A process for forming a thermal barrier coating system on a substrate is disclosed including preparing a slurry including a donor powder, an activator powder, and a binder. The donor powder includes a metallic aluminum alloy having a melting temperature higher than aluminum, and the binder includes at least one organic polymer gel. The process further includes applying the slurry to the substrate, heating the slurry to form an aluminide bond coating including an additive aluminide layer and an aluminide interdiffusion zone disposed between the substrate and the additive aluminide layer, and applying a thermal barrier coating to the aluminide bond coating. The thermal barrier coating may be a dense vertically-cracked thermal barrier coating, and the substrate may be a gas turbine component. Thermal barrier coating systems formed by the process are also disclosed.

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