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The design and development of materials for electrochemical energy storage and conversion devices requires fundamental understanding of chemical interactions at electrode/electrolyte interfaces. For Li–S batteries that hold the promise for outperforming the current generation of Li ion batteries, the interactions of lithium polysulfide (LPS) intermediates with the electrode surface strongly influence the efficiency and cycle life of the sulfur cathode. While metal oxides have been demonstrated to be useful in trapping LPS, the actual binding modes of LPS on 3d transition metal oxides and their dependence on the metal element identity across the periodic table remain poorly understood. Here, we investigate the chemical interactions between LPS and oxides of Mn, Fe, Co, and Cu by combining X-ray photoelectron spectroscopy and density functional theory calculations. We find that Li–O interactions dominate LPS binding to the oxides (Mn3O4, Fe2O3, and Co3O4), with increasing strength from Mn to Fe to Co. For C...

Mechanistic Insights into Surface Chemical Interactions between Lithium Polysulfides and Transition Metal Oxides