Plasmonic Bismuth Nanoparticles: Thiolate Pyrolysis Synthesis, Size-Dependent LSPR Property, and Their Oxidation Behavior,Inorganic Chemistry

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Plasmonic Bismuth Nanoparticles: Thiolate Pyrolysis Synthesis, Size-Dependent LSPR Property, and Their Oxidation Behavior
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2021-10-28 , DOI: 10.1021/acs.inorgchem.1c02621
Dehui Leng ₁ , Tingting Wang ₁ , YingFen Li ₁ , Zibin Huang ₁ , Huimin Wang ₁ , Yixin Wan ₁ , Xiaoxiao Pei ₁ , Junli Wang ₁

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Plasmonics, especially the localized surface plasmon resonance (LSPR) in non-noble metal bismuth nanoparticles (Bi NPs), and its spectral features and applications have stimulated increasing research interest in recent years. However, the lack of mature methods to prepare Bi NPs with a well-controlled size and/or shape significantly limits the experimental investigations concerning the LSPR optical properties. Herein, we realize the size-tunable synthesis of nearly monodisperse spherical Bi NPs through a thiolate pyrolysis reaction in solution. The instantaneous thermolysis of a layered molecular intermediate, bismuth dodecanethiolate [Bi(SC₁₂H₂₅)₃], results in a classical LaMer mechanism for the nucleation and growth of Bi NPs, allowing for a precise size control from 65 to 205 nm in the average diameter. The diameter tunability enables a systematic study on the size dependence of LSPR optical properties of Bi NPs, and we observe rich ultraviolet–visible–near-infrared spectral responses arising from the LSPR absorption and scattering of Bi NPs as their size varies, which will greatly benefit the light harvesting and manipulation in the solar spectrum. Furthermore, we find that a complete oxidation occurs to Bi NPs under air flow at the temperature when they melt and accordingly generate metastable tetragonal-phase β-Bi₂O₃ NPs that show an optical band gap of 2.15 eV and interesting temperature-dependent β → α → δ → (γ + β) polymorphic transitions.

中文翻译：

等离子铋纳米颗粒：硫醇盐热解合成、尺寸相关的 LSPR 特性及其氧化行为

近年来，等离子体，尤其是非贵金属铋纳米粒子 (Bi NPs) 中的局域表面等离子体共振 (LSPR) 及其光谱特征和应用激发了越来越多的研究兴趣。然而，缺乏成熟的方法来制备具有良好控制的尺寸和/或形状的 Bi NPs，这极大地限制了关于 LSPR 光学特性的实验研究。在这里，我们通过溶液中的硫醇盐热解反应实现了几乎单分散的球形 Bi NPs 的尺寸可调合成。层状分子中间体十二烷硫醇铋的瞬时热分解 [Bi(SC ₁₂ H ₂₅ ) ₃]，产生了用于 Bi NPs 成核和生长的经典 LaMer 机制，允许精确控制平均直径为 65 到 205 nm 的尺寸。直径可调性可以系统地研究 Bi NPs 的 LSPR 光学性质的尺寸依赖性，并且我们观察到由于 Bi NPs 的 LSPR 吸收和散射随着尺寸变化而产生的丰富的紫外-可见-近红外光谱响应，这将极大地有利于太阳光谱中的光收集和操纵。此外，我们发现在空气流动下，Bi NPs 在熔化的温度下发生完全氧化，并相应地生成亚稳态四方相 β-Bi ₂ O ₃ NPs 显示 2.15 eV 的光学带隙和有趣的温度相关 β → α → δ → (γ + β) 多态转变。

更新日期：2021-11-15

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