<br>盐催化定向生长双层二硒化钯 (PdSe2) 枝晶和钯纳米颗粒修饰的 PdSe2–Pd2Se3 结，表现出非常高的表面增强拉曼散射灵敏度,Chemistry of Materials

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盐催化定向生长双层二硒化钯 (PdSe2) 枝晶和钯纳米颗粒修饰的 PdSe2–Pd2Se3 结，表现出非常高的表面增强拉曼散射灵敏度
Chemistry of Materials ( IF 7.2 ) Pub Date : 2024-06-10 , DOI: 10.1021/acs.chemmater.4c00078
Tadasha Jena ₁ , Garima Choudhary ₂ , Md Tarik Hossain ₂ , Upasana Nath ₃ , Manabendra Sarma ₃ , P. K. Giri _{1,

2}

Affiliation

虽然大多数二维 (2D) 层状材料的化学计量不会随着层数的减少而改变，但贵重过渡金属中的多层 Pd ₂ Se ₃ 在富硒生长条件下，硫属化物（NTMD）基团将其化学计量改变为双层形式的二硒化钯（PdSe ₂ ）。 PdSe ₂ –Pd ₂ Se ₃ 结的实验实现及其在各种传感应用中的应用仍有待探索。在这里，我们介绍了双层（2L）PdSe ₂ 枝晶和PdSe ₂ –Pd ₂ Se ₃ 云母基板上的结点经过盐溶液预处理。预处理的结构触发熔融 Pd-O 液滴的形成，该液滴经历从 Pd 纳米颗粒 (NP) 到 Pd ₂ Se ₃ （在贫硒条件下）再到 PdSe 的相演化 ₂ （富硒条件下）。树枝状2L PdSe ₂ 可以通过无聚合物水辅助转移技术从生长基底转移到厘米级的任意基底，从而产生丰富的PdSe ₂ –由于转移过程中空位的产生，Pd ₂ Se ₃ 结。值得注意的是，PdSe ₂ –Pd ₂ Se ₃ 结上的 Pd NPs 热点能够以增强因子 (EF ∼ 3 × 10 ⁵ ），比 2L PdSe ₂ 高出 1 个数量级以上，用于检测由于电荷转移和电磁场等多种因素而产生的亚甲基蓝分子增强。密度泛函理论计算和有限元法 (FEM) 模拟以及拉曼成像证实了这一点。有限元模拟显示，Pd NPs 修饰的双层 PdSe _2, 的电场增强因子为 5.546 × 10 ³ ，剩余的增强因子预计将由电荷转移机制贡献。这项工作揭示了2L PdSe ₂ 和PdSe ₂ –Pd ₂ Se ₃

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Salt-Catalyzed Directed Growth of Bilayer Palladium Diselenide (PdSe2) Dendrites and Pd Nanoparticle-Decorated PdSe2–Pd2Se3 Junction Exhibiting Very High Surface Enhanced Raman Scattering Sensitivity

While the chemical stoichiometry does not change with a reduction in layer numbers for most of the two-dimensional (2D) layered materials, the multilayer Pd₂Se₃ in the noble transition-metal chalcogenides (NTMDs) group changes its stoichiometry to palladium diselenide (PdSe₂) in the bilayer form under Se-rich growth conditions. The experimental realization of PdSe₂–Pd₂Se₃ junctions and their application in various sensing applications are yet to be explored. Herein, we introduce a salt (NaCl) catalyzed chemical vapor deposition growth of bilayer (2L) PdSe₂ dendrites and PdSe₂–Pd₂Se₃ junctions on the mica substrate through the salt solution pretreatment. The pretreated structure triggers the formation of molten Pd–O droplets, which undergo a phase evolution from Pd nanoparticles (NPs) to Pd₂Se₃ (in Se-poor condition) to PdSe₂ (in Se-rich condition). Dendritic 2L PdSe₂ can be transferred from a growth substrate to an arbitrary substrate on a centimeter-scale through a polymer-free water-assisted transfer technique, which results in abundant PdSe₂–Pd₂Se₃ junctions due to the vacancy creation during the transfer process. Remarkably, Pd NPs hotspots on PdSe₂–Pd₂Se₃ junctions enable significant surface-enhanced Raman scattering (SERS) enhancement with an enhancement factor (EF ∼ 3 × 10⁵), which is more than 1 order of magnitude higher than that of 2L PdSe₂ to detect methylene blue molecules due to multiple factors, such as charge transfer and electromagnetic field enhancement. This is confirmed by density functional theory calculations and Finite element method (FEM) simulation, along with Raman imaging. The FEM simulations revealed an electric field enhancement factor of 5.546 × 10³ for Pd NPs decorated bilayer PdSe_2, and the remaining enhancement factor is expected to be contributed by charge transfer mechanisms. This work divulges the controllable protocol for the low-temperature chemical vapor deposition growth of 2L PdSe₂ and PdSe₂–Pd₂Se₃ junctions with facile transfer to arbitrary substrates and is indispensable for unleashing its full potential in a wide range of sensing, electronic, photonic, and biomedical applications.

更新日期：2024-06-10

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