Oxygen Vacancy and Bandgap Simultaneous Modulation to Achieve High Lithiophilicity and Mechanical Strength of Lithium Metal Anodes

Abstract Metal oxides with conversion and alloying mechanisms are more competitive in suppressing lithium dendrites. However, it is difficult to simultaneously regulate the conversion and alloying reactions. Herein, conversion and alloying reactions are regulated by modulation of the zinc oxide bandgap and oxygen vacancies. State‐of‐the‐art advanced characterization techniques from a microcosmic to a macrocosmic viewpoint, including neutron diffraction, synchrotron X‐ray absorption spectroscopy, synchrotron X‐ray microtomography, nanoindentation, and ultrasonic C‐scan demonstrated the electrochemical gain benefit from plentiful oxygen vacancies and low bandgaps due to doping strategies. In addition, high mechanical strength 3D morphology and abundant mesopores assist in the uniform distribution of lithium ions. Consequently, the best‐performed ZnO‐2 offers impressive electrochemical properties, including symmetric Li cells with 2000 h and full cells with 81% capacity retention after 600 cycles. In addition to providing a promising strategy for improving the lithiophilicity and mechanical strength of metal oxide anodes, this work also sheds light on lithium metal batteries for practical applications.