Pub Date : 2026-10-01Epub Date: 2026-09-11DOI: 10.1016/j.ensm.2026.105525
Taoxiang Qian, Guobin Xu, Shaoyu Hou, Yi Feng, Yaping Wang, Qian Cheng, Guobin Zhang, Shuzhang Niu, Dongju Fu
The rapid growth of electric vehicles has produced huge numbers of spent lithium-ion batteries. As the primary anode material, spent graphite requires urgent recycling to alleviate resource shortage and mitigate environmental risks. This review systematically summarizes recent progress in recycling and high-value utilization of spent graphite anode. We first describe how graphite fails during long time battery operation, typical include particle cracking, solid electrolyte interface damage, lithium dendrites growth, or copper foil corrosion. Next, primary pretreatment processes (safe disassembly, advanced crushing, foam flotation, and chemical leaching) are outlined as essential preliminary engineering steps. Focusing on structural restoration, we critically review direct regeneration technologies, encompassing optimized high-temperature graphitization, chemical remediation, and emerging low-carbon routes such as flash Joule heating, deep eutectic solvent leaching, pre-lithiation, and ultrafast physical heating (microwave). Beyond direct reuse, spent graphite can be upgraded into functional carbon materials for supercapacitors, water cleaning, and catalysts. Finally, we assessed the industrial feasibility of these methods in terms of both production costs and carbon footprint. This work provides comprehensive theoretical guidance for establishing a closed-loop, sustainable graphite recycling system.
{"title":"Spent graphite as a novel resource: Advanced regeneration technologies and life closed-loop sustainability","authors":"Taoxiang Qian, Guobin Xu, Shaoyu Hou, Yi Feng, Yaping Wang, Qian Cheng, Guobin Zhang, Shuzhang Niu, Dongju Fu","doi":"10.1016/j.ensm.2026.105525","DOIUrl":"10.1016/j.ensm.2026.105525","url":null,"abstract":"<div><div>The rapid growth of electric vehicles has produced huge numbers of spent lithium-ion batteries. As the primary anode material, spent graphite requires urgent recycling to alleviate resource shortage and mitigate environmental risks. This review systematically summarizes recent progress in recycling and high-value utilization of spent graphite anode. We first describe how graphite fails during long time battery operation, typical include particle cracking, solid electrolyte interface damage, lithium dendrites growth, or copper foil corrosion. Next, primary pretreatment processes (safe disassembly, advanced crushing, foam flotation, and chemical leaching) are outlined as essential preliminary engineering steps. Focusing on structural restoration, we critically review direct regeneration technologies, encompassing optimized high-temperature graphitization, chemical remediation, and emerging low-carbon routes such as flash Joule heating, deep eutectic solvent leaching, pre-lithiation, and ultrafast physical heating (microwave). Beyond direct reuse, spent graphite can be upgraded into functional carbon materials for supercapacitors, water cleaning, and catalysts. Finally, we assessed the industrial feasibility of these methods in terms of both production costs and carbon footprint. This work provides comprehensive theoretical guidance for establishing a closed-loop, sustainable graphite recycling system.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"91 ","pages":"Article 105525"},"PeriodicalIF":19.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148980541","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lithium nitrate (LiNO3) is a potent interphase-forming salt for Li-metal anodes; however, its low solubility in conventional carbonate solvents has limited its application. Strongly coordinating solvents dissolve LiNO3 but often intensify parasitic reactions with reactive Li metal. Here, we report a LiNO3–N,N-dimethylacetamide (DMAc) synergistically regulated localized high-concentration electrolyte (LNDT) that reconciles salt dissolution with interfacial stability. In LNDT, DMAc enables LiNO3 to serve as the primary lithium salt, while extensive incorporation of NO3- into the Li+ solvation sheath weakens DMAc–Li+ coordination and redirects interfacial reduction from solvent decomposition toward nitrate-derived reactions. This nitrate-rich solvation chemistry generates a gradient inorganic-rich SEI composed of Li3N/LiNxOy, Li2O, and LiF on Li metal, together with an ultrathin, uniform 1.6–1.9 nm CEI on LFP. The resulting dual-interphase stabilization improves Li plating/stripping reversibility, interfacial kinetics, and deposition uniformity. Consequently, Li||LFP cells retain 80.4% of their capacity after 1100 cycles at 1 C and 85.8% after 500 cycles at 3 C, while supporting high-loading LFP cathodes and thin Li-metal anodes. This work establishes a salt–solvent regulation strategy that converts strong solvation from an interfacial liability into an enabler of durable Li-metal batteries.
