Dynamics of Lithium Dendrite Growth and Inhibition: Pulse Charging Experiments and Monte Carlo Calculations.
Short-circuiting via dendrites compromises the reliability of Li-metal batteries. Dendrites ensue from instabilities inherent to electrodeposition that should be amenable to dynamic control. Here, we report that by charging a scaled coin-cell prototype with 1 ms pulses followed by 3 ms rest periods the average dendrite length is shortened ∼2.5 times relative to those grown under continuous charging. Monte Carlo simulations dealing with Li(+) diffusion and electromigration reveal that experiments involving 20 ms pulses were ineffective because Li(+) migration in the strong electric fields converging to dendrite tips generates extended depleted layers that cannot be replenished by diffusion during rest periods. Because the application of pulses much shorter than the characteristic time τc ∼ O(∼1 ms) for polarizing electric double layers in our system would approach DC charging, we suggest that dendrite propagation can be inhibited (albeit not suppressed) by pulse charging within appropriate frequency ranges.
†Linde Center for Global Environmental Science, ‡Materials and Process Simulation Center, California Institute of Technology, Pasadena, California 91125, United States.
Asghar
A
Aryanfar
†Linde Center for Global Environmental Science, ‡Materials and Process Simulation Center, California Institute of Technology, Pasadena, California 91125, United States.
Daniel
D
Brooks
†Linde Center for Global Environmental Science, ‡Materials and Process Simulation Center, California Institute of Technology, Pasadena, California 91125, United States.
Boris V
BV
Merinov
†Linde Center for Global Environmental Science, ‡Materials and Process Simulation Center, California Institute of Technology, Pasadena, California 91125, United States.
William A
WA
Goddard
†Linde Center for Global Environmental Science, ‡Materials and Process Simulation Center, California Institute of Technology, Pasadena, California 91125, United States.
Agustín J
AJ
Colussi
†Linde Center for Global Environmental Science, ‡Materials and Process Simulation Center, California Institute of Technology, Pasadena, California 91125, United States.
Michael R
MR
Hoffmann
Depletion double layers; Diffuse charge dynamics; Electromigration; Lithium batteries; Pulse electrolysis; Short-circuiting