Abstract
Development of sodium solid electrolytes with high ionic conductivity and good interface stability towards Na metal plays a dominant role in achieving stable all-solid-state sodium batteries. Herein, WS2-doped Na3-xSb1-xWxS4 and WO2-doped Na3-xSb1-xWxS4–2xO2x (x = 0.025, 0.05, 0.075, 0.1) solid electrolytes are successfully synthesized by melt-quenching method followed by an annealing procedure. Compared with 0.98 mS cm−1 for pristine Na3SbS4, the dramatically enhanced room temperature ionic conductivities of 10.37 and 8.49 mS cm−1 are achieved for Na2.95Sb0.95W0.05S4 and Na2.95Sb0.95W0.05S3.9O0.1, respectively. In addition, it is found that the introduction of oxygen in Na3SbS4 through W and O co-doping can alleviate the deteriorative Na/solid electrolyte interface induced by W substitution. The modified interface stability is demonstrated by the suppressed increase of Na plating/striping voltage and impedance for the symmetric Na/Na2.95Sb0.95W0.05S3.9O0.1/Na cells. Moreover, in contrast with rapid capacity decay for TiS2/Na2.95Sb0.95W0.05S4/Na battery, the batteries employing Na2.95Sb0.95W0.05S3.9O0.1 exhibit stable cyclic performance and good rate capability. This work provides a W and O co-doping strategy for preparing Na3SbS4 solid electrolytes with simultaneously enhanced ionic conductivity and interface stability.
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