Abstract Airborne contaminants from fires containing nuclear waste represent significant health hazards and shape the design and operation of nuclear facilities. Much of the data used to formulate DOE-HDBK-3010-94, “Airborne Release Fractions/Rates and Respirable Fractions for Nonreactor Nuclear Facilities,” from the U.S. Department of Energy, were taken over 40 years ago. The objectives of this study were to reproduce experiments from Pacific Northwest Laboratories conducted in June 1973 employing current aerosol measurement methods and instrumentation, develop an enhanced understanding of particulate formation and transport from fires containing nuclear waste, and provide modeling and experimental capabilities for updating current standards and practices in nuclear facilities. A special chamber was designed to conduct small fires containing 25 mL of flammable waste containing lutetium nitrate, ytterbium nitrate, or depleted uranium nitrate. Carbon soot aerosols showed aggregates of primary particles ranging from 20 to 60 nm in diameter. In scanning electron microscopy, ~200-nm spheroidal particles were also observed dispersed among the fractal aggregates. The 200-nm spherical particles were composed of metal phosphates. Airborne release fractions (ARFs) were characterized by leaching filter deposits and quantifying metal concentrations with mass spectrometry. The average mass-based ARF for 238U experiments was 1.0 × 10−3 with a standard deviation of 7.5 × 10−4. For the original experiments, DOE-HDBK-3010-94 states, “Uranium ARFs range from 2 × 10−4 to 3 × 10−3, an uncertainty of approximately an order of magnitude.” Thus, current measurements were consistent with DOE-HDBK-3010-94 values. ARF values for lutetium and ytterbium were approximately one to two orders of magnitude lower than 238U. Metal nitrate solubility may have varied with elemental composition and temperature, thereby affecting ARF values for uranium surrogates (Yb and Lu). In addition to ARF data, solution boiling temperatures and evaporation rates can also be deduced from experimental data.

中文翻译：

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含镧系元素硝酸盐和贫化硝酸铀的替代核废料火灾的空气中释放分数在 30% 的磷酸三丁酯煤油中

摘要 含有核废料的火灾产生的空气污染物代表着重大的健康危害，并影响着核设施的设计和运行。用于制定美国能源部的 DOE-HDBK-3010-94，“非反应堆核设施的空中释放分数/速率和可呼吸分数”的大部分数据是在 40 多年前获得的。本研究的目的是重现 1973 年 6 月太平洋西北实验室使用当前气溶胶测量方法和仪器进行的实验，加深对含有核废料的火灾的颗粒形成和传输的理解，并提供建模和实验能力以更新当前标准和核设施的实践。一个特殊的房间被设计用来进行包含 25 毫升含有硝酸镥、硝酸镱或贫化硝酸铀的易燃废物的小火。碳烟尘气溶胶显示出直径为 20 至 60 nm 的初级颗粒聚集体。在扫描电子显微镜中，还观察到约 200 nm 的球状颗粒分散在分形聚集体中。200 纳米球形颗粒由金属磷酸盐组成。空气中释放部分 (ARF) 的特征在于过滤器沉积物的浸出和质谱法量化金属浓度。238U 实验的平均基于质量的 ARF 为 1.0 × 10-3，标准偏差为 7.5 × 10-4。对于原始实验，DOE-HDBK-3010-94 指出，“铀 ARF 的范围从 2 × 10−4 到 3 × 10−3，不确定性大约是一个数量级。” 因此，电流测量值与 DOE-HDBK-3010-94 值一致。镥和镱的 ARF 值比 238U 低大约一到两个数量级。金属硝酸盐的溶解度可能随元素组成和温度而变化，从而影响铀替代物（Yb 和 Lu）的 ARF 值。除了 ARF 数据，溶液沸腾温度和蒸发率也可以从实验数据中推导出来。