Intensive study on structure transformation of muscovite single crystal under highdose γ-ray irradiation and mechanism speculation

Abstract

Intensive study on structure transformation of muscovite single crystal under high-dose g-ray irradiation is essential for its use in irradiation detection and also beneficial for mechanism cognition on defect formation within a matrix of clay used in the disposal of high-level radioactive waste (HLRW). In this work, muscovite single crystal was irradiated with Co-60 g ray in air at a dose rate of 54 Gy min-1 with doses of 0-1000 kGy. Then, structure transformation and mechanism were explored by Raman spectrum, Fourier-transform infrared spectrum, X-ray diffraction, thermogravimetric analysis, CA, scanning electron microscope and atomic force microscopy. The main results show that variations in the chemical/crystalline structure are dose-dependent. Low-dose irradiation sufficiently destroyed the structure, removing Si-OH, thus declining hydrophilicity. With dose increase up to 100 kGy, CA increased from 208 to 408. Except for hydrophilicity variation, shrink occurred in the (004) lattice plane which later recovered; the variation range at 500 kGy irradiation was 0.5% close to 0.02 Å . The main mechanisms involved were framework break and H2O radiolysis. Framework break results in Si-OH removal and H2O radiolysis results in extra OH introduction. The extra introduced OH probably results in Si-OH bond regeneration, lattice plane shrink and recovered surface hydrophilicity. The importance of framework break and H2O radiolysis on structure transformation is dose-dependence. At low doses, framework break seems more important while at high doses H2O radiolysis is important. Generally, variations in the chemical structure and surface property are nonlinear and less at high doses. This indicates using the chemical structure or surface property variation to describe irradiation is correct at low doses but not at high doses. This finding is meaningful for realizing whether muscovite is suitable for detecting high-dose irradiation or not, and mechanism exploration is efficient for identifying the procedure for defect formation within the matrix of clay used in disposal HLRW in practice.