María Cabrero-Antonino, Andrés Uscategui-Linares, Rubén Ramírez-Grau, Pablo García-Aznar, Prof. German Sastre, Dr. Jianjun Zhang, Dr. Sara Goberna-Ferrón, Dr. Josep Albero, Prof. Jiaguo Yu, Prof. Hermenegildo García, Dr. Feiyan Xu, Prof. Ana Primo
{"title":"2D/2D MOF/MXene Schottky结：延长载流子寿命和提高析氢效率","authors":"María Cabrero-Antonino, Andrés Uscategui-Linares, Rubén Ramírez-Grau, Pablo García-Aznar, Prof. German Sastre, Dr. Jianjun Zhang, Dr. Sara Goberna-Ferrón, Dr. Josep Albero, Prof. Jiaguo Yu, Prof. Hermenegildo García, Dr. Feiyan Xu, Prof. Ana Primo","doi":"10.1002/ange.202503860","DOIUrl":null,"url":null,"abstract":"<p>Harnessing sunlight for photocatalytic overall water splitting offers a sustainable approach to renewable hydrogen (H<sub>2</sub>) production, addressing global energy and environmental challenges. However, the development of efficient and durable photocatalysts remains a significant obstacle. This study introduces the design and performance of a 2D/2D Schottky heterojunction composed of Cu<sub>2</sub>[CuTCPP] MOF of nanometric size and exfoliated Ti<sub>3</sub>C<sub>2</sub> MXene for visible-light-driven overall water splitting. By leveraging the extensive interfacial contact between the two components, an interfacial electric field is generated, promoting efficient charge migration and prolonging carrier lifetimes, as confirmed through systematic density functional theory simulations, in situ irradiation X-ray photoelectron spectroscopy, femtosecond transient absorption spectroscopy, and X-ray absorption spectroscopy. Ti<sub>3</sub>C<sub>2</sub> MXene, acting as a cocatalyst for photohole transport and accumulation, reduces oxidative degradation and slows catalyst deactivation. The synergistically enhanced light absorption properties of the Cu<sub>2</sub>[CuTCPP]/Ti<sub>3</sub>C<sub>2</sub> heterojunction result in an impressive H<sub>2</sub> evolution rate exceeding 5000 µmol g<sub>cat</sub>⁻<sup>1</sup>, underscoring its potential for next-generation photocatalytic systems in renewable energy applications.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0000,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202503860","citationCount":"0","resultStr":"{\"title\":\"2D/2D MOF/MXene Schottky Junction: Prolonged Carrier Lifetime and Enhanced Hydrogen Evolution Efficiency\",\"authors\":\"María Cabrero-Antonino, Andrés Uscategui-Linares, Rubén Ramírez-Grau, Pablo García-Aznar, Prof. German Sastre, Dr. Jianjun Zhang, Dr. Sara Goberna-Ferrón, Dr. Josep Albero, Prof. Jiaguo Yu, Prof. Hermenegildo García, Dr. Feiyan Xu, Prof. Ana Primo\",\"doi\":\"10.1002/ange.202503860\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Harnessing sunlight for photocatalytic overall water splitting offers a sustainable approach to renewable hydrogen (H<sub>2</sub>) production, addressing global energy and environmental challenges. However, the development of efficient and durable photocatalysts remains a significant obstacle. This study introduces the design and performance of a 2D/2D Schottky heterojunction composed of Cu<sub>2</sub>[CuTCPP] MOF of nanometric size and exfoliated Ti<sub>3</sub>C<sub>2</sub> MXene for visible-light-driven overall water splitting. By leveraging the extensive interfacial contact between the two components, an interfacial electric field is generated, promoting efficient charge migration and prolonging carrier lifetimes, as confirmed through systematic density functional theory simulations, in situ irradiation X-ray photoelectron spectroscopy, femtosecond transient absorption spectroscopy, and X-ray absorption spectroscopy. Ti<sub>3</sub>C<sub>2</sub> MXene, acting as a cocatalyst for photohole transport and accumulation, reduces oxidative degradation and slows catalyst deactivation. The synergistically enhanced light absorption properties of the Cu<sub>2</sub>[CuTCPP]/Ti<sub>3</sub>C<sub>2</sub> heterojunction result in an impressive H<sub>2</sub> evolution rate exceeding 5000 µmol g<sub>cat</sub>⁻<sup>1</sup>, underscoring its potential for next-generation photocatalytic systems in renewable energy applications.</p>\",\"PeriodicalId\":7803,\"journal\":{\"name\":\"Angewandte Chemie\",\"volume\":\"137 29\",\"pages\":\"\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2025-05-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202503860\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Angewandte Chemie\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/ange.202503860\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Angewandte Chemie","FirstCategoryId":"1085","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/ange.202503860","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Harnessing sunlight for photocatalytic overall water splitting offers a sustainable approach to renewable hydrogen (H2) production, addressing global energy and environmental challenges. However, the development of efficient and durable photocatalysts remains a significant obstacle. This study introduces the design and performance of a 2D/2D Schottky heterojunction composed of Cu2[CuTCPP] MOF of nanometric size and exfoliated Ti3C2 MXene for visible-light-driven overall water splitting. By leveraging the extensive interfacial contact between the two components, an interfacial electric field is generated, promoting efficient charge migration and prolonging carrier lifetimes, as confirmed through systematic density functional theory simulations, in situ irradiation X-ray photoelectron spectroscopy, femtosecond transient absorption spectroscopy, and X-ray absorption spectroscopy. Ti3C2 MXene, acting as a cocatalyst for photohole transport and accumulation, reduces oxidative degradation and slows catalyst deactivation. The synergistically enhanced light absorption properties of the Cu2[CuTCPP]/Ti3C2 heterojunction result in an impressive H2 evolution rate exceeding 5000 µmol gcat⁻1, underscoring its potential for next-generation photocatalytic systems in renewable energy applications.
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