硝酸锂（LiNO3）是一种有效的锂金属阳极间相形成盐；但其在常规碳酸盐溶剂中的溶解度较低，限制了其应用。强配位溶剂溶解LiNO3，但往往加强寄生反应与活性锂金属。在这里，我们报道了LiNO3-N， n -二甲基乙酰胺（DMAc）协同调节局部高浓度电解质（LNDT），以协调盐溶解和界面稳定性。在LNDT中，DMAc使LiNO3成为主要的锂盐，而NO3-在Li+溶剂化鞘层中的广泛结合削弱了DMAc - Li+配位，并将界面还原从溶剂分解转向硝酸盐衍生反应。这种富硝酸盐的溶剂化化学在锂金属上生成了由Li3N/LiNxOy、Li2O和LiF组成的梯度富无机SEI，并在LFP上生成了超薄、均匀的1.6-1.9 nm CEI。由此产生的双界面稳定提高了锂电镀/剥离的可逆性、界面动力学和沉积均匀性。因此，Li||LFP电池在1℃下循环1100次后保持80.4%的容量，在3℃下循环500次后保持85.8%的容量，同时支持高负载的LFP阴极和薄锂金属阳极。这项工作建立了一种盐溶剂调节策略，将强溶剂化从界面缺陷转化为耐用锂金属电池的推动者。
{"title":"LiNO3–DMAc synergistic regulation of anion-rich solvation for dual-interphase stabilization in Li-metal batteries","authors":"Chaochao Gao, Tiansheng Wang, Juantao Lin, Wanwan Rao, Lin Xie, Jialin Wang, Hao Li, Wen Yu, Mi Wang, Zhenye Zhu, Jiaheng Zhang","doi":"10.1016/j.ensm.2026.105557","DOIUrl":"10.1016/j.ensm.2026.105557","url":null,"abstract":"<div><div>Lithium nitrate (LiNO<sub>3</sub>) is a potent interphase-forming salt for Li-metal anodes; however, its low solubility in conventional carbonate solvents has limited its application. Strongly coordinating solvents dissolve LiNO<sub>3</sub> but often intensify parasitic reactions with reactive Li metal. Here, we report a LiNO<sub>3</sub>–N,N-dimethylacetamide (DMAc) synergistically regulated localized high-concentration electrolyte (LNDT) that reconciles salt dissolution with interfacial stability. In LNDT, DMAc enables LiNO<sub>3</sub> to serve as the primary lithium salt, while extensive incorporation of NO<sub>3</sub><sup>-</sup> into the Li<sup>+</sup> solvation sheath weakens DMAc–Li<sup>+</sup> coordination and redirects interfacial reduction from solvent decomposition toward nitrate-derived reactions. This nitrate-rich solvation chemistry generates a gradient inorganic-rich SEI composed of Li<sub>3</sub>N/LiN<sub>x</sub>O<sub>y</sub>, Li<sub>2</sub>O, and LiF on Li metal, together with an ultrathin, uniform 1.6–1.9 nm CEI on LFP. The resulting dual-interphase stabilization improves Li plating/stripping reversibility, interfacial kinetics, and deposition uniformity. Consequently, Li||LFP cells retain 80.4% of their capacity after 1100 cycles at 1 C and 85.8% after 500 cycles at 3 C, while supporting high-loading LFP cathodes and thin Li-metal anodes. This work establishes a salt–solvent regulation strategy that converts strong solvation from an interfacial liability into an enabler of durable Li-metal batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"91 ","pages":"Article 105557"},"PeriodicalIF":19.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149084622","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nickel-rich layered oxide cathodes are promising for high-energy-density lithium-ion batteries, yet their practical deployment is limited by particle-scale mechanical degradation, particularly intergranular cracking during electrochemical cycling. The complex interplay between particle microstructure, crystallographic characteristics, and chemo-mechanical responses makes it challenging to predict and regulate particle failure. Here, we develop a particle-scale multiphysics framework to interpret intergranular cracking in realistic Ni-rich layered cathode particles, incorporating secondary particle morphologies and crystallographic orientations extracted from electron backscatter diffraction (EBSD). The framework integrates EBSD-resolved particle morphology and crystallographic orientation with orientation-dependent lithium transport, state of charge (SOC)-dependent diffusivity, and phase transition induced lattice evolution. Simulations reveal a transition in lithium-ion transport, from crystallographic orientation-dominated to diffusivity-controlled behavior as charging proceeds. Most intergranular cracks are triggered by abrupt c-axis contraction during the H2-H3 phase transition, further amplified by grain boundary misorientation. The model also captures dynamic crack opening-closure behavior during charging, consistent with in-situ observations. Guided by these insights, an orientation-regulation strategy is proposed to reduce the grain boundary misorientation, decreasing intergranular damage from 17.8 % to 7.1 %. Additionally, regulation of phase-transition behavior, lithium-ion diffusivity, and charging rate within the phase-transition regime provides effective pathways for mitigating intergranular damage, highlighting the critical role of crystallographic characteristics in particle design and operational optimization. This work establishes a mechanism-informed framework linking realistic microstructure, crystallographic characteristics, chemo-mechanical responses, and damage mitigation strategies, providing physical insights for the design of durable Ni-rich cathodes.
