Lattice-Matched CdS@Ag2S Core–Shell Structures on g-C3N4: A High-Performance Photocatalyst for Hydrogen Evolution and Pollutant Degradation under Visible Light

IF 5.5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL
Santu Shrestha, Ga Hyeon Ha, Narayan Gyawali, Subas Acharya, Insup Lee, Harshvardhan Mohan, Taeho Shin and Jae Ryang Hahn*, 
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Abstract

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.

Abstract Image

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
通过CdS与AgNO3低温阳离子交换反应制备了CdS@Ag2S核壳结构(CSAS),然后与石墨氮化碳水热合成CdS@Ag2S -g-C3N4 (CSAS - g)复合材料。在CSAS中开发的晶格匹配内置电场有效地克服了传统异质结的关键限制,如随机材料组合,晶格不匹配和高界面电阻,从而显着提高了光催化效率。csa - g复合材料表现出显著的双功能性能,H2产率为1497.2 μmol g-1 h-1,太阳能制氢效率为1.63%,表观量子效率为3.62%,分别是CdS纳米粒子(CdS- nps)和CSAS的35.4倍和2.1倍。此外,CSAS-g对双酚A、亚甲基蓝、罗丹明6G和刚果红等多种污染物表现出出色的光催化分解能力。值得注意的是,csa - g对亚甲基蓝的降解率比光解提高了937.5%,显著优于CdS-NPs、CSAS和g-C3N4。CSAS-g优异的光催化效果和耐久性是由于核壳结构和g-C3N4集成的协同作用,从而产生了优异的光吸收、高效的电荷分离、加速的界面电荷传输和丰富的活性中心。此外,核壳设计增强了抗光腐蚀能力,确保了长期稳定性。这项研究强调了晶格匹配核壳异质结构在推进下一代光催化剂用于可再生制氢和污染控制方面的变革潜力。
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来源期刊
ACS Applied Energy Materials
ACS Applied Energy Materials Materials Science-Materials Chemistry
CiteScore
10.30
自引率
6.20%
发文量
1368
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.
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