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利用基于激光的光谱技术对放射性废物进行精确的放射性碳测定。

Precise radiocarbon determination in radioactive waste by a laser-based spectroscopic technique.

机构信息

Consiglio Nazionale delle Ricerche, Istituto Nazionale di Ottica, 80078 Pozzuoli, Italy.

Consiglio Nazionale delle Ricerche, Istituto Nazionale di Ottica, 50019 Sesto Fiorentino, Italy.

出版信息

Proc Natl Acad Sci U S A. 2022 Jul 12;119(28):e2122122119. doi: 10.1073/pnas.2122122119. Epub 2022 Jul 7.

Abstract

The precise and accurate determination of the radionuclide inventory in radioactive waste streams, including those generated during nuclear decommissioning, is a key aspect in establishing the best-suited nuclear waste management and disposal options. Radiocarbon ([Formula: see text]) is playing a crucial role in this scenario because it is one of the so-called difficult to measure isotopes; currently, [Formula: see text] analysis requires complex systems, such as accelerator mass spectrometry (AMS) or liquid scintillation counting (LSC). AMS has an outstanding limit of detection, but only a few facilities are available worldwide; LSC, which can have similar performance, is more widespread, but sample preparation can be nontrivial. In this paper, we demonstrate that the laser-based saturated-absorption cavity ring-down (SCAR) spectroscopic technique has several distinct advantages and represents a mature and accurate alternative for [Formula: see text] content determination in nuclear waste. As a proof-of-principle experiment, we show consistent results of AMS and SCAR for samples of concrete and graphite originating from nuclear installations. In particular, we determined mole fractions of 1.312(9) F[Formula: see text] and 30.951(7) F[Formula: see text] corresponding to ∼1.5 and 36.2 parts per trillion (ppt), respectively, for two different graphite samples originating from different regions of the Adiabatic Resonance Crossing activator prototype installed on one irradiation line of an MC40 Scanditronix cyclotron. Moreover, we measure a mole fraction of 0.593(8) F[Formula: see text] ([Formula: see text] ppt) from a concrete sample originating from an external wall of the Ispra-1 nuclear research reactor currently in the decommissioning phase.

摘要

准确确定放射性废物流中的放射性核素库存,包括核退役期间产生的放射性核素库存,是确定最合适的核废物管理和处置方案的关键方面。放射性碳 ([Formula: see text]) 在这种情况下起着至关重要的作用,因为它是所谓的难以测量的同位素之一;目前,[Formula: see text] 分析需要复杂的系统,如加速器质谱 (AMS) 或液体闪烁计数 (LSC)。AMS 具有出色的检测限,但全球只有少数几个设施可用;LSC 可以具有类似的性能,应用更广泛,但样品制备可能并不简单。在本文中,我们证明基于激光的饱和吸收腔环形(SCAR)光谱技术具有几个明显的优势,并且代表了核废物中 [Formula: see text] 含量测定的成熟且准确的替代方法。作为原理验证实验,我们展示了来自核设施的混凝土和石墨样品的 AMS 和 SCAR 的一致结果。特别是,我们确定了来自安装在一个辐照线上的绝热共振交叉激活体原型的两个不同石墨样品的 1.312(9) F[Formula: see text] 和 30.951(7) F[Formula: see text] 的摩尔分数,分别对应于约 1.5 和 36.2 个部分每万亿(ppt),以及来自 Ispra-1 核研究反应堆退役阶段的外墙的混凝土样品的 0.593(8) F[Formula: see text] 的摩尔分数 ([Formula: see text] ppt)。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e1b1/9282372/9d1b0887fb42/pnas.2122122119fig01.jpg

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