Introducing Highly Redox‐Active Atomic Centers into Insertion‐Type Electrodes for Lithium‐Ion Batteries

Abstract

The development of alternative anode materials with higher volumetric and gravimetric capacity allowing for fast delithiation and, even more important, lithiation is crucial for next‐generation lithium‐ion batteries. Herein, the development of a completely new active material is reported, which follows an insertion‐type lithiation mechanism, metal‐doped CeO2. Remarkably, the introduction of carefully selected dopants, herein exemplified for iron, results in an increase of the achievable capacity by more than 200%, originating from the reduction of the dopant to the metallic state and additional space for the lithium ion insertion due to a significant off‐centering of the dopant atoms in the crystal structure, away from the original Ce site. In addition to the outstanding performance of such materials in high‐power lithium‐ion full‐cells, the selective reduction of the iron dopant under preservation of the crystal structure of the host material is expected to open up a new field of research.

High-entropy energy materials: challenges and new opportunities

“…(3) Coating HEMs with carbonaceous or polymeric materials to improve the electronic conductivity, buffer the volume variations during cycling and passivate the surface of highly reactive particles in order to stabilize the electrode/electrolyte interface, thereby preventing electrolyte decomposition. 151,[153][154][155][156][157][158][159][160][161][162] As for the cathode side, no conversion-type HEMs have been reported so far. However, we believe that it is feasible to introduce this conversion mechanism into cathode materials, such as metal fluorides.…”

Ordered mesoporous metal oxides for electrochemical applications: correlation between structure, electrical properties and device performance

“…Especially for nanocrystalline materials, capacitive charge storage becomes significant and plays an important role in the performance and for the kinetics. 19,156,159,[164][165][166] Analysis of CV data for mesoporous TiO 2 thin films showed that the capacitive contribution to charge storage is virtually independent of the sweep rate, while the bulk insertion significantly decreases with increasing sweep rate. 19 For mesoporous MoS 2 , Cook et al found that 80% of the theoretical specific capacity is accessible within 20 s due to pseudocapacitive charge storage.…”

Embedding Heterostructured α‐MnS/MnO Nanoparticles in S‐Doped Carbonaceous Porous Framework as High‐Performance Anode for Lithium‐Ion Batteries

“…Using a self‐designed in‐situ cell (two‐electrode), [3,5] in situ XRD analysis of α‐MnS/MnO/SCPF was performed upon galvanostatic lithiation and delithiation during the first cycle. The WE slurry with 80 wt% α‐MnS/MnO/SCPF, 10 wt% super‐C65 and 10 wt% PVdF was cast onto a beryllium (Be) disk (wet thickness of 250 μm).…”

“…This is mainly caused by the commercially‐used graphite‐based negative electrodes, which have a relatively poor specific capacity of around 372 mAh g −1 [1–3] . Accordingly, the fast‐growing needs of batteries especially for automotive applications, derives scientists and engineers to explore high‐performance anode materials [1,4,5] …”