Boosting Molecular Cross-Linking in a Phenolic Resin for Spherical Hard Carbon with Enriched Closed Pores toward Enhanced Sodium Storage Ability.

Phenolic resin (PF) is considered a promising precursor of hard carbon (HC) for advanced-performance anodes in sodium-ion batteries (SIBs) because of its facile designability and high residual carbon yield. However, understanding how the structure of PF precursors influences sodium storage in their derived HC remains a significant challenge. Herein, the microstructure of HC is controlled by the degree of cross-linking of resorcinol-benzaldehyde (RB) resin. We reveal that robust molecular cross-linking in RB resin induced by hydrothermal treatment promotes closed-pore formation in the derived HC. The mechanism is devised for the decomposition of a highly cross-linked RB three-dimensional network into randomly stacked short-range graphitic microcrystals during high-temperature carbonization, contributing to the abundant closed pores in the derived HC. In addition, the high cross-linking degree of RB resin endows its derived HC with a small-sized spherical morphology and large interlayer spacing, which improves the rate performance of HC. Consequently, the optimized hydrothermal treatment HC anode shows a higher specific capacity of 372.7 mAh g-1 and better rate performance than the HC anode without hydrothermal treatment (276.0 mAh g-1). This strategy can provide feasible molecular cross-linking engineering for the development of closed pores in PF-based HC toward enhanced sodium storage.

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.