The extreme fast-charging capability of lithium-ion batteries (LIBs) is very essential for electric vehicles (EVs). However, currently used graphite anode materials cannot satisfy the requirements of fast charging. Herein, we demonstrate that intrinsic lattice defect engineering based on a thermal treatment of graphite in CO2 is an effective method to improve the fast-charging capability of the graphite anode. The activated graphite (AG) exhibits a superior rate capability of 209 mAh g-1 at 10 C (in comparison to 15 mAh g-1 for the pristine graphite), which is attributed to a pseudocapacitive lithium storage behavior. Furthermore, the full cell LiFePO4||AG can achieve SOCs of 82% and 96% within 6 and 15 min, respectively. The intrinsic carbon defect introduced by the CO2 treatment succeeds in improving the kinetics of lithium ion intercalation at the rate-determining step during lithiation, which is identified by the distribution of relaxation times (DRT) and density functional theory (DFT) calculations. Therefore, this study provides a novel strategy for fast-charging LIBs. Moreover, this facile method is also suitable for activating other carbon-based materials.

Introducing a Pseudocapacitive Lithium Storage Mechanism into Graphite by Defect Engineering for Fast-Charging Lithium-Ion Batteries.

Perovskites have shown tremendous promise as functional materials for several energy conversion and storage technologies, including rechargeable batteries, (electro)catalysts, fuel cells, and solar cells. Due to their excellent operational stability and performance, high‐entropy perovskites (HEPs) have emerged as a new type of perovskite framework. Herein, this work reviews the recent progress in the development of HEPs, including synthesis methods and applications. Effective strategies for the design of HEPs through atomistic computations are also surveyed. Finally, an outlook of this field provides guidance for the development of new and improved HEPs.

High‐Entropy Perovskites for Energy Conversion and Storage: Design, Synthesis, and Potential Applications

Na4Fe3(PO4)2P2O7 (NFPP) is considered to be an ideal cathode material for sodium-ion batteries due to its high theoretical capacity, stable structure, small volume change, low cost, and nontoxicity. However, the inherent low electronic conductivity of polyanionic materials limits the application of this material. In this work, we improved the electronic conductivity and structural stability of the material through a dual modification synergistic strategy of manganese ion doping and surface carbon coating and prepared Na4Fe2.9Mn0.1(PO4)2P2O7@C (0.1 Mn-NFPP@C) composites by a simple mechanical-assisted chemical synthesis method. It can release 119.6 mAh g–1 at 0.1C. The capacity retention rate is 97.4% after 100 cycles at 1C and 84.8% after 3000 cycles at 10C. Many tests and calculations in this work also show that 0.1 Mn-NFPP@C modified by Mn2+ doping and carbon coating has higher electronic conductivity and electrochemical kinetics and thus exhibits better electrochemical performance. 

Mn-Doped Na4Fe3(PO4)2P2O7 as a Low-Cost and High-Performance Cathode Material for Sodium-Ion Batteries

Na4Fe3(PO4)2(P2O7) (NFPP) is an attractive cathode material for sodium-ion batteries (SIBs) due to its low-cost, robust framework, and cross-linked Na+ migrate channels. However, the real implementation of NFPP remains in its infancy, mainly hindered by the inferior intrinsic electronic conductivity. Herein, a doping strategy by incorporating manganese into NFPP lattice (NFMPP) is proposed to lower the band gap and Na+ migrate barriers, thus ultimately rendering robust ligand framework, improved electronic transmission and fast ions diffusion. Greatly, the ultralong-lasting cyclability (88.1% capacity retention for over 10000 cycles at 50 C), impressive rate capability (42.7 mAh g−1 at 200 C), and decent electrochemical performance over a wide operation-temperature range from − 40–60 ℃ are achieved. The structural evolution and charge compensation mechanism during cell operation are systematically explored utilizing in situ X-ray diffraction (XRD) and X-ray absorption near edge structure (XANES) measurements, confirming a minimized volume fluctuation and highly reversible Fe2+/Fe3+ redox reaction. Full cell comprising a NFMPP cathode and pre-sodiated hard carbon anode is also yielded as proof of concept. The superior electrochemical performances, and the insertion/extraction mechanism investigation sheds light to the feasibility of utilizing NFMPP as a cathode material for low-cost and high-performance gride-scale energy storage systems (EESs). 

