在使用氢/氘动力学同位素效应水解形成二氧化钚纳米颗粒的过程中首次观察到[氢氧化钚酰]簇。
First observation of [Pu(OH)O] cluster during the hydrolytic formation of PuO nanoparticles using H/D kinetic isotope effect.
作者信息
Cot-Auriol Manon, Virot Matthieu, Dumas Thomas, Diat Olivier, Menut Denis, Moisy Philippe, Nikitenko Sergey I
机构信息
ICSM, Univ Montpellier, CEA, CNRS, ENSCM, Marcoule, France.
CEA, DES, ISEC, DMRC, Univ Montpellier, Marcoule, France.
出版信息
Chem Commun (Camb). 2022 Nov 24;58(94):13147-13150. doi: 10.1039/d2cc04990b.
New insights are provided about the formation mechanism of PuO nanoparticles (NPs) by investigating an unprecedented kinetic isotope effect observed during their hydrolytic synthesis in HO or DO and attributed to OH/OD zero point energy difference. The signature of a Pu(IV) oxo-hydroxo hexanuclear cluster, appearing as an important intermediate during the formation of the 2 nm PuO NPs (synchrotron SAXS/XAS), is further revealed indicating that their formation is controlled by H-transfer reactions occurring during hydroxo to oxo-bridge conversions.
通过研究在H₂O或D₂O中水解合成PuO纳米颗粒（NPs）过程中观察到的前所未有的动力学同位素效应，并将其归因于OH/OD零点能量差，为PuO纳米颗粒的形成机制提供了新的见解。进一步揭示了Pu(IV)氧代-氢氧根六核簇的特征，它是2nm PuO纳米颗粒形成过程中的重要中间体（同步加速器小角X射线散射/ X射线吸收光谱），这表明它们的形成受羟基到氧桥转化过程中发生的氢转移反应控制。
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