The study investigates the direct oxidation of methane to methanol under mild conditions, a challenging process due to its low activity and selectivity. The researchers designed ultra-thin PdₓAu₁₋ₓ nanosheets and discovered a volcano-type relationship between the binding strength of hydroxyl radicals on the catalyst surface and catalytic performance. The optimized Pd₀.₅Au₁ nanosheets exhibited a methanol production rate of 147.8 millimoles per gram of Pd per hour with a selectivity of 98% at 70 °C, making it one of the most efficient catalysts for this reaction. The findings highlight the importance of regulating Au coverage to balance the reaction-triggering and reaction-conversion steps, and provide insights into the reaction mechanisms and optimal catalyst design for efficient methane-to-methanol conversion.The study investigates the direct oxidation of methane to methanol under mild conditions, a challenging process due to its low activity and selectivity. The researchers designed ultra-thin PdₓAu₁₋ₓ nanosheets and discovered a volcano-type relationship between the binding strength of hydroxyl radicals on the catalyst surface and catalytic performance. The optimized Pd₀.₅Au₁ nanosheets exhibited a methanol production rate of 147.8 millimoles per gram of Pd per hour with a selectivity of 98% at 70 °C, making it one of the most efficient catalysts for this reaction. The findings highlight the importance of regulating Au coverage to balance the reaction-triggering and reaction-conversion steps, and provide insights into the reaction mechanisms and optimal catalyst design for efficient methane-to-methanol conversion.