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Two-dimensional (2D) nanomaterials have attracted tremendous attention from researchers working in the field of heterogeneous catalysis. Owing to the unique advantages offered by 2D nanomaterials, such as high surface area, abundant reaction sites, improved electrical and optical properties, excellent support materials, etc., they have been widely utilized in synthesizing several hybrid materials and in different catalytic applications. This chapter focuses, in particular, on the application of 2D nanomaterial-based catalysts in sustainable ammonia (NH3) synthesis. In recent years, research has delved into establishing new technologies for green and sustainable NH3 synthesis as a replacement for the conventional Haber–Bosch process. In this chapter, three such approaches, namely, photocatalysis, electrocatalysis, and photoelectrocatalysis, are discussed in detail. Some recent examples of 2D nanomaterial-based composites, doped systems, and defect-engineered and hybrid materials are presented to provide a glimpse of these three processes. Finally, a summary of progress in this field and an outline of future directions for sustainable NH3 production are discussed.

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