| Citation: |
CHEN Zuoyang, HUO Zhipeng, ZHANG Hong, et al. Micron Spindle-shaped PbWO4-B4C/HDPE Composites and their Neutron and Gamma-ray Radiation Shielding Properties[J]. Acta Materiae Compositae Sinica.
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Three micron spindle-shaped PbWO4 with different microstructures are synthesized by varying the concentration of the surfactant CTAB (cetyltrimethylammonium bromide) and the reaction time. The synthesized and commercial PbWO4 are used as fillers, and mixed with B4C and HDPE (high-density polyethene) to prepare composites for neutron and gamma-ray radiation shielding. X-ray diffraction (XRD) analysis reveals that the growth priority of the four main crystal planes of PbWO4 is: (200) > (312) > (112) > (204). Field emission scanning electron microscope (FESEM) and specific surface area analyses reveal that PbWO4 undergoes Ostwald ripening and oriented attachment mechanisms to form morphologically regular micron spindle-shaped microstructures, and their specific surface areas (SBET) are 0.64 m2/g, 1.02 m2/g, and 1.76 m2/g, respectively. The commercial PbWO4 is an irregular structure and large-sized bulk with a much lower SBET of 0.21 m2/g. The thermostability and mechanical properties such as melt temperature (Tp) and yield stress (σy) of micron spindle-shaped PbWO4-B4C/HDPE composites are better than those of commercial PbWO4-B4C/HDPE. Pb has good ductility and can improve the tensile stress and toughness of the material. The neutron and gamma-ray radiation shielding tests show that the micron spindle-shaped PbWO4-based composites with high specific surface areas have much better shielding performances than the commercial PbWO4. The composite with the best radiation performance has a total neutron cross-section (Σ) of 0.22 cm−1 for 252Cf neutron source and a linear attenuation coefficient (μ) of 0.099 cm−1 for 137Cs gamma-ray source.
PURPOSE: High-energy neutrons and gamma-ray generated by nuclear technology applications have high penetrability and can damage human health. High doses of radiation exposure can lead to genetic mutations, cancer and even death. Therefore, research on efficient radiation shielding materials is necessary.METHODS: Polyethylene is rich in H elements that can slow down fast neutrons and convert them into thermal neutrons. BC has a high thermal neutron absorption cross-section. PbWO has a high effective atomic number (), which can enhance the shielding performance of the composite material for gamma-ray. In this study, the crystal growth of PbWO was controlled by varying the concentration of cetyltrimethylammonium bromide (CTAB) and the reaction time. And the synthesized micron spindle-shaped PbWO and commercial PbWO with irregular morphology were used as fillers and ball-milled and mixed with BC and polyethylene powders then hot-pressed to make composites for neutrons and gamma-ray shielding. The effect of the microstructure of PbWO fillers on the thermal, mechanical and radiation shielding properties of the composites was studied and elucidated in tetail.RESULTS: The XRD spectra of the PbWO fillers are in good agreement with the standard diffraction peaks (JCPDS: 19-0708), and there is no impurity phase. The crystal growth preference of synthesized PbWO is (200) > (312) > (112) > (204). The surfactant (CTAB) can promote crystal growth and the concentration of CTAB was controlled to obtain three kinds of PbWO fillers with different specific surface areas. Scanning Electron Microscope (SEM) images show that the crystal growth of PbWO conforms to the Ostwald ripening process. The morphology of the synthesized PbWO-I fillers is partly composed of nanoparticles that have not yet completed the ripening process, as well as pyramidal and micron spindle-shaped particles that have completed the ripening process. Most of these PbWO-I particles are in the size of 1-2 μm. Afterwards, the pyramidal particles are oriented along the same crystallographic planes and gradually grow to form micron spindle-shaped structures. This process is called the ‘oriented attachment’ mechanism. The microscopic size of the PbWO-II filler is 3-5 μm, while the PbWO-III filler is a larger micron spindle-shaped structure with a size of 5-9 μm. The commercial PbWO is a lumpy structure with large differences in microscopic size without a specific morphology. The specific surface area of the synthesized PbWO is higher than that of the commercial PbWO.The pore size distribution graph shows that synthesized PbWO has more mesopores than the commercial PbWO. Tiny slits are formed during the oriented attaching process of pyramidal particles, and the larger the size the more slits formed. Therefore, PbWO-III has the highest specific surface area of 1.76 m/g. The results of thermogravimetric (TG) and differential scanning calorimetry (DSC) tests show that the initial decomposition temperature () and semi-decomposition temperature () of micron spindle-shaped PbWO composites were higher than that of commercial PbWO composite. As the specific surface area of the filler increases, the peak temperature () of the DSC curve of the material increases. Mechanical test results show that the yield stress of the composites increased from 16.67 MPa of commercial PbWO to 19.78 MPa of the micron spindle-shaped PbWO-III. The tensile strength () was also increased from 19.40 MPa to 20.09 MPa. Shielding performance tests show that the PbWO-III composite has the lowest neutron and gamma-ray transmission rates. The thickness () required to reach a 95% shielding rate for the Cf neutron source is 13.0 cm, and the total neutron cross-section () is 0.22 cm. The thickness () required to reach a 65% shielding rate for Cs gamma-ray source is 11.0 cm, and the linear attenuation coefficient () and mass attenuation coefficient () are larger than those of the other materials. The material has smaller half-value layer (HVL) and mean free range (MFP) than those of the other materials. The PbWO-III composite has the highest probability of interaction with gamma photons and neutrons and has the best radiation shielding performance.CONCLUSIONS: (1) The synthesized micron spindle-shaped PbWO fillers have higher specific surface area than commercial PbWO, and can provide more restriction sites in the HDPE matrix. The thermal vibration of the HDPE molecular chains are hindered to a greater extent, thus the thermal stability of the composites containing synthesized PbWO fillers are improved.(2) The synthesized micron spindle-shaped PbWO fillers with higher specific surface area can provide more restriction sites in the HDPE matrix, which can limit the relative displacement of the molecular chains of the HDPE matrix under the state of external force. So the tensile strength of the synthesized composites are higher than that of the commercial one. Moreover, since Pb has good ductility, it can improve the elongation at break and toughness of the composites.(3) The synthesized micron spindle-shaped PbWO fillers with high specific surface area can effectively increase the probability of interaction between the composites and the radiation particles, and enhance the radiation shielding performance of the composites.
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