Revealing the Self-Doping Defects in Carbon Materials for the Compact Capacitive Energy Storage of Zn-Ion Capacitors.

Zn-ion capacitors are attracting great attention owing to the abundant and relatively stable Zn anodes but are impeded by the low capacitance of porous carbon cathodes with insufficient energy storage sites. Herein, using ball-milled graphene with different defect densities as the models, we reveal that the self-doping defects of carbon show a capacitive energy storage behavior with robust charge-transfer kinetics, providing a capacitance contribution of ca. 90 F g-1 per unit of defect density (AD/AG value from Raman spectra) in both aqueous and organic electrolytes. Furthermore, a simple NaCl-assisted ball-milling method is developed to prepare novel graphene blocks (BSG) with abundant self-doping defect density, enriched pores, balanced electric conductivity, and high compact density (0.83 g cm-3). The optimized ion and electron transfer paths promote efficient utilization of the self-doping defects in BSG, contributing to improved gravimetric and volumetric capacitance (224 F g-1/186 F cm-3 at 0.5 A g-1) and remarkable rate performance (52.2% capacitance retention at 20 A g-1). The defect engineering strategy may open up a new avenue to improve the capacitive performance of dense carbons for Zn-ion capacitors.

Interfacial Anchored Sesame Ball-like Ag/C To Guide Lithium Even Plating and Stripping Behavior.

Lithium (Li) metal is a candidate anode for the next generation of high-energy density secondary batteries. Unfortunately, Li metal anodes (LMAs) are extremely reactive with electrolytes to accumulate uncontrolled dendrites and to generate unwanted parasitic electrochemical reactions. Much attention has been focused on carbon materials to address these issues. Ulteriorly, the failure mechanism investigation of lithiophilic sites on carbon materials has been not taken seriously. Herein, we design a new type of sesame ball-like carbon sphere (AgNPs@CS, an average diameter of ∼700 nm) with uniformly interfacial anchored silver nanoparticles (AgNPs), which is used as the dendrite-free Li metal anode host. This anchored structure significantly enhances reversible and chemical affinity of Li, effectively inhibiting "dead Li". In addition, the protective effect of the carbon layer can avoid the damage of lithiophilic AgNPs in the carbon matrix. With a plating/striping capacity of 2 mA h cm-2, the AgNPs@CS electrode can be cycled over 2400 h at 0.5 mA cm-2. When the stripping voltage increases to 1 V, the AgNPs@CS electrode also enables excellent cycling stability to achieve over 260 cycles (1 mA cm-2, 1 mA h cm-2) and 130 cycles (2 mA cm-2, 1 mA h cm-2). This material by electrochemical characterization highlights the efficacy of this facile method for developing dendrite-free LMAs.