In order to promote the development of coal gangue aggregate concrete and the resource utilization of coal gangue solid waste, the coal gangue samples were crushed into aggregates, and then the macroscopic characteristics and microscopic structures of the aggregates were characterized through methods such as calcination, sulfuric acid solution dry-wet cycle, XRD, TG-DTG, and SEM-EDS, based on the Chinese national aggregate standard, the key influencing factors of the physicochemical properties of coal gangue aggregates were analyzed. The results show that coal gangue with lower loss on ignition and carbon content has smaller crushing value, lower water absorption rate, and stronger soundness. The carbon content and carbon distribution significantly affect the macroscopic physicochemical properties of coal gangue aggregates. Carbon, as a defect, is uniformly distributed in coal gangue, which increases the crushing value of coal gangue aggregates and greatly reduces their soundness, leading to the “second-order adverse effect” and “opening window effect”, which are detrimental to the durability of coal gangue aggregate concrete. The composition and physicochemical properties of a large number of coal gangue samples were determined, and the correlation between composition overlay effects on physicochemical properties were analyzed using a “three-dimensional surface”. This analysis confirms the adverse effects of carbon defects on the physicochemical properties of coal gangue aggregates. Carbon content can be used as the primary control index for coal gangue in resource utilization.
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