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Higher-metal (HM) nitrides are a fascinating family of materials being increasingly researched due to their unique physical and chemical properties. However, few focus on investigating their application in a solar steam generation because the controllable and large-scale synthesis of these materials remains a significant challenge. Herein, it is reported that higher-metal molybdenum nitride nanosheets (HM-Mo5 N6 ) can be produced at the gram-scale using amine-functionalized MoS2 as precursor. The first-principles calculation confirms am