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DOI: 10.1002/adma. 201602028 inherent challenges described above. Here, we experimentally show that engineered defects in graphene can alleviate these bottlenecks resulting in a new paradigm of energy storage beyond the predicted theoretical limits. Defects are often perceived as performance limiters in graphene. Yet, our experimental findings conclusively demonstrate that controllably induced defects in specific configurations can achieve 150% enhancement (≈ 50 µF cm− 2) in measurable capacitance of fewlayer graphene (FLG). Our detailed density function (DFT) theory calculations show that the nitrogen dopants in the pyrrolic configuration result in a high DOS (EF) and thereby mitigate the influence of CQ. Furthermore, the interlayer spaces in FLG can be accessed by tetraethylammonium (TEA+) ions effectively through defect-induced pores leading to increased charge storage. More importantly, we show that these high capacitances can be extended to coin-cell devices based on FLG foams that result in energy densities at least five times higher than the conventional activated carbon SCs. Previously, it was observed that the best performance of SCs can be realized when the average micropore size in nanostructured bulk electrodes (eg, carbide-derived carbon) matches the size of the ions in the electrolyte.[8–16] It is expected that such a resonant effect is true even for defect-induced pores in quasi-2D FLG substrates (Figure 1a). Accordingly, in order to identify the best-suited electrolyte, we theoretically studied the interactions of two different ions–TEA+ and tetrabutylammonium (TBA+) with defect-induced pores in FLG. The …