Investigations of the Ag (I)-substituted Keggin K[HAgPWO] as a bifunctional Lewis acidic and basic catalyst are reported that explore the stabilization of LiS moieties so that reversible redox reactions in S-based electrodes would be possible. Spectroscopic investigations showed that the LiS-moieties can be strongly adsorbed on the {AgPWO} cluster, where the Ag(I) ion can act as a Lewis acid site to further enhance the adsorption of the S-moieties, and these interactions were investigated and rationalized using DFT. These results were used to construct an electrode for use in a Li-S battery with a very high S utilization of 94%, and a coulometric capacity of 1580 mAh g. This means, as a result of using the AgPOM, both a high active S content, as well as a high areal S mass loading, is achieved in the composite electrode giving a highly stable battery with cycling performance at high rates (1050 and 810 mAh g at 1C and 2C over 100 to 300 cycles, respectively).
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