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The Role of Dissolved Hydrogen on the Corrosion/Dissolution of Spent Nuclear Fuel

机译：溶解氢在乏核燃料腐蚀/溶解中的作用

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摘要

The literature on nuclear fuel dissolution and radionuclide release studies in aqueous solutions containing dissolved hydrogen has been reviewed. These studies include investigations with spent PWR and MOX fuels, fuel specimens doped with alpha emitters to mimic "aged" fuels, SIMFUELs fabricated to simulate spent fuel properties, and unirradiated uranium dioxide pellets and powders. In all these studies, dissolved hydrogen was shown to suppress fuel corrosion and in spent fuel studies to suppress radionuclide release. A number of mechanisms have been either demonstrated or proposed to explain these effects, all of which involve the activation of hydrogen to produce the strongly reducing H" radical, which scavenges radiolytic oxidants and suppresses fuel oxidation and dissolution (i.e., corrosion). Both gamma and alpha radiation have been shown to produce H" surface species. With gamma radiation this could involve the absorption of gamma energy by the solid leading to water decomposition to OH" and H" radicals, with the OH" radical subsequently reacting with hydrogen to yield an additional H". This latter radical then suppresses fuel oxidation and scavenges radiolytic oxidants. With alpha radiation, the need to neutralize oxygen vacancies generated by recoil events can initiate the same process by decomposing water. In the absence of radiation fields activation can occur on the surface of noble metal (epsilon) particles. Since these particles are galvanically-coupled to the fuel matrix they act as anodes for hydrogen oxidation (which proceeds through surface H" species) and forces the UO_2 to adopt a low potential. Also, there is some evidence to suggest that H_2 can be activated on the UO_2 surface in the presence of hydrogen peroxide, but the process appears to be inefficient. Depending on the radiation fields present and the number density of epsilon particles, complete suppression of fuel corrosion appears possible even for hydrogen pressures as low as 0.1 to 1 bar. Since the corrosion of steel liners within failed waste containers could produce hydrogen pressures up to 50 bar, fuel corrosion could be completely suppressed under the long-term conditions expected in sealed repositories.
机译：关于含溶解氢的水溶液中核燃料溶解和放射性核素释放研究的文献已有综述。这些研究包括以下方面的研究：乏压水堆和MOX燃料，掺杂有α发射体以模仿“老化”燃料的燃料样本，为模拟乏燃料特性而制造的SIMFUEL，以及未经辐照的二氧化铀颗粒和粉末。在所有这些研究中，溶解氢均能抑制燃料腐蚀，而在乏燃料研究中则能抑制放射性核素的释放。已经证明或提出了许多机制来解释这些作用，所有这些机制都涉及激活氢以产生强烈还原的H“自由基，该自由基清除放射性氧化剂并抑制燃料的氧化和溶解（即腐蚀）。已经证明α和α辐射会产生H”表面物质。对于伽马辐射，这可能涉及固体吸收伽马能量，导致水分解为OH“和H”自由基，而OH“自由基随后与氢反应生成另外的H”。然后，该后者自由基抑制燃料氧化并清除辐射性氧化剂。对于α辐射，中和因反冲事件而产生的氧气空位的需求可以通过分解水来启动相同的过程。在没有辐射场的情况下，活化可发生在贵金属（ε）颗粒的表面上。由于这些粒子通过电流耦合到燃料基体，因此它们充当氢氧化的阳极（氢氧化通过表面H”物质进行），迫使UO_2处于低电位。此外，有证据表明H_2可以被激活在存在过氧化氢的情况下在UO_2表面上进行，但该过程似乎效率不高，根据存在的辐射场和ε粒子的数量密度，即使氢气压力低至0.1至1，也可能完全抑制燃料腐蚀由于失效的废物容器中钢衬板的腐蚀会产生高达50 bar的氢气压力，因此在密封储存库中预期的长期条件下，燃料腐蚀将得到完全抑制。

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  • 来源
    《Nuclear energy and the environment》|2009年|p.349-380|共32页
  • 会议地点 Washington DC(US);Washington DC(US)
  • 作者

    M. E. Broczkowski; D. Zagidulin; D. W. Shoesmith;

  • 作者单位

    The University of Western Ontario, London Ontario, Canada N6A 5B7;

    The University of Western Ontario, London Ontario, Canada N6A 5B7;

    The University of Western Ontario, London Ontario, Canada N6A 5B7;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 核能工业;
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