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It would be unwise to assume ‘conventional’ lithium-ion batteries are approaching the end of their era and so we discuss current strategies to improve the current and next generation systems, where a holistic approach will be needed to unlock higher energy density while also maintaining lifetime and safety. We end by briefly reviewing areas where fundamental science advances will be needed to enable revolutionary new battery systems.

The 2019 Nobel Prize in Chemistry has been awarded to John B. Goodenough, M. Stanley Whittingham and Akira Yoshino for their contributions in the development of lithium-ion batteries, a technology that has revolutionized our way of life. Here we look back at the milestone discoveries that have shaped the modern lithium-ion batteries for inspirational insights to guide future breakthroughs.

Although the closed pore structure plays a key role in contributing low-voltage plateau capacity of hard carbon anode for sodium-ion batteries, the formation mechanism of closed pores is still under debate. Here, we employ waste wood-derived hard carbon as a template to systematically establish the formation mechanisms of closed pores and their effect on sodium storage performance. We find that the high crystallinity cellulose in nature wood decomposes to long-range carbon layers as the wall of closed pore, and the amorphous component can hinder the graphitization of carbon layer and induce the crispation of long-range carbon layers. The optimized sample demonstrates a high reversible capacity of 430 mAh g −1 at 20 mA g −1 (plateau capacity of 293 mAh g −1 for the second cycle), as well as good rate and stable cycling performances (85.4% after 400 cycles at 500 mA g −1 ). Deep insights into the closed pore formation will greatly forward the rational design of hard carbon anode with high capacity. It is essential to investigate the formation mechanism of closed pore, which contributes to low-voltage plateau capacity of hard carbon anode in sodium ion batteries. Herein, the authors explore the impact of wood precursor components and carbonization temperature on closed pore formation in hard carbon for enhanced battery performance.

In the field of lithium-based batteries, there is often a substantial divide between academic research and industrial market needs. This is in part driven by a lack of peer-reviewed publications from industry. Here we present a non-academic view on applied research in lithium-based batteries to sharpen the focus and help bridge the gap between academic and industrial research. We focus our discussion on key metrics and challenges to be considered when developing new technologies in this industry. We also explore the need to consider various performance aspects in unison when developing a new material/technology. Moreover, we also investigate the suitability of supply chains, sustainability of materials and the impact on system-level cost as factors that need to be accounted for when working on new technologies. With these considerations in mind, we then assess the latest developments in the lithium-based battery industry, providing our views on the challenges and prospects of various technologies. In the field of lithium-based batteries, there is often a divide between academic research and industrial needs. Here, the authors present a view on applied research to help bridge academia and industry, focusing on metrics and challenges to be considered for the development of practical batteries.

The slow redox kinetics of polysulfides and the difficulties in decomposition of Li 2 S during the charge and discharge processes are two serious obstacles to the practical application of lithium-sulfur batteries. Herein, we construct the Fe-Co diatomic catalytic materials supported by hollow carbon spheres to achieve high-efficiency catalysis for the conversion of polysulfides and the decomposition of Li 2 S simultaneously. The Fe atom center is beneficial to accelerate the discharge reaction process, and the Co atom center is favorable for charging process. Theoretical calculations combined with experiments reveal that this excellent bifunctional catalytic activity originates from the diatomic synergy between Fe and Co atom. As a result, the assembled cells exhibit the high rate performance (the discharge specific capacity achieves 688 mAh g −1 at 5 C) and the excellent cycle stability (the capacity decay rate is 0.018% for 1000 cycles at 1 C). The slow redox kinetics of polysulfides and the difficulties in decomposition of Li 2 S are two serious obstacles to lithium-sulfur batteries. Here, the authors report an isolated Fe-Co heteronuclear diatomic catalyst to achieve high efficiency bifunctional catalysis for lithium-sulfur batteries.

Aggressive chemistry involving Li metal anode (LMA) and high-voltage LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NCM811) cathode is deemed as a pragmatic approach to pursue the desperate 400 Wh kg −1 . Yet, their implementation is plagued by low Coulombic efficiency and inferior cycling stability. Herein, we propose an optimally fluorinated linear carboxylic ester (ethyl 3,3,3-trifluoropropanoate, FEP) paired with weakly solvating fluoroethylene carbonate and dissociated lithium salts (LiBF 4 and LiDFOB) to prepare a weakly solvating and dissociated electrolyte. An anion-enrichment interface prompts more anions’ decomposition in the inner Helmholtz plane and higher reduction potential of anions. Consequently, the anion-derived interface chemistry contributes to the compact and columnar-structure Li deposits with a high CE of 98.7% and stable cycling of 4.6 V NCM811 and LiCoO 2 cathode. Accordingly, industrial anode-free pouch cells under harsh testing conditions deliver a high energy of 442.5 Wh kg −1 with 80% capacity retention after 100 cycles. The implementation of Li metal anode with high-voltage Ni/Co rich cathode is plagued by low coulombic efficiency and inferior cycling stability. Here authors propose an anion-enriched interface to facilitate the columnar-structure of Li deposits to solve this issue.

