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Abstract: Metal organic frameworks (MOFs) are considered as promising candidates for supercapacitors because of high specific area and potential redox sites. However, their shuffled orientations and low conductivity nature lead to severely‐degraded performance. Designing an accessibly‐manipulated and efficient method to address those issues is of outmost significance for MOF application in supercapacitors. It is the common way that MOFs scarify themselves as templates or precursors to prepare target products. But to reversely think it, using target products to prepare MOF could be the way to unlock the bottleneck of MOFs' performance in supercapacitors. Herein, a novel strategy using Co(OH)2 as both the template and precursor to fabricate vertically‐oriented MOF electrode is proposed. The electrode shows a double high specific capacitance of 1044 Fg−1 and excellent rate capability compared to MOF in powder form. An asymmetric supercapacitor was also fabricated, which delivers a maximum energy density of 28.5 W h kg−1 at a power density of 1500 W kg−1, and the maximum of 24000 W kg−1 can be obtained with a remaining energy density of 13.3 W h kg−1. Therefore, the proposed strategy paves the way to unlock the inherent advantages of MOFs and also inspires for advanced MOF synthesis with optimum performance. [ABSTRACT FROM AUTHOR]

Anion intercalation in graphite is deemed as a promising electrode chemistry in aqueous energy storage systems due to its high onset potential. Given the limited space in graphite, multivalent anions are favorable to achieve high specific capacity. However, relevant studies are scarce so that fundamental understandings of multivalent anion intercalation remain unclear. Herein, the intercalation behaviors of ClO4−, SO42−, and PO43− in graphite are systematically investigated. High capacity and interaction between anion and graphite are proved to be contradictory as the electric charge increases. As a result, ClO4− and SO42− intercalation exhibits promising performance in primitive graphite, while PO43− intercalation is much restricted due to the intensified electronic interaction. Two Zn–graphite dual‐ion batteries based on ClO4− and SO42− intercalations display high voltages of 1.85 V, and specific energies of 106 and 112 Wh kg−1. This work provides fundamental understandings of multivalent anion intercalation and guidance to fabricate aqueous batteries (ABs) with high energy density. [ABSTRACT FROM AUTHOR]