Concrete is the primary building material for nuclear facilities, making it one of the most common forms of radioactive waste generated when decommissioning a nuclear facility. Of the total waste generated at the Connecticut Yankee and Maine Yankee nuclear power plants in the United States, concrete waste accounts for 83.5% of the total for Connecticut Yankee and 52% for Maine Yankee. In order to dispose of the low- to medium-level radioactive concrete waste generated during the decommissioning of nuclear power plants, it is necessary to analyze the radioactivity concentration of gamma nuclides such as Co-58, Co-60, Cs-137, and Ce-144. Gamma-ray spectroscopy is commonly used method to measure the radioactivity concentration of gamma nuclides in the radioactive waste; however, due to the nature of gamma detectors, gamma rays from sequentially decaying nuclides such as Co-60 or Y-88 are subject to True Coincidence Summing (TCS). TCS reduces the Full Energy Peak Efficiency (FEPE) of specific gamma ray and it can cause underestimation of radioactivity concentration. Therefor the TCS effect must be compensated for in order to accurately assess the radioactivity of the sample. In addition, samples with high density and large volume will experience a certain level of self-shielding effect of gamma rays, so this must also be compensated for. The Radioactive Waste Chemical Analysis Center at the Korea Atomic Energy Research Institute performs nuclide analysis for the final disposal of low- and intermediate-level concrete waste. Since a large number of samples must be analyzed within the facility, the analytical method must simultaneously satisfy accuracy and speed. In this study, we report on the results of evaluating the accuracy of the radioactivity concentration correction by applying an efficiency transfer method that appears to satisfy these requirements to concrete standard reference material.

Many radionuclides emit two or more gamma rays in a cascade once they decay. At this time, gamma rays are detected at the same time, and the signals are overlapped and measured as one added signal. This is called the summing coincidence effect, and it causes an error of more than 10% depending on the detection efficiency, measurement conditions, and target nuclide. It is known to be greater as the efficiency of the detector increases and as the distance between the source and the detector decreases. It is necessary to consider the summing coincidence effect since the efficiency of the HPGe detector owned by the KHNP CRI is as high as 65%. In this study, We would like to propose an appropriate gamma nuclide analysis method for radioactive waste generated from NPP by evaluating the influence on the summing coincidence effect.

According to the ‘Regulations on the Delivery of Low and Medium Level Radioactive Waste’, Notification No. 2021-26 of the Nuclear Safety and Security Commission, a history of radioactive waste and a total amount of radioactivity in a drum are mandatory. At this time, the inventory of radionuclides that make up more than 95% of the total radioactivity contained in the waste drum should be identified, including the radioactivity of H-3, C-14, Fe-55, Co-58, Co-60, Ni-59, Ni-63, Sr- 90, Nb-94, Tc-99, I-129, Cs-137, Ce-144, and total alpha. Among nuclides to be identified, gamma-emitting nuclides are usually analyzed with a gamma ray spectrometer such as HPGe. When a specific gamma-ray is measured with a detector, several types of peaks generated by recombination or scattering of electrons are simultaneously detected in addition to the corresponding gamma-ray in gamma-ray spectroscopy. Among them, the full energy peak efficiency (FEPE) with the total gamma energy is used for equipment calibration. However, this total energy peak efficiency may not be accurately measured due to the coincidence summing effect. There are two types of coincidence summing: Random and True. The random coincidence summing occurs when two or more gamma particles emitted from multiple nuclides are simultaneously absorbed within the dead time of the detector, and this effect becomes stronger as the counting rate increases. The true coincidence summing is caused by simultaneous absorption of gamma particles emitted by two or more consecutive energy levels transitioning from single nuclide within the dead time of the detector. This effect is independent of the counting rate but affected by the geometry and absolute efficiency of the detector. The FEPE decreases and the peak count of region where the energy of gamma particles is combined increases when the coincidence summing occurs. At the Radioactive Waste Chemical Analysis Center, KAERI, samples with a dead time of 5% or more are diluted and re-measured in order to reduce the random coincidence summing when evaluating the gamma nuclide inventory of radioactive waste. In addition, a certain distance is placed between the sample and the detector during measurement to reduce the true coincidence summing. In this study, we evaluate the coincidence summing effect in our apparatus for the measurement of radioactive waste samples.

동시 합성 보정 효과는 검출기의 효율이 향상할 때 그리고 선원과 검출기 사이의 거리가 가까울수록 크게 나타나는 것으로 알려져 있다. 점 선원(60Co)을 사용하여 검출기 중심축 방향 및 방사상 방향에서 거리에 따른 변화를 주어 P/T 비를 구하여 동시합성 보정을 하였다. 따라서 본 연구에서는 중심축 및 방사상 방향에서 동시합성 보정한 값들을 혼합부피선원(450 mL CRM source)에 적용하여 P/T에 따른 전체 피크효율 변화를 Geant4과 비교하였다. 또한 검출기와 시료가 아주 밀착된 상태에서 맵핑법에서 구한 효율을 환경시료 중에서 해양 시료인 미역에 적용하여 P/T 비의 적합성을 평가하고자 한다. 500 keV 이상의 효율의 영향을 받는 에너지 영역에 1,836 keV로 보정한 효율을 적용한 결과 측정값과 보정값의 상대오차는 3.2 % peak 효율이 보정되어 잘 일치하였다. 450 mL CRM source처럼 부피가 커질수록 P/T 비는 ± 5%까지 감소하였다. 이것은 검출기로부터 선원이 멀어짐에 따라 방출된 감마선의 산란이 많아지기 때문이며, 이처럼 P/T 변화는 동시합성 보정 피크 효율에 영향을 줌을 확인하였다.