Mesophase Pitch-Derived Carbons with High Electronic and Ionic Conductivity Levels for Electric Double-Layer...

We develop a temperature-programmed pretreatment strategy for converting aliphatic-rich petroleum pitch into a mesophase framework, which can then be activated using KOH to produce high-performance carbons for electric double-layer capacitors (EDLCs). In the pretreatment of pitch at an optimal temperature, both the temperature ramp and holding time influence the mesophase structure, which governs the pore structure and crystallinity of the resulting activated carbon. High carbon microporosity is beneficial to capacitance maximization but detrimental to ion transport. To resolve this problem, we develop a multistep ramp incorporating aliphatic species into the aromatic framework during mesophase formation. This incorporation process produces a mesophase framework that can be activated to form carbons with high crystallinity, thereby enhancing electronic conductivity and hierarchical porosity, which improves ionic conductivity. The resulting carbon electrode is used to assemble a symmetric EDLC, which exhibits a capacitance of 160 F g^-1 and excellent high-rate retention in a propylene carbonate solution of N,N-diethyl-N-methylethanaminium tetrafluoroborate. The EDLC delivers a superior specific energy of 40 Wh kg^-1 (based on the total carbon mass) within a voltage range of 0-2.7 V and sustained a high energy of 24 Wh kg^-1 at a high power of 50 kW kg^-1. The findings of this study demonstrate that incorporating aliphatic species into aromatic mesophase frameworks plays a crucial role in regulating the crystallinity and pore structure of pitch-derived carbons for charge storage.