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Cr涂層鋯合金包殼高溫蒸汽氧化動(dòng)力學(xué)及微觀機(jī)理研究
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中廣核研究院有限公司

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High-temperature steam oxidation kinetics and mechanisms of Cr-coated Zr alloy claddings
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    摘要:

    Cr涂層鋯合金包殼具備抗高溫蒸汽氧化性能優(yōu)異、耐腐蝕和耐磨蝕性能良好、工程應(yīng)用難度較小等特點(diǎn),成為最具前景的近期型事故容錯(cuò)燃料候選材料之一。本文以Zr-1Nb合金管為基體材料,采用磁控濺射工藝制備均勻致密Cr涂層,涂層厚度范圍12~15 μm。通過(guò)同步綜合熱分析儀開(kāi)展雙面高溫蒸汽氧化試驗(yàn),氧化溫度為1000°C、1100°C和1200°C,氧化時(shí)間為300~5000 s不等,系統(tǒng)研究反應(yīng)堆事故工況下Cr涂層鋯合金包殼高溫蒸汽氧化行為。采用掃描電子顯微鏡、能譜儀和X射線衍射儀表征高溫氧化產(chǎn)物膜微觀形貌特征、氧化層厚度、元素分布以及物相組成等,建立Cr涂層氧化動(dòng)力學(xué)模型,探討高溫氧化機(jī)理。研究表明,高溫蒸汽環(huán)境中,Cr涂層鋯合金包殼外壁形成致密Cr2O3層,有效阻止O元素?cái)U(kuò)散至Zr合金基體,從而提升復(fù)合包殼的耐高溫性能。其次,Cr涂層高溫蒸汽氧化動(dòng)力學(xué)曲線遵循拋物線規(guī)律,氧化速率常數(shù)比鋯合金低大約2個(gè)數(shù)量級(jí),顯著提升鋯合金包殼抗高溫蒸汽氧化性能。

    Abstract:

    The Cr-coated Zr alloy materials appear to be one promising short-term accident tolerant fuel cladding concept, due to their outstanding high-temperature oxidation resistance and improved resistance to fretting wear. In addition, there are few barriers or challenges to be applied to nuclear reactors for coated Zr alloy claddings. In this paper, 12-15 μm-thickness coatings have been deposited by magnetron-sputtering process on the outer surface of Zr-1Nb alloy tubes. Two-sided isothermal oxidation tests were performed in flowing steam by synchronous thermogravimetric analyzer, at temperatures ranging from 1000°C to 1200°C and for oxidation times ranging from 300 s to 5000 s, with the object of systematically studying the behavior during accidents. Scanning electron microscopy equipped with energy dispersive X-ray spectroscopy and X-ray diffraction were utilized to characterize the microstructure, element distributions and phase of oxide scale to study the oxidation kinetics and mechanisms of Cr coating. Based on these analyses, dense chromia scale was developed on the outer surface of cladding during steam oxidation, preventing the oxygen atoms from diffusing into the substrate, to improve the high-temperature resistance of the composited claddings. In addition, the oxidation kinetics of the Cr coating was nearly parabolic and the rate constants was at least two orders of magnitude lower than the Zr alloy, enhancing high-temperature steam oxidation resistance of Zr alloy claddings.

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廖業(yè)宏,彭振馴,嚴(yán)俊,王占偉,李思功,任啟森. Cr涂層鋯合金包殼高溫蒸汽氧化動(dòng)力學(xué)及微觀機(jī)理研究[J].稀有金屬材料與工程,2023,52(1):291~299.[Liao Yehong, Peng Zhenxun, Yan Jun, Wang Zhanwei, Li Sigong, Ren Qisen. High-temperature steam oxidation kinetics and mechanisms of Cr-coated Zr alloy claddings[J]. Rare Metal Materials and Engineering,2023,52(1):291~299.]
DOI:10.12442/j. issn.1002-185X.20220364

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  • 收稿日期:2022-04-27
  • 最后修改日期:2022-09-11
  • 錄用日期:2022-09-22
  • 在線發(fā)布日期: 2023-02-13
  • 出版日期: 2023-02-08