Additional Lithium Storage on Dynamic Electrode Surface by Charge Redistribution in Inactive Ru Metal

Abstract

Beyond a traditional view that metal nanoparticles formed upon electrochemical reaction are inactive against lithium, recently their electrochemical participations are manifested and elucidated as catalytic and interfacial effects. Here, ruthenium metal composed of ≈5 nm nanoparticles is prepared and the pure ruthenium as a lithium‐ion battery anode for complete understanding on anomalous lithium storage reaction mechanism is designed. In particular, the pure metal electrode is intended for eliminating the electrochemical reaction‐derived Li2O phase accompanied by catalytic Li2O decomposition and the interfacial lithium storage at Ru/Li2O phase boundary, and thereby focusing on the ruthenium itself in exploring its electrochemical reactivity. Intriguingly, unusual lithium storage not involving redox reactions with electron transfer but leading to lattice expansion is identified in the ruthenium electrode. Size‐dependent charge redistribution at surface enables additional lithium adsorption to occur on the inactive but more environmentally sensitive nanoparticles, providing innovative insight into dynamic electrode environments in rechargeable lithium chemistry.

Unveiling the Genesis and Effectiveness of Negative Fading in Nanostructured Iron Oxide Anode Materials for Lithium-Ion Batteries

“…21,23,25,27−29 Interestingly, the reversible capacity of some nanostructured metal oxide anode materials is higher than the theoretical capacity expected based on conventional reaction mechanisms. 30,31 Some studies have attempted to unveil the origin of this extra capacity, and certain explanations have been proposed, 32,33 including (1) interfacial charge storage between metal nanoparticles and Li 2 O or defects in the nanostructure, 34−37 (2) formation of a reversible polymeric gel-like film via electrolyte decomposition, 14,38−42 and (3) redox reactions of Li-containing species. 2,15,43−46 Because these anomalous capacities are usually delivered in the low-voltage region after completion of the conventional reaction, the system becomes substantially complicated compared to the initial stage due to deep lithiation reactions of the electrode materials and electrolytes.…”

“…For electric vehicles to be widely accepted by the public, the sluggish electrochemical behavior of traditional lithium-ion batteries (LIBs) must be addressed by developing alternative electrode materials. Advanced electrode materials for LIBs may adopt a broad range of nanostructures that can be combined to afford appropriate electrochemical properties. − Thus, far, various transition metal oxides (TMOs) have been studied as anode materials for LIBs, and such oxides show high performance. − They provide a reversible capacity that is two to three times higher than the theoretical capacity of graphite, are strongly resistant to corrosion, and have excellent rate capability, with a low processing cost. − Extensive efforts have been dedicated to developing Fe 2 O 3 -based anode materials. Compared with other conversion-based TMOs or transition metal dichalcogenides (TMDCs), Fe 2 O 3 shows much better applicability and environmental compatibility due to its characteristics of low price, low toxicity, high theoretical capacity (1005 mAh·g –1 ), and eco-friendliness. − The density of Fe 2 O 3 (ca.…”

Achieving ultrastability and efficient lithium storage capacity with high-energy iron(ii) oxalate anode materials by compositing Ge nano-conductive sites

“…This suggests that a moderate amount of nano Ge metal attachment may reduce the formation of SEI films during the first discharge of iron oxalate, thus reducing the irreversible capacity. 50 The capacity retention for the second cycle has the same trend of 65.85, 71.89, 70.50, and 60.03%, respectively. As shown in Fig.…”

Controlling Gas Generation of Li-Ion Battery through Divinyl Sulfone Electrolyte Additive

“…Ab initio molecular dynamics (AIMD) simulations were proven to be useful for electrolyte reactions [14,15] as well as for the modeling of a battery's electrode [16][17][18]. In our study, AIMD simulations of electrolyte mixtures were performed to better understand the effects of DVSF additives.…”