| Summary: | Chemical vapor deposition is the most promising technique for the mass production of high-quality graphene, in which the metal substrate plays a crucial role in the catalytic decomposition of the carbon source, assisting the attachment of the active carbon species, and regulating the structure of the graphene film. Due to some drawbacks of single metal substrates, alloy substrates have gradually attracted attention owing to their complementarity in the catalytic growth of graphene. In this review, we focus on the rational design of binary alloys, such as Cu/Ni, Ni/Mo, and Cu/Si, to control the layer numbers and growth rate of graphene. By analyzing the elementary steps of graphene growth, general principles are summarized in terms of the catalytic activity, metal–carbon interactions, carbon solubility, and mutual miscibility. Several challenges in this field are also put forward to inspire the novel design of alloy catalysts and the synthesis of graphene films bearing desirable properties.
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