Preparation of Li2O–Al2O3–SiO2–B2O3（LASB）glass-ceramic with low thermal expansion coefficient from spent hydrogenation catalysts and crystallization kinetics

Abstract

The recovery of spent hydrogenation catalysts occupies advantages in both alleviating environmental burden and resource shortage. Whereas, the development of conventional hydrometallurgical recovery of molybdenum (Mo) and nickel (Ni) from spent MoNi/Al2O3 catalysts has been limited by the numerous processes and the accompanying generation of waste liquids and residues. Herein, A new recycling route for the preparation of spent hydrogenation catalysts with low thermal expansion coefficients (CTE) was proposed, which has the advantages of short process, green environment and high value utilization. The Li2O–Al2O3–SiO2–B2O3 (LASB) parent glass containing Mo and Ni were obtained by melting with different contents of the spent catalysts. The thermal expansion coefficient of the glass was minimized to 6.08 × 10−6/°C at an addition of 25 wt% of the spent catalysts. Moreover, according to the crystallization peak in DTA curve, glass-ceramics were prepared by one-step crystallization heat treatment at different crystallization temperatures. The main crystalline phase of the glass-ceramic precipitated by heating at 685 °C is β-quartz (Li2Al2Si3O10), which gives the glass-ceramics the lowest coefficient of thermal expansion (0.96 × 10−6/°C) of glass-ceramic as well as the maximum density (2.45 g/cm3) and Vickers hardness (705.8 Hv). Furthermore, the activation energy (354.65 ± 17.42) kJ/mol) and Avrami index (5.39) associated with crystallization were extracted from the fitting of different theoretical model, indicating the three-dimensional crystallization of the LASB glass-ceramics. This technology provides a waste-to-material strategy for hazardous waste and a clean production route for the preparation of the functional glass-ceramics.