Robust iron-based cathode for ultralong-lasting Na-ion battery with a wide operation-temperature

The high‐entropy materials (HEM) have attracted increasing attention in catalysis and energy storage due to their large configurational entropy and multiunique properties. However, it is failed in alloying‐type anode due to their Li‐inactive transition‐metal compositions. Herein, inspired by high‐entropy concept, the Li‐active elements instead of transition‐metal ones are introduced for metal‐phosphorus synthesis. Interestingly, a new ZnxGeyCuzSiwP2 solid solution is successfully synthesized as proof of concept, which is first verified to cubic system in F‐43m. More specially, such ZnxGeyCuzSiwP2 possesses wide‐range tunable region from 9911 to 4466, in which the Zn0.5Ge0.5Cu0.5Si0.5P2 accounts for the highest configurational entropy. When served as anode, ZnxGeyCuzSiwP2 delivers large capacity (>1500 mAh g−1) and suitable plateau (≈0.5 V) for energy storage, breaking the conventional view that HEM is helpless for alloying anode due to its transition‐metal compositions. Among them, the Zn0.5Ge0.5Cu0.5Si0.5P2 exhibits the highest initial coulombic efficiency (ICE) (93%), Li‐diffusivity (1.11 × 10−10), lowest volume‐expansion (34.5%), and best rate performances (551 mAh g−1 at 6400 mA g−1) owing to its largest configurational entropy. Possible mechanism reveals the high entropy stabilization enables good accommodation of volume change and fast electronic transportation, thus supporting superior cyclability and rate performances. This large configurational entropy strategy in metal‐phosphorus solid solution may open new avenues to develop other high‐entropy materials for advanced energy storage.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202300271

Understanding the Configurational Entropy Evolution in Metal‐Phosphorus Solid Solution for Highly Reversible Li‐Ion Batteries

A microstructure engineered perovskite super anode with Li-storage life of exceeding 10,000 cycles

Iron-based mixed-polyanionic cathode Na4Fe3(PO4)2(P2O7) (NFPP) has advantages of environmental benignity, easy synthesis, high theoretical capacity, and remarkable stability. From NFPP, a novel Li-replaced material NaLi3Fe3(PO4)2(P2O7) (NLFPP) is synthesized through active Na-site structural engineering by an electrochemical ion exchange approach. The NLFPP cathode can show high reversible capacities of 103.2 and 90.3 mA h g-1 at 0.5 and 5C, respectively. It also displays an impressive discharge capacity of 81.5 mA h g-1 at an ultrahigh rate of 30C. Density functional theory (DFT) calculation demonstrates that the formation energy of NLFPP is the lowest among NLFPP, NFPP, and NaFe3(PO4)2(P2O7), indicating that NLFPP is the easiest to form and the conversion from NFPP to NLFPP is thermodynamically favorable. The Li substitution for Na in the NFPP lattice causes an increase in the unit cell parameter c and decreases in a, b, and V, which are revealed by both DFT calculations and in situ X-ray powder diffraction (XRD) analysis. With hard carbon (HC) as the anode, the NLFPP//HC full cell shows a high reversible capacity of 91.1 mA h g-1 at 2C and retains 82.4% after 200 cycles. The proposed active-site-specific structural tailoring via electrochemical ion exchange will give new insights into the design of high-performance cathodes for lithium-ion batteries.

Active-Site-Specific Structural Engineering Enabled Ultrahigh Rate Performance of the NaLi3Fe3(PO4)2(P2O7) Cathode for Lithium-Ion Batteries.

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A microstructure engineered perovskite super anode with Li-storage life of exceeding 10,000 cycles

Active-Site-Specific Structural Engineering Enabled Ultrahigh Rate Performance of the NaLi3Fe3(PO4)2(P2O7) Cathode for Lithium-Ion Batteries.