Synergized Multimetal Oxides with Amorphous/Crystalline Heterostructure as Efficient Electrocatalysts for Lithium–Oxygen Batteries

Abstract

High theoretical specific energy of rechargeable lithium–oxygen (Li–O2) batteries makes them very promising in the development of long driving range electric vehicles and energy storage on large‐scale. However, the large polarization and poor cycling stability associated with insufficient catalytic cathodes and the insulating nature of discharge products limit their practical applications. Here, the fabrication of a trimetallic CoFeCe oxide with an amorphous/crystalline heterostructure acting as an electrocatalyst for the Li–O2 battery cathode is reported. The best‐performing CoFeCe oxide cathode manages to deliver an initial discharge capacity of 12 340 mAh g−1, while maintaining an impressively enhanced cyclic stability over 2900 h at 100 mA g−1. As revealed by combined experimental results and density functional theory (DFT) analysis, synergistic interaction between oxide components, amorphous–crystalline domains, unique heterostructure with minimized lattice mismatch, and the enhanced adsorption of the key intermediate LiO2 are critical factors in boosting the electrocatalytic activity of CoFeCe toward the formation of decomposable Li2O2. This work offers a new insight to rationally design and synthesize an effective multimetal oxide electrocatalyst for the Li–O2 battery cathode.

2D SnSe Cathode Catalyst Featuring an Efficient Facet‐Dependent Selective Li2O2 Growth/Decomposition for Li–Oxygen Batteries

“…09‐0355) were collected after discharge at a voltage window 2.35−4.35 V, demonstrating good crystallinity of the discharge products. [ 53 ] The discharge products decomposed completely after charging, and the crystallinity of the SnSe nanosheet changed slightly after 100 cycles. Raman spectroscopy and Fourier transform infrared spectroscopy (FTIR) provide further evidence for the species on the electrode surface.…”

Harnessing the Defects at Hetero‐Interface of Transition Metal Compounds for Advanced Charge Storage: A Review

“…For example, the addition of Ce when constructing a Fe 2 O 3 –CoO heterojunction resulted in the formation of a CeO 2 buffer layer, which reduced the lattice mismatch and dislocation between the two materials and improved the cyclic stability and capacity of the ternary oxide. [ 193 ] 5) Recent experimental and computational studies have shown that there can be more than one kind of defect at the hetero‐interface at the same time, and each kind of defect can change the state of the interface, thereby affecting the energy storage performance of the transition metal oxide. Thus, future work should focus on maximizing the performance of heterostructure electrodes by manipulating various defects at the interface.…”

Interfacial engineering in amorphous/crystalline heterogeneous nanostructures as a highly effective battery-type electrode for hybrid supercapacitors

“…More importantly, the loosely packed structure is more conducive to buffer volume change and rapid ion transmission during the redox process in the bulk of the phosphide. 18 However, pure amorphous materials often exhibit lower conductivity and toughness than crystalline materials, which limit their individual application. Inspired by these, crystalline bimetallic oxides combined with amorphous phosphides to form a unique amorphous-crystalline structure, which combined with the advantages of high electrical conductivity and high specific capacity of the crystal phase, and with the disordered arrangement of the amorphous phase, which can achieve excellent rate capability and cycling stability.…”