Heteroatom-Rich Porous Carbons Derived from Nontoxic Green Organic Crystals for High-Performance Symmetric and Asymmetric Supercapacitors with Aqueous/Gel Electrolyte

Abstract

Developing heteroatom-rich porous carbon (HPC) for electricity storage promotes the use of green sustainable energy. To efficiently prepare and optimize HPC, it is necessary to explore its formation/doping mechanism. Here, HPCs are prepared from nontoxic organic crystals, and quantum chemical calculations and ReaxFF MD simulations are performed. Effects of carbon chains and functional groups on HPCs are investigated. In micromorphology, the open-chain compound changes little and is etched into interconnected particles. The compounds containing ring chains change a lot and form 2D thin layers. The dimer forms 3D flower-like structures composed of thin layers. During doping, N in the amino group has a tendency to form pyrrolic-N, and N in the N-heterocycle has a tendency to form quaternary-N. L-lysine-derived HPC shows a large specific surface area (3353.99 m 2 g −1 ). For symmetric supercapacitor, it possesses high specific capacitance (439.11 F g −1 at 0.3 A g −1 and 265.57 F g −1 at 100 A g −1 ) and high cyclic stability (maintained 96.86% after 5000 cycles). For asymmetric supercapacitor, it shows more pseudocapacitance (accounted for 33.84% at 20 mV s −1 ) and higher specific capacitance (586.58 F g −1 at 0.3 A g −1 and 457.40 F g −1 at 100 A g −1 ). In gel electrolyte, its power density and energy density increase by 39.58% and 133.21%, respectively, with voltage rising from 1 V to 1.4 V. The results provide theoretical guidance and high-performance HPCs for clean energy storage/conversion.

Adapting a Kinetics-Enhanced Carbon Nanostructure to Li/Na Hybrid Water-in-Salt Electrolyte for High-Energy Aqueous Supercapacitors

“…Upon cycling, the Li 10 Na 3 OTf-loaded device reveals high electrochemical recoverability (98%, Figure S16a), desirable capacitive endurance (85.5% energy retention after 10 000 successive cycling at 10 A g –1 , Figure a), and Coulombic efficiency (98.4%, Figure a). Correspondingly, the energy supply reaches 39.2 Wh kg –1 @550 W kg –1 and maintains at 28.2 Wh kg –1 @22 kW kg –1 (Figures b and S16b,c), outperforming those of other reported aqueous devices. ,,,,,,− The appropriate compatibility of carbon nanostructure/electrolyte integrates their respective advantages (Figure c), providing the possibility for electronic applications with different rated voltages. More attractively, a single device successfully supports the timer (1.5 V) to work continuously over 6 h (Figure d).…”

“…During temperature-programmed thermolysis, KOH first removes residual Cl atoms trapped in TBQ/ X polymer networks to fix the micromorphology, and then tends to break thermolysis-trigger reactive sites and non-cyclic carbon chains for microstructure evolution. − As presented in Figure , TBQ/ X derived carbons based on different chain motifs exhibit variable morphologies, such as nanoparticles (C TBQ/DQ , Figure a), nanofibers (C TBQ/MD , Figure b), nanosheets (C TBQ/OD , Figure c), and honeycomb-like foams (C TBQ/AB , Figure d). Additionally, elemental maps (Figure e–h) of C TBQ/ X show uniform dispersion of heteroatom doping.…”

Ultralong-Life Supercapacitors Using Pyridine-Derived Porous Carbon Materials

“…The C-700 sample exhibited a superior electrochemical cycle performance, and it still maintained 160.9 F/g specific capacitance (91.7% of the initial) after 89,000 cycles. The excellent cycle performance is highly competitive to other similar carbon materials doped with heteroatoms, for example, heteroatom-rich porous carbon (96.86% retention after 5000 cycles), 58 phosphorus-and boron-incorporated activated carbon (88% retention after 30,000 cycles), 59 N-graphyne (87% retention after 3000 cycles), 60 and N-doped porous carbon (94.1% retention after 10,000 cycles). 51 The reference results show that carbon materials with different morphologies and electrochemical performances can be obtained by adjusting the raw material ratio, carbonization temperature, 63 and heating time.…”

Ionothermal synthesis of magnetic N-doped porous carbon to immobilize Pd nanoparticles: An efficient heterogeneous catalyst for reduction of nitroaromatic compounds

“…[38], L-lysine, tyrosine, and L-cysteine [39]. In addition, N-doped porous carbon substrates are prepared and synthesized by various methods, including hard and soft templates [40], thermal polymerization [41], post-treatment [42], and chemical vapor deposition (CVD) [43], solvothermal and ionothermal methods [44,45].…”