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Nolis, Gene M.,Adil, Abdullah,Yoo, Hyun Deog,Hu, Linhua,Bayliss, Ryan D.,Lapidus, Saul H.,Berkland, Lisa,Phillips, Patrick J.,Freeland, John W.,Kim, Chunjoong,Klie, Robert F.,Cabana, Jordi American Chemical Society 2018 The Journal of Physical Chemistry Part C Vol.122 No.8
<P>In this report, the feasibility of reversible Ca<SUP>2+</SUP> or Zn<SUP>2+</SUP> intercalation into a crystalline cubic spinel Mn<SUB>2</SUB>O<SUB>4</SUB> cathode has been investigated using electrochemical methods in an aqueous electrolyte. A combination of synchrotron XRD and XANES studies identified the partial structural transformation from a cubic to a tetragonally distorted spinel Mn<SUB>3</SUB>O<SUB>4</SUB>, accompanied by the reduction of Mn<SUP>4+</SUP> to Mn<SUP>3+</SUP> and Mn<SUP>2+</SUP> during discharge. TEM/EDX measurements confirmed that practically no Ca<SUP>2+</SUP> was inserted upon discharge. However, non-negligible amounts of Zn were detected after Mn<SUB>2</SUB>O<SUB>4</SUB> was reduced in the Zn<SUP>2+</SUP> electrolyte, but through the formation of secondary phases that, in some cases, appeared adjacent to the surface of a cathode particle. This report aims to identify bottlenecks in the application of manganese oxide cathodes paired with Ca or Zn metal anodes and to justify future efforts in designing prototype multivalent batteries.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jpccck/2018/jpccck.2018.122.issue-8/acs.jpcc.7b12084/production/images/medium/jp-2017-12084c_0006.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/jp7b12084'>ACS Electronic Supporting Info</A></P>