{"title":"揭示可见光照射下局部极化中隙态在TiO2/BiVO4异质结中增强载流子转移中的作用。","authors":"Zixi Yin, Xingchen Liu, Guijie Liang, Yin Wang","doi":"10.1038/s41598-025-10259-9","DOIUrl":null,"url":null,"abstract":"<p><p>TiO<sub>2</sub>/BiVO<sub>4</sub> heterojunctions are considered to be one of the most promising materials for photocatalysts due to their extended carrier lifetime, high visible light response, and good stability. However, while Type-II TiO<sub>2</sub>/BiVO<sub>4</sub> heterojunctions are well-studied, the fundamental mechanism behind the Type-I configurations remains unclear, particularly regarding their unexpected high photocatalytic activity despite theoretically unfavorable band alignment. Herein, we reveal that localized polaronic mid-gap states (SP states) can mediate efficient charge transfer and recombination in TiO<sub>2</sub>/BiVO<sub>4</sub> using time-resolved photoluminescence (PL) spectroscopy and transient absorption spectroscopy (TAS), providing direct experimental evidence of this mechanism. The existence of SP states enables exceptional methyl orange degradation efficiency (nearly 100% in 1 h under visible light) despite the theoretically unfavorable Type-I alignment. This work redefines the potential of Type-I systems for visible-light photocatalysis by demonstrating how polaron engineering overcomes the limitations of traditional band structures, advancing their applications in solar utilization.</p>","PeriodicalId":21811,"journal":{"name":"Scientific Reports","volume":"15 1","pages":"24343"},"PeriodicalIF":3.9000,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12234835/pdf/","citationCount":"0","resultStr":"{\"title\":\"Unveiling the role of localized polaronic mid-gap states in enhanced carrier transfer in TiO<sub>2</sub>/BiVO<sub>4</sub> heterojunctions under visible light irradiation.\",\"authors\":\"Zixi Yin, Xingchen Liu, Guijie Liang, Yin Wang\",\"doi\":\"10.1038/s41598-025-10259-9\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>TiO<sub>2</sub>/BiVO<sub>4</sub> heterojunctions are considered to be one of the most promising materials for photocatalysts due to their extended carrier lifetime, high visible light response, and good stability. However, while Type-II TiO<sub>2</sub>/BiVO<sub>4</sub> heterojunctions are well-studied, the fundamental mechanism behind the Type-I configurations remains unclear, particularly regarding their unexpected high photocatalytic activity despite theoretically unfavorable band alignment. Herein, we reveal that localized polaronic mid-gap states (SP states) can mediate efficient charge transfer and recombination in TiO<sub>2</sub>/BiVO<sub>4</sub> using time-resolved photoluminescence (PL) spectroscopy and transient absorption spectroscopy (TAS), providing direct experimental evidence of this mechanism. The existence of SP states enables exceptional methyl orange degradation efficiency (nearly 100% in 1 h under visible light) despite the theoretically unfavorable Type-I alignment. This work redefines the potential of Type-I systems for visible-light photocatalysis by demonstrating how polaron engineering overcomes the limitations of traditional band structures, advancing their applications in solar utilization.</p>\",\"PeriodicalId\":21811,\"journal\":{\"name\":\"Scientific Reports\",\"volume\":\"15 1\",\"pages\":\"24343\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2025-07-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12234835/pdf/\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Scientific Reports\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://doi.org/10.1038/s41598-025-10259-9\",\"RegionNum\":2,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MULTIDISCIPLINARY SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Scientific Reports","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41598-025-10259-9","RegionNum":2,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
Unveiling the role of localized polaronic mid-gap states in enhanced carrier transfer in TiO2/BiVO4 heterojunctions under visible light irradiation.
TiO2/BiVO4 heterojunctions are considered to be one of the most promising materials for photocatalysts due to their extended carrier lifetime, high visible light response, and good stability. However, while Type-II TiO2/BiVO4 heterojunctions are well-studied, the fundamental mechanism behind the Type-I configurations remains unclear, particularly regarding their unexpected high photocatalytic activity despite theoretically unfavorable band alignment. Herein, we reveal that localized polaronic mid-gap states (SP states) can mediate efficient charge transfer and recombination in TiO2/BiVO4 using time-resolved photoluminescence (PL) spectroscopy and transient absorption spectroscopy (TAS), providing direct experimental evidence of this mechanism. The existence of SP states enables exceptional methyl orange degradation efficiency (nearly 100% in 1 h under visible light) despite the theoretically unfavorable Type-I alignment. This work redefines the potential of Type-I systems for visible-light photocatalysis by demonstrating how polaron engineering overcomes the limitations of traditional band structures, advancing their applications in solar utilization.
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