Sustainable Polyvinyl Chloride-Derived Soft Carbon Anodes for Potassium-Ion Storage: Electrochemical Behaviors and Mechanism.

Soft carbon is a promising anode material for potassium-ion batteries due to its favorable properties such as low cost, high conductivity, stable capacity, and low potential platform. Polyvinyl chloride, as a white pollutant, is a soft carbon precursor that can be carbonized at varying temperatures to produce soft carbons with controllable defect and crystal structures. This work investigates the effect of carbonization temperature on the crystalline structures of the obtained soft carbons. In situ Raman spectroscopy was used to elucidate the adsorption-intercalation charge storage mechanism of potassium ions in soft carbons. Soft carbons prepared at the temperature of 800 °C have a defect-rich, short-range ordered structure, which provides optimal intercalation and adsorption sites for potassium ions, resulting in a satisfactory capacity of 302 mAh g-1 . This work presents new possibilities for designing soft carbon materials from recycling plastics for potassium-ion batteries.

Synergistic effect of nitrogen and oxygen dopants in 3D hierarchical porous carbon cathodes for ultra-fast zinc ion hybrid supercapacitors.

Zinc-ion hybrid supercapacitor is one of the most promising electrochemical energy storage devices for the applications needing both high energy densities and power densities. Nitrogen doping is an effective way to enhance the capacitive performance of porous carbon cathodes in zinc-ion hybrid supercapacitor. However, accurate evidence is yet needed to demonstrate how nitrogen dopants influence the charge storage of Zn2+ and H+ cations. Herein, we prepared 3D interconnected hierarchical porous carbon nanosheets by a one-step explosion method. The effect of nitrogen dopants on pseudocapacitance was analyzed by the electrochemical behaviors of as-prepared porous carbon samples with similar morphology and pore structure but different nitrogen and oxygen doping levels. Ex-situ XPS and DFT calculation demonstrate that nitrogen dopants promote the pseudocapacitive reactions by lowering the energy barrier for the change of oxidation states of carbonyl moieties. Owing to the improved pseudocapacitance by nitrogen/oxygen dopants and fast diffusion of Zn2+ ions in 3D interconnected hierarchical porous carbon matrix, the as-constructed ZIHCs show both high gravimetric capacitance (301 F g-1 at 0.1 A g-1) and excellent rate capability (a capacitance retention of 30% at 200 A g-1).

Enzymatic Hydrolysis Lignin-Derived Porous Carbons through Ammonia Activation: Activation Mechanism and Charge Storage Mechanism.

The low energy density and low cost performance of electrochemical capacitors (ECs) are the principal factors that limit the wide applications of ECs. In this work, we used enzymatic hydrolysis lignin as the carbon source and an ammonia activation methodology to prepare nitrogen-doped lignin-derived porous carbon (NLPC) electrode materials with high specific surface areas. We elucidated the free radical mechanism of ammonia activation and the relationship between nitrogen doping configurations, doping levels, and preparation temperatures. Furthermore, we assembled NLPC∥NLPC symmetric ECs and NLPC∥Zn asymmetric ECs using aqueous sulfate electrolytes. Compared with the ECs using KOH aqueous electrolyte, the energy densities of NLPC∥NLPC and NLPC∥Zn ECs were significantly improved. The divergence of charge storage characteristics in KOH, Na2SO4, and ZnSO4 electrolytes were compared by analyzing their area surface capacitance. This work provides a strategy for the sustainable preparation of lignin-derived porous carbons toward ECs with high energy densities.

Molten Salt Self-Template Synthesis Strategy of Oxygen-Rich Porous Carbon Cathodes for Zinc Ion Hybrid Capacitors.

Porous carbon materials are widely used in capacitive energy storage devices because of their chemical stability, low cost, and controllable textures. Molten salt self-template methods are powerful and sustainable synthesis strategies for preparing porous carbons with tunable pore textures and surface chemistries. Herein, we propose a self-template synthesis strategy for preparing oxygen-rich porous carbons (ORC) by directly carbonizing potassium chloroacetate (ClCH2COOK) as the single carbon source. The potassium chloride salts generated in the carbonization play the roles of the template and etchant agent in the pore formation process. The as-prepared ORC samples feature abundant mesopores (average pore sizes of 1.95-2.19 nm and mesopore ratio of 36.4%), high specific surface areas (1410-1886 m2 g-1), and high oxygen doping levels (4.3-8.2 atom %). The zinc ion hybrid capacitors with an ORC cathode exhibited an ultrahigh capacitance of 308 F g-1 at 0.5 A g-1 and a high energy density of 136.5 Wh kg-1 at a power density of 570 W kg-1. Density functional theory demonstrates that oxygen-containing functional groups are conducive to the adsorption of Zn ions. Our work proposes a general synthesis methodology for the synthesis of oxygen-rich porous carbons for a variety of electrochemical energy storage devices.