Aluminium and magnesium insertion in sulfur-based spinels: a first-principles study

Area of Science:

• Materials Science
• Electrochemistry
• Computational Chemistry

Background:

• Development of advanced energy storage solutions is crucial for next-generation technologies.
• Aluminum (Al) and magnesium (Mg) ion batteries offer potential advantages over conventional lithium-ion systems.
• Identifying suitable electrode materials is a key challenge for Al- and Mg-ion battery development.

Purpose of the Study:

• To computationally screen sulfur-based spinel materials as potential hosts for Al and Mg ion insertion.
• To evaluate the impact of transition metal substitution on electrode performance characteristics.
• To identify promising cathode materials for Al- and Mg-ion batteries.

Main Methods:

• Computational screening of sulfur-based materials with a spinel crystal structure.
• Systematic calculation of thermodynamic stability, average voltage, binding energy, and volume expansion.
• Evaluation of Al and Mg diffusion kinetics within the material structures.

Main Results:

• Transition metal substitution significantly influences the electrochemical properties of spinel materials.
• The Ni-based spinel exhibited a relatively high Al and Mg insertion voltage.
• Low diffusion barriers for Al and Mg ions were observed in the Ni-based spinel.

Conclusions:

• Sulfur-based spinels are viable candidates for Al- and Mg-ion battery electrode materials.
• The Ni-based spinel demonstrates excellent potential as a cathode material for both Al- and Mg-ion batteries.
• Further experimental validation is warranted to confirm the computational findings.