This Critical Review reviews the origin and chemical and rheological complexity of radioactive waste at the U.S. Department of Energy Hanford Site. The waste, stored in underground tanks, was generated via three distinct processes over decades of plutonium extraction operations. Although close records were kept of original waste disposition, tank-to-tank transfers and conditions that impede equilibrium complicate our understanding of the chemistry, phase composition, and rheology of the waste. Tank waste slurries comprise particles and aggregates from nano to micro scales, with varying densities, morphologies, heterogeneous compositions, and complicated responses to flow regimes and process conditions. Further, remnant or changing radiation fields may affect the stability and rheology of the waste. These conditions pose challenges for transport through conduits or pipes to treatment plants for vitrification. Additionally, recalcitrant boehmite degrades glass quality and the high aluminum content must be reduced prior to vitrification for the manufacture of waste glass of acceptable durability. However, caustic leaching indicates that boehmite dissolves much more slowly than predicted given surface normalized rates. Existing empirical models based on ex situ experiments and observations generally only describe material balances and have not effectively predicted process performance. Recent advances in the areas of in situ microscopy, aberration-corrected transmission electron microscopy, theoretical modeling across scales, and experimental methods for probing the physics and chemistry at mineral–fluid and mineral–mineral interfaces are being implemented to build robustly predictive physics-based models.

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回顾美国能源部汉福德场对放射性废物的科学认识

这篇批判性评论回顾了美国能源部汉福德场址放射性废物的起源、化学和流变复杂性。这些废物储存在地下储罐中，是在几十年的钚提取作业中通过三个不同的过程产生的。尽管保存了原始废物处置的密切记录，但罐间转移和阻碍平衡的条件使我们对废物的化学、相组成和流变学的理解复杂化。罐式废物浆料包括从纳米到微米尺度的颗粒和聚集体，具有不同的密度、形态、异质成分以及对流动状态和工艺条件的复杂响应。此外，残留或变化的辐射场可能会影响废物的稳定性和流变性。这些条件对通过导管或管道运输到处理厂进行玻璃化处理提出了挑战。此外，顽固的勃姆石会降低玻璃质量，并且必须在玻璃化之前降低高铝含量，以生产具有可接受耐久性的废玻璃。然而，苛性浸出表明勃姆石的溶解速度比给定的表面归一化速率预测的要慢得多。基于异地实验和观察的现有经验模型通常只描述物质平衡，并没有有效地预测过程性能。原位显微镜、像差校正透射电子显微镜、跨尺度理论建模、