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Open Access Review Issue
Regulating Lithium Metal Nucleation and Growth for Dendrite Suppression: From Liquid-Electrolyte to Solid-State Batteries
Journal of Electrochemistry 2025, 31(11)
Published: 12 November 2025
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Lithium metal anodes, with a theoretical capacity of up to 3860 mAh·g−1, are regarded as the cornerstone for developing next-generation high-energy-density batteries. However, several key challenges hinder their practical applications, including dendrite formation, unstable solid electrolyte interphase (SEI), side reactions with electrolytes, and associated safety risks. This review systematically explores the mechanisms of lithium nucleation, growth, and stripping in both liquid and solid-state battery systems, analyzing critical theoretical concepts like heterogeneous nucleation thermodynamics, surface diffusion kinetics, space charge effects, and SEI-induced nucleation, which are crucial for understanding the genesis of dendrite growth. Additionally, the review discusses the electrochemical-mechanical coupling failures that lead to SEI degradation and the formation of dead lithium. For liquid systems, the review proposes strategies to mitigate dendrite formation and SEI instability, which include electrolyte optimization, artificial SEI design, and electrode framework design. In solid-state batteries, the review offers a granular analysis of the interface challenges associated with polymer, sulfide, and halide electrolytes and summarizes different solutions for different solid-state electrolytes. Meanwhile, the review emphasizes the importance of advanced characterization techniques and computational modeling in understanding and regulating the interface between lithium metal and electrolytes. Looking ahead, the review highlights future research directions that emphasize the integration of cross-disciplinary approaches to tackle these interconnected challenges. By addressing these issues, the path will be clear for the rapid commercialization and widespread application of lithium metal batteries, bringing us closer to realizing stable, high-energy-density batteries that can satisfy the escalating demands of modern energy storage applications across various industries.

Review Issue
Li-Rich Mn-Based Layered Oxide Cathodes for Solid-State Rechargeable Batteries
Journal of the Chinese Ceramic Society 2025, 53(6): 1764-1776
Published: 18 May 2025
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Solid-state batteries (SSBs) are a promising next-generation secondary battery due to their potential for high energy density and enhanced safety, offering solutions to the problems inherent in conventional lithium-ion batteries (LIBs) with organic liquid electrolytes (i.e., flammability, corrosion susceptibility, and high-voltage instability). In the construction of SSBs, the selection of the cathode materials is critical to achieving a high energy density, particularly when coupled with lithium metal anodes. However, conventional cathodes often affect the energy density of SSBs due to their constrained specific capacities. It is thus crucial for achieving substantial improvements in the energy density of SSBs to develop high specific capacity cathodes. The Li-rich Mn-based layered oxide (LRMO) is a promising cathode material for SSBs for energy densities of above 600 W·h·kg–1 due to their high discharge specific capacities. Furthermore, LRMO cathodes offer some additional advantages, i.e., reduction of Co and Ni content, leverage of the abundance of Mn to achieve lower materials costs and improved safety. Their application in SSBs also mitigates the dissolution of TM-ions into the electrolyte, thereby enhancing the structural stability and capacity retention during long-term cycling progress. In addition, the resource-efficient composition of LRMO cathodes also align with environmentally friendly and sustainable development goals.

This review represents that the LRMO cathode materials are characterized by a composite crystal structure comprising two key components, i.e., Li2MnO3 phase and LiMO2(M=Mn, Ni, Co) phase. Li2MnO3 phase can be considered as a superlattice-structured variant of LiMO2, formulated as Li[LixMn1-x]O2. This superlattice-structured introduces unique unhybridized O 2p states, arising from Li—O—Li configurations. These unique oxygen states enable the participation of oxygen in charge compensation processes. Consequently, the high capacity in LRMO cathodes is attributed to the synergistic contributions of both TM cations and oxygen redox reactions.

LRMO cathodes, while exhibiting a distinctive biphasic structure, encounter significantly some challenges in SSBs. Specifically, the application of LRMO cathodes in SSBs is hindered by two primary issues. Firstly, the inherent incompatibility between Li2MnO3 phase and SEs interfaces results in sluggish reaction kinetics, severely restricting the activation of oxygen redox activity and consequently reducing the associated capacity contribution. Secondly, a chemical potential mismatch between SEs and LRMO cathodes drives spontaneous reactions at the composite cathode interfaces. These reactions lead to the formation of mixed ionic/electronic conductive CEI. Furthermore, irreversible oxygen escape further oxidizes the SEs interface, generating the passivation layers. These passivation layers increase interfacial impedance and imped ion transport, ultimately hindering practical advancements in SSBs technology.

