Because of abundant resource, low cost and high reversible specific capacity, hard carbon (HC) is considered to be the most likely commercial anode material for sodium-ion batteries (SIBs). Therefore, the...

Hard Carbon for Sodium-ion Batteries: Progress, Strategy and Future Perspective

Recent progress in rational structural regulation for high-efficiency potassium-ion batteries is reviewed. 

Recent advances in rational design for high-performance potassium-ion batteries

Compared to traditional modulation by metal cations doping, oxyanions offer a higher possibility of mediating the performance of electrocatalysts toward oxygen evolution reaction (OER) due to their special polyanion configurations and large electronegativity. However, the mechanism and rules of oxyanions mediation remain poorly understood. Herein, an in situ electrochemical oxyanion (NO3−, PO43−, SO42−, or SeO42−) steering strategy to study the variation and rules of OER performance for transition‐metal (TM = Ni, Fe, Co) hydroxide electrocatalysts is reported. Electrocatalytic experiments indicate both activity and stability of oxyanion‐modified TM hydroxides follow the order of PO43− > NO3− > SO42− > SeO42−. Electrochemical incorporation of PO43− or NO3− improves activity and stability of TM hydroxides. Conversely, SO42− or SeO42− doping significantly accelerates TM leaching and thus impairs OER performance. Theoretical calculations reveal that electrochemical oxyanion doping simultaneously modulates TM‐O covalency and TM‐3d band centers, correlating with TM stability and OER activity of TM hydroxides. This research constructs an oxyanion‐mediated rule for designing high‐performance electrocatalysts toward energy transformation.

In Situ Electrochemical Oxyanion Steering of Water Oxidation Electrocatalysts for Optimized Activity and Stability

Engineering carbonaceous cathode materials with adequately accessible active sites is crucial for unleashing their charge storage potential. Herein, activated meso-microporous carbon nanofibers are constructed to enhance the zinc ion storage density by forming a gradient-pore structure. A dominating pore size of 0.86 nm is tailored to cater for the solvated [Zn(H2 O)6 ]2+ . Moreover, these gradient porous nanofibers feature rapid ion/electron dual conduction pathways and offer abundant active surfaces with high affinity to electrolyte. When employed in Zn-ion capacitors, the electrode delivers significantly enhanced capacity (257 mAh g-1 ), energy density (200 Wh kg-1 at 78 W kg-1 ), and cyclic stability (95% retention after 10000 cycles) compared to non-activated carbon nanofibers electrode. A series of in-situ characterization techniques unveil that the improved Zn2+ storage capability stems from size compatibility between the pores and [Zn(H2 O)6 ]2+ , the co-adsorption of Zn2+ , H+ , and SO4 2- , as well as reversible surface chemical interaction. This work presents an effective method to engineering meso-microporous carbon materials towards high energy-density storage, and also offers insights into the Zn2+ storage mechanism in such gradient-pore structures. This article is protected by copyright. All rights reserved.

Gradient Pores Enhance Charge Storage Density of Carbonaceous Cathodes for Zn-Ion Capacitor.

The shortage of resources such as lithium and cobalt has promoted the development of novel battery systems with low cost, abundance, high performance, and efficient environmental adaptability. Due to the abundance and low cost of sodium, sodium-ion battery chemistry has drawn worldwide attention in energy storage systems. It is widely considered that wide-temperature tolerance sodium-ion batteries (WT-SIBs) can be rapidly developed due to their unique electrochemical and chemical properties. However, WT-SIBs, especially for their electrode materials and electrolyte systems, still face various challenges in harsh-temperature conditions. In this review, we focus on the achievements, failure mechanisms, fundamental chemistry, and scientific challenges of WT-SIBs. The insights of their design principles, current research, and safety issues are presented. Moreover, the possible future research directions on the battery materials for WT-SIBs are deeply discussed. Progress toward a comprehensive understanding of the emerging chemistry for WT-SIBs comprehensively discussed in this review will accelerate the practical applications of wide-temperature tolerance rechargeable batteries.

Emerging Chemistry for Wide-Temperature Sodium-Ion Batteries.

Introducing anionic redox in layered oxides is an effective approach to breaking the capacity limit of conventional cationic redox. However, the anionic redox reaction generally suffers from excessive oxidation of lattice oxygen to O2 and O2 release, resulting in local structural deterioration and rapid capacity/voltage decay. Here, a Na0.71Li0.22Al0.05Mn0.73O2 (NLAM) cathode material is developed by introducing Al3+ into the transition metal (TM) sites. Thanks to the strong Al–O bonding strength and small Al3+ radius, the TMO2 skeleton and the holistic TM–O bonds in NLAM are comprehensively strengthened, which inhibits the excessive lattice oxygen oxidation. The obtained NLAM exhibits a high reversible capacity of 194.4 mAh g‐1 at 20 mA g‐1 and decent cyclability with 98.6% capacity retention over 200 cycles at 200 mA g−1. In situ characterizations reveal that the NLAM experiences phase transitions with an intermediate OP4 phase during the charge–discharge. Theoretical calculations further confirm that the Al substitution strategy is beneficial for improving the overlap between Mn 3d and O 2p orbitals. This finding sheds light on the design of layered oxide cathodes with highly reversible anionic redox for sodium storage.

Comprehensively Strengthened Metal‐Oxygen Bonds for Reversible Anionic Redox Reaction

Cr-doped Na3V2(PO4)3@C enables high-capacity with V2+/V5+ reaction and stable sodium storage

Hard carbon is generally accepted as the choice of anode material for sodium-ion batteries. However, integrating high capacity, high initial Coulombic efficiency (ICE), and good durability in hard carbon materials remains challenging. Herein, N-doped hard carbon microspheres (NHCMs) with abundant Na+ adsorption sites and tunable interlayer distance are constructed based on the amine-aldehyde condensation reaction using m-phenylenediamine and formaldehyde as the precursors. The optimized NHCM-1400 with a considerable N content (4.64%) demonstrates a high ICE (87%), high reversible capacity with ideal durability (399 mAh g-1 at 30 mA g-1 and 98.5% retention over 120 cycles), and decent rate capability (297 mAh g-1 at 2000 mA g-1 ). In situ characterizations elucidate the adsorption-intercalation-filling sodium storage mechanism of NHCMs. Theoretical calculation reveals that the N-doping decreases the Na+ adsorption energy on hard carbon.

Amine-Aldehyde Condensation-Derived N-Doped Hard Carbon Microspheres for High-Capacity and Robust Sodium Storage.

Hard carbon is a kind of abundant-resource and cost-effective anode material for potassium-ion batteries to realize commercialization shortly. However, the poor rate performance and ambiguous energy storage mechanism of hard carbon remain great bottlenecks. In this study, bagasse-pyrolyzed hard carbon (BC) is prepared by the pyrolysis of bagasse, which exhibits a larger surface area and better electrical conductivity than sugarcane-pyrolyzed hard carbon (SC). The BC exhibits a high reversible capacity of 235 mAh g–1 at 100 mA g–1 and a high rate (161 mAh g–1 at 1000 mA g–1) for K+ storage, which are better than those of SC (108 mAh g–1 and 49 mAh g–1). In situ X-ray diffraction and Raman results reveal the “adsorption–intercalation” K+ storage mechanism and prove that the favorable defects endow BC with better electrochemical capability. 

Bagasse-Derived Hard Carbon Anode with an Adsorption–Intercalation Mechanism for High-Rate Potassium Storage

Kiwi twig biochar recycling promoting the reduction of NO by a MnO2 catalyst

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