Spin-modulated catalysis in sulfur cathodes for improved performance in lithium–sulfur batteries
Chaoyue Zhang, Jing Yu, Chenyang Huang, Gema Cabello, Xuede Qi, Guo Wen Sun, Chaoqi Zhang, Ren He, Dawei Yang, Canhuang Li, Junshan Li, Xueqiang Qi, Javier Rubio Garcia, Marta Estrader, Jordi Arbiol, Jinyuan Zhou, Andreu Cabot
Abstract
The rapid growth of electric vehicles and the increasing integration of renewable energy into the grid have heightened the demand for high-capacity energy storage systems based on abundant, low-cost materials. To address the limitations of conventional ion-intercalation batteries, conversion-type electrodes have gained significant attention, as their energy storage relies on chemical redox reactions often requiring activation or acceleration via electrocatalysis. Recent studies reveal that electrocatalytic activity is governed not only by active-site density and charge-carrier availability, but also by the spin states of electrons within the catalyst. Consequently, understanding the role of electronic spin states in battery performance, and how to manipulate them to enhance energy storage, has become a critical research frontier. This review provides a comprehensive overview of current strategies to modulate spin states in electrocatalysts for conversion-type cathodes. While external magnetic fields remain the primary method to probe and control electron spin, more practical and scalable approaches, such as atomic coordination engineering and surface spin filters, are emerging. Particular focus is given to sulfur cathodes, which offer exceptional theoretical energy density and capacity but depend heavily on catalytic hosts to enable efficient sulfur redox reactions. The review also surveys experimental techniques for probing spin states and theoretical approaches for modeling spin-related phenomena at the atomic scale. Finally, it highlights emerging research directions, underscoring the potential of spin-state modulation as a transformative strategy for next-generation energy storage technologies. Understanding the role of electronic spin states in electrodes is vital for improving battery performance. This Review discusses strategies to modulate spin states in electrocatalysts for conversion-type cathodes, with a focus on sulfur cathodes.