Heteroatom-Doped Pillared Porous Carbon Architectures with Ultrafast Electron and Ion Transport Capabilities under High Mass Loadings for High-Rate Supercapacitors

Abstract

Retaining fast electron and ion transport of electrode materials at high mass loadings holds significant importance to supercapacitors. Carbon-based materials with ultrathin electrodes or small amounts of active materials on the current collectors, that is, active materials with a low mass loading (<1 mg cm–2), have achieved high capacitances and power densities with a fast charging/discharging rate. Yet, the low mass loading leads to low capacitances based on area or the device and, consequently, poor energy. Simultaneously, it cannot be readily scaled to commercial electrodes that have practical levels of mass loading above 10 mg cm–2. Here, we demonstrate N, O, and S self-doped pillared porous carbon architectures (AMJ-3) through the integration of the heteroatom-doping method and architectonic design, which exhibit excellent frequency response with a scan rate up to 7 V s–1 at 1.6 mg cm–2 and 500 mV s–1 at 12 mg cm–2. Furthermore, an ultrafast AMJ-3//AMJ-3 symmetric supercapacitor can be charged/discharged within 0.49 s to deliver both high specific energy of 11 Wh kg–1 and ultrahigh power of 107 kW kg–1 in 1 M Na2SO4. Most importantly, AMJ-3//AMJ-3 symmetric supercapacitor can simultaneously achieve excellent energy density normalized to area (0.21 mWh cm–2) at a high mass loading of 24 mg cm–2.

Inhibiting Solvent Co‐Intercalation in a Graphite Anode by a Localized High‐Concentration Electrolyte in Fast‐Charging Batteries

“…In the C 1s spectra of all electrolytes studied, the relative contents of compounds containing C−O bonds (284.5 eV) is low (Figure 3 a). [18] The graphite surface contains less organic components. It indicates that the decomposition of DME has not yet proceeded.…”

Approaching the Theoretical Sodium Storage Capacity and Ultrahigh Rate of Layer‐Expanded MoS2 by Interfacial Engineering on N‐Doped Graphene

“…The Nyquist plots consist of a semicircle at the high‐medium frequency region and a sloping tail at the low frequency region (Figure S19a, Supporting Information), which are assigned to the charge‐transfer resistance ( R ct ) and Warburg impedance ( Z w ), respectively. [ 35 ] The kinetic parameters are well‐fitted according to the equivalent circuit (Figure S19b, Supporting Information). As shown in Figure 4e, MoS 2 /NG exhibits a R ct value of 91 Ω, two times lower than MoS 2 /G (187 Ω) due to the robust charge‐transfer kinetics enabled by the strong interfacial interaction (MoN bonds) between MoS 2 and N‐doped graphene.…”

A Short Review on the Electrochemical Performance of Hierarchical and Nitrogen-Doped Activated Biocarbon-Based Electrodes for Supercapacitors

“…The development of composites that combine pseudocapacitive behavior and EDLC response in highly porous structures (favored by high surface area and superior electrical conductivity) represents an important strategy to reach electrodes with outstanding electrochemical performance. Zhao et al [ 7 ] reported the development of high energy density and ultrahigh power density from the assembly of electrodes in the form of porous carbon pillars doped with heteroatoms.…”

“…Alternatives to incorporate pseudocapacitance in highly porous carbon derivatives involve the self-doping and artificial doping processes in porous structures. Artificial doping is based on the post-treatment of thermally treated carbon with amines, urea, or phosphoric acid [ 7 ]. On the other hand, self-doping is based on direct carbonization/pyrolysis of specific biomass rich in groups that introduce a more homogeneous distribution of heteroatoms into the structure’s bulk.…”

“…Given this, the presence of heteroatoms (N, P, S, B, and O) in biomass is preferable, allowing that doped materials can be obtained under thermal treatment and activation. Some examples of intrinsically doped biomass sources are gelatin from animal bones and nitrogen-rich japonica seed [ 7 ], winter-jujube (source of O and N) [ 9 ], Albizia flowers [ 10 ], Cicada slough (source of N, O, S, and P heteroatoms) [ 10 ], sharia bambusicola (source of N and Si) [ 11 ], boric acid and phosphoric acid (source of B, P, N, and O) [ 12 ], and chitosan as an essential source of N and P for self-doped heteroatom structures. It is typical for these structures that they are favored by the most straightforward strategies (one-pot methodology) [ 13 ], resulting in cost-effective electrodes and that favor scale-up based strategies.…”