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Two-dimensional (2D) atomic layer materials have attracted a great deal of attention due to their superior chemical, physical, and electronic properties, and have demonstrated excellent performance in various applications such as energy storage devices, catalysts, sensors, and transistors. Nevertheless, the cost-effective and large-scale production of high-quality 2D materials is critical for practical applications and progressive development in the industry. Electrochemical exfoliation is a recently introduced technique for the facile, environmentally friendly, fast, large-scale production of 2D materials. In this review, we summarize recent advances in different types of electrochemical exfoliation methods for efficiently preparing 2D materials, along with the characteristics of each method, and then introduce their applications as electrode materials for energy storage devices. Finally, the remaining challenges and prospects for developing the electrochemical exfoliation process of 2D materials for energy storage devices are discussed. 

Metal-free carbon materials have emerged as cost-effective and high-performance catalysts for the production of hydrogen peroxide (H 2 O 2 ) through the two-electron oxygen reduction reaction (ORR). Here, we show that 3D crumpled graphene with controlled oxygen and defect configurations significantly improves the electrocatalytic production of H 2 O 2 . The crumpled graphene electrocatalyst with optimal defect structures and oxygen functional groups exhibits outstanding H 2 O 2 selectivity of 92–100% in a wide potential window of 0.05–0.7 V vs. reversible hydrogen electrode (RHE) and a high mass activity of 158 A g −1 at 0.65 V vs. RHE in alkaline media. In addition, the crumpled graphene catalyst showed an excellent H 2 O 2 production rate of 473.9 mmol gcat −1 h −1 and stability over 46 h at 0.4 V vs. RHE. Moreover, density functional theory calculations revealed the role of the functional groups and defect sites in the two-electron ORR pathway through the scaling relation between OOH and O adsorption strengths. These results establish a structure-mechanism-performance relationship of functionalized carbon catalysts for the effective production of H 2 O 2 .