An Aluminum-Sulfur Battery with a Fast Kinetic Response.

The electrochemical performance of the aluminum-sulfur (Al-S) battery has very poor reversibility and a low charge/discharge current density owing to slow kinetic processes determined by an inevitable dissociation reaction from Al2 Cl7- to free Al3+ . Al2 Cl6 Br- was used instead of Al2 Cl7- as the dissociation reaction reagent. A 15-fold faster reaction rate of Al2 Cl6 Br- dissociation than that of Al2 Cl7- was confirmed by density function theory calculations and the Arrhenius equation. This accelerated dissociation reaction was experimentally verified by the increase of exchange current density during Al electro-deposition. Using Al2 Cl6 Br- instead of Al2 Cl7- , a kinetically accelerated Al-S battery has a sulfur utilization of more than 80 %, with at least four times the sulfur content and five times the current density than that of previous work.

Atomically Dispersed Iron Active Sites Promoting Reversible Redox Kinetics and Suppressing Shuttle Effect in Aluminum-Sulfur Batteries.

Rechargeable aluminum-sulfur (Al-S) batteries have been considered as a highly potential energy storage system owing to the high theoretical capacity, good safety, abundant natural reserves, and low cost of Al and S. However, the research progress of Al-S batteries is limited by the slow kinetics and shuttle effect of soluble polysulfides intermediates. Herein, an interconnected free-standing interlayer of iron single atoms supported on porous nitrogen-doped carbon nanofibers (FeSAs-NCF) on the separator is developed and used as both catalyst and chemical barrier for Al-S batteries. The atomically dispersed iron active sites (Fe-N4) are clearly identified by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption near-edge structure. The Al-S battery with the FeSAs-NCF shows an improved specific capacity of 780 mAh g-1 and enhanced cycle stability. As evidenced by experimental and theoretical results, the atomically dispersed iron active centers on the separator can chemically adsorb the polysulfides and accelerate reaction kinetics to inhibit the shuttle effect and promote the reversible conversion between aluminum polysulfides, thus improving the electrochemical performance of the Al-S battery. This work provides a new way that can not only promote the conversion of aluminum sulfides but also suppress the shuttle effect in Al-S batteries.