LRMO cathodes hold a significant promise for SSBs, as evidenced by research progress across various SEs, including sulfides, halides, polymers, and oxides. To fully realize this potential, some strategies addressing the inherent incompatibility between LRMO cathodes and SEs are crucial. These strategies encompass bulk/ interfacial structure design, nanostructured particle engineering, and the construction of stable Li+/e transport pathways. These approaches can suppress oxygen escape, enhance the high-voltage stability of solid-solid interfaces, and ultimately stabilize oxygen redox while optimizing interfacial dynamics. Consequently, the implementation of these strategies leads to a significant enhancement in the electrochemical performance of LRMO-based SSBs.

Summary and prospects

LRMO cathodes have attracted considerable attention for SSBs due to their high discharge specific capacity and energy density. Advancements in SSBs utilizing sulfide, halide, polymer, and oxide SEs demonstrate a potential of LRMO cathodes to overcome limitations currently hindering their industrial applications in liquid electrolyte systems. These limitations include gas evolution, TM dissolution, and voltage decay. However, the practical application of LRMO cathodes in SSBs faces some challenges stemming from their inherent properties, such as poor electronic conductivity attributed to their biphasic structure, sluggish interfacial charge transfer kinetics, oxygen escape, high-voltage interfacial instability, and electrochemical-mechanical degradation. Consequently, a comprehensive understanding of failure mechanisms and the development of advanced modification strategies for LRMO cathodes in SSBs are urgently needed. This necessitates several key research directions. Firstly, optimizing large-scale synthesis techniques for single-crystal LRMO cathodes is crucial, coupled with systematic investigation into their degradation mechanisms within SSBs. Such studies should elucidate the complex interplay of mechanical, electrical, and chemical coupling within SSBs. Secondly, the development of zero-strain LRMO cathodes, designed to maintain structural integrity with minimal volume changes during cycling, can effectively mitigate mechanical stress, suppress crack formation (both intergranular and intragranular), and significantly improve long-term cycling stability. Furthermore, machine learning-driven multiscale modeling offers an effective tool for the rational design of bulk/interfacial structures, facilitating superior compatibility and high-voltage stability at the solid-solid interfaces. Finally, the exploration of high-voltage-tolerant SEs specifically tailored for LRMO cathodes, alongside innovations in scalable fabrication processes for ultrathin electrolyte membranes and electrode films, is essential. The synergistic convergence of materials innovation, interfacial engineering and scalable manufacturing offers a transformative potential for realizing the full capabilities of LRMO cathodes. This convergence is crucial for advancing SSBs toward unprecedented levels of energy density, reliability and sustainability. Specifically, these combined efforts will facilitate the production of large-format batteries at the A·h-level, ultimately enabling the large-scale commercialization of SSBs incorporating LRMO cathodes.

Open Access Review Issue
The shifting technology landscape of electrical energy storage toward carbon neutrality in China
Technology Review for Carbon Neutrality 2025, 1: 9550004
Published: 23 January 2025
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Downloads:884

The strategic deployment of electrical energy storage technologies enables a new power system with higher renewable energy integration and further empowers the whole society’s transition to a green, sustainable, and technologically advanced energy economy. Here we review the shifting landscape of electrical energy storage technologies in China, commenting on the technological advantages, breakthroughs, bottlenecks, and future directions of technologies from ultrashort-term options like flywheels to ultralong-term solutions like hydrogen storage. Levelized cost of those technologies are key in predicting their future deployment, while diversified local energy storage solutions are necessary to accommodate local energy resources and consumption. To promote deployment of electrical energy storage technologies, multi-sectoral policies encompassing innovation policy, regulatory policy, financial incentives, workforce training, as well as locally tailored planning are needed.

