Marco Montalbano, Gianluigi Marra, Mariangela Longhi, Laura Prati, Elena Selli, Maria Vittoria Dozzi
{"title":"{001}面富集形态和金纳米颗粒沉积对铝钛矿二氧化钛光活性的共同作用","authors":"Marco Montalbano, Gianluigi Marra, Mariangela Longhi, Laura Prati, Elena Selli, Maria Vittoria Dozzi","doi":"10.1021/acsami.4c12465","DOIUrl":null,"url":null,"abstract":"The interplay on anatase TiO<sub>2</sub> photoactivity between particle morphology and gold nanoparticles (NPs) deposition, via either deposition–precipitation (DP) or photodeposition (P), is here investigated by evaluating the photoactivity of Au modified anatase (Au/TiO<sub>2</sub>) nanocrystals with either a pseudospherical shape or a nanosheet structure in both reduction and oxidation test reactions. The presence of Au NPs on the anatase surface only slightly affects its photoactivity in Cr(VI) reduction, which is kinetically limited by the anodic half-reaction, whereas a larger exposure of highly oxidant {001} facets is beneficial for overcoming this rate-determining step. In the photocatalytic oxidation of both formic acid, proceeding through a direct mechanism, and rhodamine B (RhB) on surface fluorinated photocatalysts, occurring through a hydroxyl-radical-mediated mechanism, the presence of gold NPs produces a significant photoactivity increase only with spherically shaped photocatalysts, mainly exposing {101} facets. These results are rationalized in light of the preferential migration of photogenerated, oppositely charged carriers toward different crystal facets. In fact, when the Au/TiO<sub>2</sub> material mainly exposes the more oxidant {001} facets, where photoproduced holes preferentially migrate, recombination between these latter and the electrons captured by Au NPs is favored. Instead, Au NPs on {101} facets efficiently capture photopromoted electrons, preferentially migrating toward such facets with a consequent improvement of photoproduced charge separation.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3000,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Combined Role of {001} Facet-Enriched Morphology and Gold Nanoparticle Deposition on Anatase TiO2 Photoactivity\",\"authors\":\"Marco Montalbano, Gianluigi Marra, Mariangela Longhi, Laura Prati, Elena Selli, Maria Vittoria Dozzi\",\"doi\":\"10.1021/acsami.4c12465\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The interplay on anatase TiO<sub>2</sub> photoactivity between particle morphology and gold nanoparticles (NPs) deposition, via either deposition–precipitation (DP) or photodeposition (P), is here investigated by evaluating the photoactivity of Au modified anatase (Au/TiO<sub>2</sub>) nanocrystals with either a pseudospherical shape or a nanosheet structure in both reduction and oxidation test reactions. The presence of Au NPs on the anatase surface only slightly affects its photoactivity in Cr(VI) reduction, which is kinetically limited by the anodic half-reaction, whereas a larger exposure of highly oxidant {001} facets is beneficial for overcoming this rate-determining step. In the photocatalytic oxidation of both formic acid, proceeding through a direct mechanism, and rhodamine B (RhB) on surface fluorinated photocatalysts, occurring through a hydroxyl-radical-mediated mechanism, the presence of gold NPs produces a significant photoactivity increase only with spherically shaped photocatalysts, mainly exposing {101} facets. These results are rationalized in light of the preferential migration of photogenerated, oppositely charged carriers toward different crystal facets. In fact, when the Au/TiO<sub>2</sub> material mainly exposes the more oxidant {001} facets, where photoproduced holes preferentially migrate, recombination between these latter and the electrons captured by Au NPs is favored. 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Combined Role of {001} Facet-Enriched Morphology and Gold Nanoparticle Deposition on Anatase TiO2 Photoactivity
The interplay on anatase TiO2 photoactivity between particle morphology and gold nanoparticles (NPs) deposition, via either deposition–precipitation (DP) or photodeposition (P), is here investigated by evaluating the photoactivity of Au modified anatase (Au/TiO2) nanocrystals with either a pseudospherical shape or a nanosheet structure in both reduction and oxidation test reactions. The presence of Au NPs on the anatase surface only slightly affects its photoactivity in Cr(VI) reduction, which is kinetically limited by the anodic half-reaction, whereas a larger exposure of highly oxidant {001} facets is beneficial for overcoming this rate-determining step. In the photocatalytic oxidation of both formic acid, proceeding through a direct mechanism, and rhodamine B (RhB) on surface fluorinated photocatalysts, occurring through a hydroxyl-radical-mediated mechanism, the presence of gold NPs produces a significant photoactivity increase only with spherically shaped photocatalysts, mainly exposing {101} facets. These results are rationalized in light of the preferential migration of photogenerated, oppositely charged carriers toward different crystal facets. In fact, when the Au/TiO2 material mainly exposes the more oxidant {001} facets, where photoproduced holes preferentially migrate, recombination between these latter and the electrons captured by Au NPs is favored. Instead, Au NPs on {101} facets efficiently capture photopromoted electrons, preferentially migrating toward such facets with a consequent improvement of photoproduced charge separation.
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.