Electrochemical Ce(III)/Ce(IV) Redox Behavior and Ce Oxide Nanostructure Recovery over Thio-Terpyridine-Functionalized Au/Carbon Paper Electrodes,ACS Applied Materials & Interfaces

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Electrochemical Ce(III)/Ce(IV) Redox Behavior and Ce Oxide Nanostructure Recovery over Thio-Terpyridine-Functionalized Au/Carbon Paper Electrodes
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-06-03 , DOI: 10.1021/acsami.1c05105
So Jeong Park ₁ , Min Hee Joo _{1,

2} , Ju Hyun Yang _{1,

2} , Sung-Min Hong _{1,

2} , Choong Kyun Rhee ₁ , Jun-Gill Kang ₃ , Youngku Sohn _{1,

2}

Affiliation

Understanding the electrochemical behaviors of Ce(III)/Ce(IV) ions is essential for better treatment, separation, and recycling of lanthanide (Ln) and actinide (An) elements. Herein, electrochemical redox behavior and interconversion of Ce(III)/Ce(IV) ions and their recoveries were demonstrated over newly developed thio-terpyridine-functionalized Au-modified carbon paper electrodes in acidic and neutral electrolytes. Cyclic voltammetry and amperometry were performed for the electrodes with and without thio-terpyridine functionalization. Ce oxide nanostructure recovery was successfully conducted by amperometry, and the electrodeposited nanostructured Ce materials were fully characterized by scanning electron microscopy, high-resolution transmission electron microscopy, X-ray diffraction crystallography, and X-ray photoelectron spectroscopy. Geometry optimization and the electronic energy state calculations were conducted by density functional theory at the B3LYP/GENECP level for the complexes of Ce(III) and Ce(IV) ions with the thio-terpyridine in an aqueous state. The present unique results provide valuable information on understanding redox behaviors of Ln and An ions for their recycling and treatment processes.

中文翻译：

电化学 Ce(III)/Ce(IV) 氧化还原行为和 Ce 氧化物纳米结构在硫代三联吡啶官能化 Au/碳纸电极上的恢复

了解 Ce(III)/Ce(IV) 离子的电化学行为对于更好地处理、分离和回收镧系 (Ln) 和锕系 (An) 元素至关重要。在此，在酸性和中性电解质中，通过新开发的硫代三联吡啶官能化 Au 改性碳纸电极证明了 Ce(III)/Ce(IV) 离子的电化学氧化还原行为和相互转化及其回收率。对具有和不具有硫代三联吡啶官能化的电极进行循环伏安法和电流分析法。通过电流分析法成功地进行了氧化铈纳米结构的恢复，并且通过扫描电子显微镜、高分辨率透射电子显微镜、X 射线衍射晶体学和 X 射线光电子能谱充分表征了电沉积纳米结构的 Ce 材料。几何优化和电子能态计算是通过密度泛函理论在 B3LYP/GENECP 水平上进行的，用于 Ce(III) 和 Ce(IV) 离子与硫代三联吡啶在水溶液中的复合物。目前的独特结果为了解 Ln 和 An 离子在其回收和处理过程中的氧化还原行为提供了有价值的信息。

更新日期：2021-06-16

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