Open Access Review Issue
The future of carbon anodes for lithium-ion batteries: The rational regulation of graphite interphase
Carbon Future 2024, 1(3): 9200017
Published: 24 September 2024
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Downloads:3300

Interphase regulation of graphite anodes is indispensable for augmenting the performance of lithium-ion batteries (LIBs). The resulting solid electrolyte interphase (SEI) is crucial in ensuring anode stability, electrolyte compatibility, and efficient charge transfer kinetics, which in turn dictates the cyclability, fast-charging capability, temperature tolerance, and safety of carbon anodes. Continuous research endeavors are deepening our comprehension of the interphasial chemistry, underscoring the imperative to refine the SEI through economically viable and scalable techniques. The ongoing advancement of surface coating techniques involving amorphous carbons or Li-ion conductors, along with electrolyte formulations optimization such as the integration of film-forming additives, has become the cornerstones in regulating the SEI. These innovations are reshaping the landscape of current LIBs by refining the electrode interphase, paving the way to construct more potent and efficient energy storage systems. The relentless drive to optimize the interphase through cutting-edge technologies is central to the future of LIBs, with the ambitious goals of achieving higher energy densities, ensuring safety, and promoting sustainability in energy storage solutions. This review affords a comprehensive overview of the progression in carbon anode development and current status of their industrialization, underscoring the critical role of interphase regulation engineering in advancing the LIB technology.

Open Access Review Issue
Advances on Composite Cathodes for Lithium-Sulfur Batteries
Journal of Electrochemistry 2022, 28(12): 2219013
Published: 16 December 2022
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Downloads:113

Lithium-sulfur (Li-S) batteries are deemed as high-promising next-generation energy storage technique due to their ultrahigh theoretical energy density, where the sulfur cathodes with high specific capacity guarantee the energy density advantage and directly determine the battery performances. After decades of exploration, the most promising sulfur cathodes are sulfur/carbon composite (S/C) cathodes and sulfurized polyacrylonitrile (SPAN) cathodes. In this manuscript, recent advances on S/C and SPAN cathodes in Li-S batteries are comprehensively reviewed. The electrochemical reaction circumstances on S/C and SPAN cathodes are firstly introduced and compared to reveal the working mechanisms of the two types of Li-S batteries. The S/C cathodes mainly undergo solid-liquid-solid multi-phase conversion processes with typical double-plateau charge-discharge polarization curves. In comparison, the SPAN cathodes follow solid-solid conversion and exhibit single-plateau charge-discharge characteristics. Following that, key challenges and targeted optimizing strategies of the S/C and SPAN cathodes are respectively presented and discussed. For Li-S batteries with S/C cathodes, the main optimizing strategies are electrode structure modification, efficient electrocatalyst design, and redox comediation. For SPAN cathodes, the main optimizing strategies are electrode structure modification, morphology regulation by co-polymerization, heteroatom doping at molecular level, and extrinsic redox mediation. At last, current research status of Li-S batteries with S/C or SPAN cathodes are systematically analyzed through the comparison of several battery parameters, and perspectives on challenges and opportunities of S/C and SPAN cathodes in Li-S batteries are presented to guide future researches.

Open Access Review Issue
A perspective on energy chemistry of low-temperature lithium metal batteries
iEnergy 2022, 1(1): 72-81
Published: 25 March 2022
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Downloads:260

Dendrite growth of lithium (Li) metal anode severely hinders its practical application, while the situation becomes more serious at low temperatures due to the sluggish kinetics of Li-ion diffusion. This perspective is intended to clearly understand the energy chemistry of low-temperature Li metal batteries (LMBs). The low-temperature chemistries between LMBs and traditional Li-ion batteries are firstly compared to figure out the features of the low-temperature LMBs. Li deposition behaviors at low temperatures are then discussed concerning the variation in Li-ion diffusion behaviors and solid electrolyte interphase (SEI) features. Subsequently, the strategies to enhance the diffusion kinetics of Li ions and suppress dendrite growth including designing electrolytes and electrode/electrolyte interfaces are analyzed. Finally, conclusions and outlooks are drawn to shed lights on the future design of high-performance low-temperature LMBs.

