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作为镅 - 241 驱动的放射性同位素动力系统替代物的氧化钕微球的无尘溶胶 - 凝胶合成

Dust-Free Sol-Gel Synthesis of Neodymium Oxide Microspheres as a Surrogate for Americium-241 Fueled Radioisotope Power Systems.

作者信息

Granger-Jones Jessica A, Finkeldei Sarah C

机构信息

Department of Chemistry, University of California, Irvine, Irvine, California 92697, United States.

Department of Materials Science and Engineering, University of California, Irvine, Irvine, California 92697, United States.

出版信息

ACS Omega. 2025 May 16;10(21):21767-21776. doi: 10.1021/acsomega.5c01418. eCollection 2025 Jun 3.

DOI:10.1021/acsomega.5c01418
PMID:40488089
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12138607/
Abstract

New designs for radioisotope power systems (RPS) explore the use of Am-241 as a fuel source. Neodymium is a common surrogate for americium and the work here presents a citrate-modified internal gelation route was applied to synthesize neodymium oxide microspheres, as a surrogate for americium oxide microspheres with applications in these new RPS designs. Neodymium has not previously been gelled on its own using the internal gelation route as the pH of neodymium hydrolysis and precipitation is higher than that achieved in the internal gelation process. However, the inclusion of citric acid as a precursor allows for the neodymium to deprotonate and coordinate to the citrate groups rather than hydrolyze, which results in the precipitation of a 1:1 neodymium citrate gel. Subsequent heat treatment to 950 °C under adequate air flow decomposes the residual organics and citrate groups resulting in the formation of the high temperature trigonal phase of NdO. The work here details the chemistry involved in the citrate-modified internal gelation process as well as outlines methods for the optimization of microsphere fabrication. The sol-gel microspheres fabricated through this adapted synthesis method can be pelletized for use in RPS systems without the need for dust-producing steps, such as milling, thus providing the platform for the safer fabrication of RPS.

摘要

放射性同位素动力系统(RPS)的新设计探索了使用镅 - 241作为燃料源。钕是镅的常见替代物,本文介绍了一种柠檬酸盐改性的内凝胶法,用于合成氧化钕微球,作为氧化镅微球的替代物,应用于这些新型RPS设计中。钕以前未通过内凝胶法单独凝胶化,因为钕水解和沉淀的pH值高于内凝胶过程中所能达到的pH值。然而,加入柠檬酸作为前驱体可使钕去质子化并与柠檬酸根配位而不是水解,从而导致1:1的柠檬酸钕凝胶沉淀。随后在充足的气流下于950℃进行热处理,分解残留的有机物和柠檬酸根,形成高温三角相的NdO。本文详细介绍了柠檬酸盐改性内凝胶过程中涉及的化学原理,并概述了优化微球制备的方法。通过这种改进的合成方法制备的溶胶 - 凝胶微球可以造粒用于RPS系统,而无需诸如研磨等产生粉尘的步骤,从而为更安全地制造RPS提供了平台。

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本文引用的文献

1
First-Principle Studies of the Vibrational Properties of Carbonates under Pressure.压力下碳酸盐振动性质的第一性原理研究
Sensors (Basel). 2021 May 24;21(11):3644. doi: 10.3390/s21113644.
2
Aqueous complexation of citrate with neodymium(III) and americium(III): a study by potentiometry, absorption spectrophotometry, microcalorimetry, and XAFS.柠檬酸盐与钕(III)和镅(III)的水相络合:电位滴定法、吸收分光光度法、微量量热法和X射线吸收精细结构光谱法研究
Dalton Trans. 2014 May 7;43(17):6446-54. doi: 10.1039/c4dt00343h.
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Curium(III) citrate speciation in biological systems: a europium(III) assisted spectroscopic and quantum chemical study.
镥(III)柠檬酸盐在生物体系中的形态:铕(III)辅助的光谱和量子化学研究。
Dalton Trans. 2012 Dec 7;41(45):13969-83. doi: 10.1039/c2dt31480k. Epub 2012 Oct 1.