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In view of the long-standing controversy over the reversibility of transitionmetals in Sn-based alloys as anode for Li-ion batteries, an in situ real-timemagnetic monitoring method was used to investigate the evolution of Sn-Cointermetallic during the electrochemical cycling. Sn-Co alloy film anodes withdifferent compositions were prepared via magnetron sputtering without usingbinders and conductive additives. The magnetic responses showed that the Coparticles liberated by Li insertion recombine fully with Sn during thedelithiation to reform Sn-Co intermetallic into stannum richer phases Sn7Co3.However, as the Co content increases, it can only recombine partially with Sninto cobalt richer phases Sn3Co7. The unconverted Co particles may form a densebarrier layer and prevent the full reaction of Li with all the Sn in the anode,leading to lower capacities. These critical results shed light on understandingthe reaction mechanism of transition metals, and provide valuable insightstoward the design of high-performance Sn alloy based anodes.

In Operando magnetometry study on the charge storage mechanism of SnCo alloy lithium ion batteries