Open Access Research Article Issue
Quantitative kinetic analysis on oxygen reduction reaction: A perspective
Nano Materials Science 2021, 3(3): 313-318
Published: 28 April 2021
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Oxygen reduction reaction (ORR) constitutes the core process of many energy storage and conversion devices including metal–air batteries and fuel cells. However, the kinetics of ORR is very sluggish and thus high-performance ORR electrocatalysts are highly regarded. Despite recent progress on minimizing the ORR half-wave potential as the current evaluation indicator, in-depth quantitative kinetic analysis on overall ORR electrocatalytic performance remains insufficiently emphasized. In this paper, a quantitative kinetic analysis method is proposed to afford decoupled kinetic information from linear sweep voltammetry profiles on the basis of the Koutecky–Levich equation. Independent parameters regarding exchange current density, electron transfer number, and electrochemical active surface area can be respectively determined following the proposed method. This quantitative kinetic analysis method is expected to promote understanding of the electrocatalytic effect and point out further optimization direction for ORR electrocatalysis.

Open Access Research Article Issue
Seawater-based electrolyte for zinc–air batteries
Green Chemical Engineering 2020, 1(2): 117-123
Published: 28 September 2020
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Aqueous zinc–air batteries (ZABs) are highly regarded as a promising electrochemical energy storage device owing to high energy density, low cost, and intrinsic safety. The employment of seawater to replace the currently used deionized water in electrolyte will bring great economic benefits and broaden the application occasions of ZABs. However, ZABs using seawater-based electrolyte remain uninvestigated without an applicable cathode electrocatalyst or a successful battery prototype. Herein, seawater-based electrolyte is successfully employed in ZABs with satisfactory performances. The influence of chloride anions on the cathode electrocatalytic reactivity and battery performance is systemically investigated. Both noble-metal-based and noble-metal-free electrocatalysts are applicable to the chloride-containing alkaline electrolyte. Further evaluation of ZABs with seawaterbased electrolyte demonstrates comparable battery performances with the conventional electrolyte in terms of polarization, capacity, and rate performance. This study demonstrates a successful prototype of seawater-based ZABs and enlightens the utilization of natural resources for clean and sustainable energy storage.

Research Article Issue
Dendrite-free sandwiched ultrathin lithium metal anode with even lithium plating and stripping behavior
Nano Research 2019, 12(9): 2224-2229
Published: 26 March 2019
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Thin artificial solid electrolyte coatings are effective to enhance the electrochemical performances and safety issues of lithium (Li) metal anode. However, massive and efficient fabrication of artificial protection layers on Li metal anode surface remains challenging. Herein, we describe a sandwiched Li metal anode fabricated through a continuous roll to roll calendering method to implant a thin and large-area carbon layer on Li metal anode surface at room temperature. Specifically, a carbon layer (~ 3 μm in thickness) can be entirely grafted from Cu substrate to 50 μm Li belt surface due to the stickiness of metallic Li. The carbon layer not only plays a critical role in providing rich nucleation sites for Li plating, but more importantly diminishes the metallurgical nonuniformity effects (slip lines) on stripping. Therefore, even Li plating/stripping morphologies are achieved and the as-obtained sandwiched Li/C composite anodes exhibit improved cycling stability both in Li | LiFePO4 and Li | S coin cells and pouch cells. This continuous roll to roll calendering strategy opens a new avenue for grafting various thin artificial protection layers on Li metal surface for safe rechargeable batteries.

Review Article Issue
Review of nanostructured current collectors in lithium–sulfur batteries
Nano Research 2017, 10(12): 4027-4054
Published: 04 July 2017
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Lithium–sulfur (Li–S) batteries are receiving increasing attention because of their high theoretical energy density and the natural abundance of S. However, their practical applications are impeded by the low areal S loading in the cathode and the fatal Li dendrites in the anode of the Li-S cells, which yield an inferior practical energy density and introduce safety concerns, respectively. In this review, we focus on an emerging approach—the nanostructured current collector—to overcome these two critical challenges for Li-S batteries. We describe the general attributes of nanostructured current collectors and examine how these attributes enhance the S utilization with a high S loading and suppress the Li dendrites by regulating the Li-deposition behavior. We present various assembly blocks that have been used for the construction of advanced nanostructured current collectors to build better S cathodes and Li anodes. Finally, we investigate the current challenges and possible solutions regarding the practical applications of nanostructured current collectors in Li-S batteries.

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