhang, Yi Ding, Xin Hua, Lingli Song, Songqin Liu","doi":"10.1021/acsami.4c21187","DOIUrl":null,"url":null,"abstract":"Photocatalysis and photo-Fenton oxidation are promising advanced oxidation technologies for water treatment. Nevertheless, their relatively slow kinetics largely limited their practical applications. Herein, we performed synergistic photocatalysis and photo-Fenton reactions in water microdroplets for the degradation of organic dyes. The efficiency of the microdroplet-based photoreactions was significantly improved with a degradation rate of 98.96% in microdroplets, while it was only 38.14% in the bulk solution. The enhanced degradation efficiency was due to the synergistic effect of the photocatalysis and photo-Fenton reactions in the microdroplets. First, the enrichment of both the dye (rhodamine B) and the catalyst (g-C<sub>3</sub>N<sub>4</sub> nanosheets) at the aqueous interfaces enlarged the local surface concentration, playing a role in the reaction acceleration. Second, the spontaneously generated hydrogen peroxide (17.13 μM) at the aqueous interfaces triggered the photo-Fenton cycle and thus largely promoted the charge separation of g-C<sub>3</sub>N<sub>4</sub> as well as the effective utilization of the photogenerated electrons and holes, leading to a significantly improved degradation efficiency of organic dyes. Further, we quantified the reaction kinetics of individual microdroplets in a real-time manner. The reaction constant in 10 μm microdroplets was 4.86 × 10<sup>–3</sup> s<sup>–1</sup>, which was 22 times higher than that in the bulk phase (0.22 × 10<sup>–3</sup> s<sup>–1</sup>). This study provided a better understanding of accelerated photoreactions at aqueous interfaces and a strategy for addressing the low efficiency of organic dye degradation.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"132 1","pages":""},"PeriodicalIF":8.2000,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Accelerated Synergistic Photo-Fenton/Photocatalysis Reactions at Aqueous Interfaces\",\"authors\":\"Ziyue Zhang, Yi Ding, Xin Hua, Lingli Song, Songqin Liu\",\"doi\":\"10.1021/acsami.4c21187\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Photocatalysis and photo-Fenton oxidation are promising advanced oxidation technologies for water treatment. Nevertheless, their relatively slow kinetics largely limited their practical applications. Herein, we performed synergistic photocatalysis and photo-Fenton reactions in water microdroplets for the degradation of organic dyes. The efficiency of the microdroplet-based photoreactions was significantly improved with a degradation rate of 98.96% in microdroplets, while it was only 38.14% in the bulk solution. The enhanced degradation efficiency was due to the synergistic effect of the photocatalysis and photo-Fenton reactions in the microdroplets. First, the enrichment of both the dye (rhodamine B) and the catalyst (g-C<sub>3</sub>N<sub>4</sub> nanosheets) at the aqueous interfaces enlarged the local surface concentration, playing a role in the reaction acceleration. Second, the spontaneously generated hydrogen peroxide (17.13 μM) at the aqueous interfaces triggered the photo-Fenton cycle and thus largely promoted the charge separation of g-C<sub>3</sub>N<sub>4</sub> as well as the effective utilization of the photogenerated electrons and holes, leading to a significantly improved degradation efficiency of organic dyes. Further, we quantified the reaction kinetics of individual microdroplets in a real-time manner. The reaction constant in 10 μm microdroplets was 4.86 × 10<sup>–3</sup> s<sup>–1</sup>, which was 22 times higher than that in the bulk phase (0.22 × 10<sup>–3</sup> s<sup>–1</sup>). This study provided a better understanding of accelerated photoreactions at aqueous interfaces and a strategy for addressing the low efficiency of organic dye degradation.\",\"PeriodicalId\":5,\"journal\":{\"name\":\"ACS Applied Materials & Interfaces\",\"volume\":\"132 1\",\"pages\":\"\"},\"PeriodicalIF\":8.2000,\"publicationDate\":\"2025-02-09\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Materials & Interfaces\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acsami.4c21187\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Materials & Interfaces","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsami.4c21187","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Accelerated Synergistic Photo-Fenton/Photocatalysis Reactions at Aqueous Interfaces
Photocatalysis and photo-Fenton oxidation are promising advanced oxidation technologies for water treatment. Nevertheless, their relatively slow kinetics largely limited their practical applications. Herein, we performed synergistic photocatalysis and photo-Fenton reactions in water microdroplets for the degradation of organic dyes. The efficiency of the microdroplet-based photoreactions was significantly improved with a degradation rate of 98.96% in microdroplets, while it was only 38.14% in the bulk solution. The enhanced degradation efficiency was due to the synergistic effect of the photocatalysis and photo-Fenton reactions in the microdroplets. First, the enrichment of both the dye (rhodamine B) and the catalyst (g-C3N4 nanosheets) at the aqueous interfaces enlarged the local surface concentration, playing a role in the reaction acceleration. Second, the spontaneously generated hydrogen peroxide (17.13 μM) at the aqueous interfaces triggered the photo-Fenton cycle and thus largely promoted the charge separation of g-C3N4 as well as the effective utilization of the photogenerated electrons and holes, leading to a significantly improved degradation efficiency of organic dyes. Further, we quantified the reaction kinetics of individual microdroplets in a real-time manner. The reaction constant in 10 μm microdroplets was 4.86 × 10–3 s–1, which was 22 times higher than that in the bulk phase (0.22 × 10–3 s–1). This study provided a better understanding of accelerated photoreactions at aqueous interfaces and a strategy for addressing the low efficiency of organic dye degradation.
期刊介绍:
ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.