Achieving long-term stable zinc anodes at high currents/capacities remains a great challenge for practical rechargeable zinc-ion batteries. Herein, we report an imprinted gradient zinc electrode that integrates gradient conductivity and hydrophilicity for long-term dendrite-free zinc-ion batteries. The gradient design not only effectively prohibits side reactions between the electrolyte and the zinc anode, but also synergistically optimizes electric field distribution, zinc ion flux and local current density, which induces preferentially deposited zinc in the bottom of the microchannels and suppresses dendrite growth even under high current densities/capacities. As a result, the imprinted gradient zinc anode can be stably cycled for 200 h at a high current density/capacity of 10 mA cm −2 /10 mAh cm −2 , with a high cumulative capacity of 1000 mAh cm −2 , which outperforms the none-gradient counterparts and bare zinc. The imprinted gradient design can be easily scaled up, and a high-performance large-area pouch cell (4*5 cm 2 ) is also demonstrated. Zinc metal anodes suffer from electrolyte corrosion and dendrite growth issues during electrochemical cycling. Here, the authors propose a gradient design to imprint the zinc anode, which both prohibits side reactions and alleviates zinc deposition behaviour.

Li-ion batteries (LIBs) for electric vehicles and aviation demand high energy density, fast charging and a wide operating temperature range, which are virtually impossible because they require electrolytes to simultaneously have high ionic conductivity, low solvation energy and low melting point and form an anion-derived inorganic interphase 1 – 5 . Here we report guidelines for designing such electrolytes by using small-sized solvents with low solvation energy. The tiny solvent in the secondary solvation sheath pulls out the Li + in the primary solvation sheath to form a fast ion-conduction ligand channel to enhance Li + transport, while the small-sized solvent with low solvation energy also allows the anion to enter the first Li + solvation shell to form an inorganic-rich interphase. The electrolyte-design concept is demonstrated by using fluoroacetonitrile (FAN) solvent. The electrolyte of 1.3 M lithium bis(fluorosulfonyl)imide (LiFSI) in FAN exhibits ultrahigh ionic conductivity of 40.3 mS cm −1 at 25 °C and 11.9 mS cm −1 even at −70 °C, thus enabling 4.5-V graphite||LiNi 0.8 Mn 0.1 Co 0.1 O 2 pouch cells (1.2 Ah, 2.85 mAh cm −2 ) to achieve high reversibility (0.62 Ah) when the cells are charged and discharged even at −65 °C. The electrolyte with small-sized solvents enables LIBs to simultaneously achieve high energy density, fast charging and a wide operating temperature range, which is unattainable for the current electrolyte design but is highly desired for extreme LIBs. This mechanism is generalizable and can be expanded to other metal-ion battery electrolytes. An electrolyte design using small-sized fluoroacetonitrile solvents to form a ligand channel produces lithium-ion batteries simultaneously achieving high energy density, fast charging and wide operating temperature range, desirable features for batteries working in extreme conditions.

Structure deterioration and side reaction, which originated from the solvated H 2 O, are the main constraints for the practical deployment of both cathode and anode in aqueous Zn-ion batteries. Here we formulate a weakly solvating electrolyte to reduce the solvating power of H 2 O and strengthen the coordination competitiveness of SO 4 2− to Zn 2+ over H 2 O. Experiment results and theoretical simulations demonstrate that the water-poor solvation structure of Zn 2+ is achieved, which can (i) substantially eliminate solvated-H 2 O-mediated undesirable side reactions on the Zn anode. (ii) boost the desolvation kinetics of Zn 2+ and suppress Zn dendrite growth as well as structure aberration of the cathode. Remarkably, the synergy of these two factors enables long-life full cells including Zn/NaV 3 O 8 ·1.5H 2 O, Zn/MnO 2 and Zn/CoFe(CN) 6 cells. More importantly, practical rechargeable AA-type Zn/NVO cells are assembled, which present a capacity of 101.7 mAh and stability of 96.1% capacity retention after 30 cycles at 0.66 C. The practical deployment of aqueous zinc-ion batteries is hindered by the structure deterioration and side reactions at electrodes. Here, the authors introduce a weakly solvating electrolyte with butanone as an electrolyte additive to stabilize both the cathode and anode of aqueous zinc-ion batteries simultaneously.

The sulfur reduction reaction (SRR) plays a central role in high-capacity lithium sulfur (Li-S) batteries. The SRR involves an intricate, 16-electron conversion process featuring multiple lithium polysulfide intermediates and reaction branches 1 – 3 . Establishing the complex reaction network is essential for rational tailoring of the SRR for improved Li-S batteries, but represents a daunting challenge 4 – 6 . Herein we systematically investigate the electrocatalytic SRR to decipher its network using the nitrogen, sulfur, dual-doped holey graphene framework as a model electrode to understand the role of electrocatalysts in acceleration of conversion kinetics. Combining cyclic voltammetry, in situ Raman spectroscopy and density functional theory calculations, we identify and directly profile the key intermediates (S 8 , Li 2 S 8 , Li 2 S 6 , Li 2 S 4 and Li 2 S) at varying potentials and elucidate their conversion pathways. Li 2 S 4 and Li 2 S 6 were predominantly observed, in which Li 2 S 4 represents the key electrochemical intermediate dictating the overall SRR kinetics. Li 2 S 6 , generated (consumed) through a comproportionation (disproportionation) reaction, does not directly participate in electrochemical reactions but significantly contributes to the polysulfide shuttling process. We found that the nitrogen, sulfur dual-doped holey graphene framework catalyst could help accelerate polysulfide conversion kinetics, leading to faster depletion of soluble lithium polysulfides at higher potential and hence mitigating the polysulfide shuttling effect and boosting output potential. These results highlight the electrocatalytic approach as a promising strategy for tackling the fundamental challenges regarding Li-S batteries. We investigate the mechanism underlying the sulfur reduction reaction that plays a central role in high-capacity lithium sulfur batteries, highlighting the electrocatalytic approach as a promising strategy for tackling the fundamental challenges associated with these batteries.