In Situ Templating Approach To Fabricate Small-Mesopore-Dominant S-Doped Porous Carbon Electrodes for Supercapacitors and Li-Ion Batteries

Abstract

To enable large capacity and high rate capability of porous carbon electrodes for lithium-ion batteries (LIBs) and supercapacitors, the combination of doping active heteroatoms, tailoring pore architectures, and narrowing pore sizes is a powerful engineered strategy. However, such porous carbons with multiple synergistic effects are almost impossible to be achieved simultaneously by conventional synthesis methods in a few steps. Herein, two mechanistically coupled polymers of poly(2thiophenemethanol) (PThM) and SiO 2 in one step process were synchronically produced by twin-polymerization of a single-source hybrid monomer of tetrathenyloxysilane consisting of tetraethyl orthosilicate (TEOS) and ThM moieties. The resultant interpenetrated SiO 2 /PThM composites were then subjected to thermal annealing and subsequent etching, yielding a mesopore-dominant S-doped porous carbon (SPC-1) with large-micropores (1.3−2.0 nm), narrow pore distribution (1.3−4.1 nm, centered at 3.1 nm), rich S heteroatoms (>5%), and high specific surface area (792 m 2 /g). Remarkably, the symmetric supercapacitor based on SPC-1 delivers a specific capacitance of 420 F/g at 0.5 A/g and an energy density as high as 14.6 W h/ kg at the power density of 125 W/kg. As an anode for LIBs, SPC-1 delivers large reversible capacity (571 mAh/g), high rate capability, and excellent cyclic stability (without capacity decay after 500 cycles). More importantly, SPC-1 shows better electrochemical performance compared to a large mesopore (6−30 nm)-dominant S-doped porous carbon (SPC-2) derived by simultaneous polymerization of TEOS and ThM. This work reports an unusual in situ templating approach capable of synergistically combining chemical doping and pore engineering of carbonaceous materials for high-performance supercapacitors and LIBs.

Preparation of Sulfur‐doped Carbon for Supercapacitor Applications: A Review

“…SPC exhibited excellent specific capacitance value due to the narrow pore size distribution, high SSA, high content of S-doping. [54] Deng et. al.…”

“…The heteroatom doping enhances the electronic conductivity, surface wettability, electrochemical reactivity, and interface compatibility between the electrode and electrolyte. [53,54] Different heteroatoms, such as nitrogen, boron, phosphorus, oxygen, and sulfur, are used as carbon-doping elements in SCs applications. [55,56] Among them, S-doped carbon has gained considerable attention in SCs applications.…”

Accurate Control Multiple Active Sites of Carbonaceous Anode for High Performance Sodium Storage: Insights into Capacitive Contribution Mechanism

“…The TEM image in Figure 1d reveals an ordered interconnected wormhole-like microporous structure with average pore size nearly 5 nm. After calcining, several graphitic microcrystallites ( Figure 1e) appear like bent layered ribbon planes with a lattice spacing of 0.41 nm, larger than typical graphitized carbon (0.34 nm), [46] which is ascribed to the introduction of larger S atom and well meet the requirements of sodium ion intercalation spacing in graphitic carbon planes in the meantime. [32] The EDS mappings ( Figure 1f) exhibit C, O, S, and N elements are evenly distribute on the N 0.2 S 0.8 -MC surface.…”

Multiple Active Sites Carbonaceous Anodes for Na+ Storage: Synthesis, Electrochemical Properties and Reaction Mechanism Analysis

“…[ 93 ] First, a typical Nyquist plot of Na battery mainly consist of two semicircles in medium and high frequency ranges, with a short slope tail at low frequency. [ 164,165 ] The first intercept at Z ’ axis (at very high frequency region) corresponds to the electrolyte resistance ( R S ), the former semicircle position at high frequency region is assigned to interlayer diffusion process on the stable SEI nanolayer ( R Suf ), the latter semicircle at medium frequency region is attributed to R CT , and the final slope tail at low frequency region is ascribed to the Warburg impedance ( Z W ) corresponding to the ion diffusion impedance into porous structure. [ 166 ] Hence, the R mainly reflects the intrinsic property of the electrode, and the fitting linear was further carried out to evaluate the Warburg coefficient (σ) and D Na+ according to the Equations (5) and (6) σω −1/2 corresponds to real part ( Z ′), −j σω −1/2 belongs to imaginary part ( Z ″) and Z W is Warburg impedance.…”