Santu Shrestha, Ga Hyeon Ha, Narayan Gyawali, Subas Acharya, Insup Lee, Harshvardhan Mohan, Taeho Shin and Jae Ryang Hahn*,
{"title":"晶格匹配CdS@Ag2S g-C3N4的核壳结构:一种高性能可见光下的氢演化和污染物降解光催化剂","authors":"Santu Shrestha, Ga Hyeon Ha, Narayan Gyawali, Subas Acharya, Insup Lee, Harshvardhan Mohan, Taeho Shin and Jae Ryang Hahn*, ","doi":"10.1021/acsaem.5c02363","DOIUrl":null,"url":null,"abstract":"<p >A CdS@Ag<sub>2</sub>S core–shell architecture (CSAS) was fabricated via a low-temperature cation-exchange reaction between CdS and AgNO<sub>3</sub>, followed by hydrothermal integration with graphitic carbon nitride to form a CdS@Ag<sub>2</sub>S–g-C<sub>3</sub>N<sub>4</sub> (CSAS–g) composite. The development of a lattice-matched built-in electric field at the CSAS effectively overcame key limitations of conventional heterojunctions such as random material combinations, lattice mismatches, and high interfacial resistance, thereby significantly enhancing photocatalytic efficiency. The CSAS–g composite demonstrated remarkable bifunctional performance, achieving a significant H<sub>2</sub> production rate (1497.2 μmol g<sup>–1</sup> h<sup>–1</sup>), corresponding to a solar-to-hydrogen efficiency (1.63%) and an apparent quantum efficiency of 3.62%─which are 35.4 and 2.1 times higher than those of CdS nanoparticles (CdS-NPs) and CSAS, respectively. Additionally, CSAS–g exhibited outstanding photocatalytic decomposition of several pollutants, including bisphenol A, methylene blue, Rhodamine 6G, and Congo red. Notably, the methylene blue degradation rate of CSAS–g was 937.5% higher than that of photolysis and significantly outperformed CdS-NPs, CSAS, and g-C<sub>3</sub>N<sub>4</sub>. The exceptional photocatalytic efficacy and durability of CSAS–g were ascribed to the cooperative effects of the core–shell structure and g-C<sub>3</sub>N<sub>4</sub> integration, which resulted in superior light absorption, efficient charge separation, accelerated interfacial charge transport, and an abundance of active centers. Furthermore, the core–shell design provided enhanced photocorrosion resistance, ensuring long-term stability. This study highlights the transformative potential of lattice-matched core–shell heterostructures in advancing next-generation photocatalysts for renewable hydrogen production and pollution control.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 17","pages":"12969–12983"},"PeriodicalIF":5.5000,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Lattice-Matched CdS@Ag2S Core–Shell Structures on g-C3N4: A High-Performance Photocatalyst for Hydrogen Evolution and Pollutant Degradation under Visible Light\",\"authors\":\"Santu Shrestha, Ga Hyeon Ha, Narayan Gyawali, Subas Acharya, Insup Lee, Harshvardhan Mohan, Taeho Shin and Jae Ryang Hahn*, \",\"doi\":\"10.1021/acsaem.5c02363\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >A CdS@Ag<sub>2</sub>S core–shell architecture (CSAS) was fabricated via a low-temperature cation-exchange reaction between CdS and AgNO<sub>3</sub>, followed by hydrothermal integration with graphitic carbon nitride to form a CdS@Ag<sub>2</sub>S–g-C<sub>3</sub>N<sub>4</sub> (CSAS–g) composite. The development of a lattice-matched built-in electric field at the CSAS effectively overcame key limitations of conventional heterojunctions such as random material combinations, lattice mismatches, and high interfacial resistance, thereby significantly enhancing photocatalytic efficiency. The CSAS–g composite demonstrated remarkable bifunctional performance, achieving a significant H<sub>2</sub> production rate (1497.2 μmol g<sup>–1</sup> h<sup>–1</sup>), corresponding to a solar-to-hydrogen efficiency (1.63%) and an apparent quantum efficiency of 3.62%─which are 35.4 and 2.1 times higher than those of CdS nanoparticles (CdS-NPs) and CSAS, respectively. Additionally, CSAS–g exhibited outstanding photocatalytic decomposition of several pollutants, including bisphenol A, methylene blue, Rhodamine 6G, and Congo red. Notably, the methylene blue degradation rate of CSAS–g was 937.5% higher than that of photolysis and significantly outperformed CdS-NPs, CSAS, and g-C<sub>3</sub>N<sub>4</sub>. The exceptional photocatalytic efficacy and durability of CSAS–g were ascribed to the cooperative effects of the core–shell structure and g-C<sub>3</sub>N<sub>4</sub> integration, which resulted in superior light absorption, efficient charge separation, accelerated interfacial charge transport, and an abundance of active centers. Furthermore, the core–shell design provided enhanced photocorrosion resistance, ensuring long-term stability. 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Lattice-Matched CdS@Ag2S Core–Shell Structures on g-C3N4: A High-Performance Photocatalyst for Hydrogen Evolution and Pollutant Degradation under Visible Light
A CdS@Ag2S core–shell architecture (CSAS) was fabricated via a low-temperature cation-exchange reaction between CdS and AgNO3, followed by hydrothermal integration with graphitic carbon nitride to form a CdS@Ag2S–g-C3N4 (CSAS–g) composite. The development of a lattice-matched built-in electric field at the CSAS effectively overcame key limitations of conventional heterojunctions such as random material combinations, lattice mismatches, and high interfacial resistance, thereby significantly enhancing photocatalytic efficiency. The CSAS–g composite demonstrated remarkable bifunctional performance, achieving a significant H2 production rate (1497.2 μmol g–1 h–1), corresponding to a solar-to-hydrogen efficiency (1.63%) and an apparent quantum efficiency of 3.62%─which are 35.4 and 2.1 times higher than those of CdS nanoparticles (CdS-NPs) and CSAS, respectively. Additionally, CSAS–g exhibited outstanding photocatalytic decomposition of several pollutants, including bisphenol A, methylene blue, Rhodamine 6G, and Congo red. Notably, the methylene blue degradation rate of CSAS–g was 937.5% higher than that of photolysis and significantly outperformed CdS-NPs, CSAS, and g-C3N4. The exceptional photocatalytic efficacy and durability of CSAS–g were ascribed to the cooperative effects of the core–shell structure and g-C3N4 integration, which resulted in superior light absorption, efficient charge separation, accelerated interfacial charge transport, and an abundance of active centers. Furthermore, the core–shell design provided enhanced photocorrosion resistance, ensuring long-term stability. This study highlights the transformative potential of lattice-matched core–shell heterostructures in advancing next-generation photocatalysts for renewable hydrogen production and pollution control.
期刊介绍:
ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.