{"title":"Chemo-mechanical modeling of crystallographic anisotropy-driven intergranular cracking in realistic Ni-rich cathode particles","authors":"Zhiheng Yao, Ying Chen, Yiming Yao, Weiling Luan, Haofeng Chen","doi":"10.1016/j.ensm.2026.105554","DOIUrl":"10.1016/j.ensm.2026.105554","url":null,"abstract":"<div><div>Nickel-rich layered oxide cathodes are promising for high-energy-density lithium-ion batteries, yet their practical deployment is limited by particle-scale mechanical degradation, particularly intergranular cracking during electrochemical cycling. The complex interplay between particle microstructure, crystallographic characteristics, and chemo-mechanical responses makes it challenging to predict and regulate particle failure. Here, we develop a particle-scale multiphysics framework to interpret intergranular cracking in realistic Ni-rich layered cathode particles, incorporating secondary particle morphologies and crystallographic orientations extracted from electron backscatter diffraction (EBSD). The framework integrates EBSD-resolved particle morphology and crystallographic orientation with orientation-dependent lithium transport, state of charge (SOC)-dependent diffusivity, and phase transition induced lattice evolution. Simulations reveal a transition in lithium-ion transport, from crystallographic orientation-dominated to diffusivity-controlled behavior as charging proceeds. Most intergranular cracks are triggered by abrupt <em>c</em>-axis contraction during the H2-H3 phase transition, further amplified by grain boundary misorientation. The model also captures dynamic crack opening-closure behavior during charging, consistent with in-situ observations. Guided by these insights, an orientation-regulation strategy is proposed to reduce the grain boundary misorientation, decreasing intergranular damage from 17.8 % to 7.1 %. Additionally, regulation of phase-transition behavior, lithium-ion diffusivity, and charging rate within the phase-transition regime provides effective pathways for mitigating intergranular damage, highlighting the critical role of crystallographic characteristics in particle design and operational optimization. This work establishes a mechanism-informed framework linking realistic microstructure, crystallographic characteristics, chemo-mechanical responses, and damage mitigation strategies, providing physical insights for the design of durable Ni-rich cathodes.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"91 ","pages":"Article 105554"},"PeriodicalIF":19.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149084625","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Micro-silicon (μSi) is a promising high-capacity anode material for sulfide solid-state lithium batteries; however, repeated lithiation/delithiation induces severe chemo-mechanical degradation, accompanied by electrode-scale full electrochemical sintering, localized stress concentration, crack propagation, and interfacial contact loss. Herein, we construct a homogeneous organic-inorganic hybrid solid electrolyte interphase (H-SEI) network throughout the μSi electrode to enable confined electrochemical sintering via interphase engineering. Unlike conventional gradient SEI architectures, the interconnected H-SEI network simultaneously integrates high mechanical modulus and is proposed to promote interfacial interactions with both silicon and sulfide solid electrolyte. The homogeneous interphase reduces the formation of high-volume-expansion crystalline Li15Si4, redistributes lithiation-induced stress, and confines electrochemical sintering at the microparticle scale, preventing its propagation across the electrode. Meanwhile, the uniformly distributed organic components maintain intimate and stable Si/LPSCl contact during long-term electrochemical cycling. Benefiting from the synergistic regulation of electrochemical sintering and interfacial stability, the H-SEI-modified μSi electrode delivers a high areal capacity of 2.15 mAh cm-2, ultralong cycling stability over 1400 cycles with an ultralow average capacity decay rate of 0.032% per cycle, and excellent rate capability of 958 mAh g-1 at 8.75 A g-1. This work provides an effective interphase engineering strategy for regulating electrochemical sintering and chemo-mechanical evolution in micro-silicon anodes, offering new insights into the development of durable sulfide solid-state lithium batteries.
微硅（μSi）是一种很有前途的高容量硫化物固态锂电池负极材料；然而，重复的锂化/去硫化会导致严重的化学-机械降解，伴随着电极尺度的全电化学烧结、局部应力集中、裂纹扩展和界面接触损失。在此，我们在μSi电极上构建了一个均匀的有机-无机杂化固体电解质界面（H-SEI）网络，通过界面工程实现了受限电化学烧结。与传统的梯度SEI结构不同，相互连接的H-SEI网络同时集成了高机械模量，并被提议促进与硅和硫化物固体电解质的界面相互作用。均匀的界面相减少了高体积膨胀晶体Li15Si4的形成，重新分配了锂化引起的应力，并将电化学烧结限制在微粒尺度上，阻止了其在电极上的传播。同时，均匀分布的有机组分在长期电化学循环过程中保持了密切稳定的Si/LPSCl接触。得益于电化学烧结和界面稳定性的协同调节，h - sei修饰的μSi电极具有2.15 mAh cm-2的高面积容量，1400次以上的超长循环稳定性，每循环的超低平均容量衰减率为0.032%，在8.75 a g-1时具有958 mAh g-1的优异速率容量。本研究为调控微硅阳极的电化学烧结和化学力学演化提供了一种有效的相间工程策略，为开发耐用硫化物固态锂电池提供了新的见解。
{"title":"Homogeneous solid electrolyte interphase network confines electrochemical sintering toward ultra-stable micro-silicon sulfide solid-state anodes","authors":"Lu Guo, Qian Xu, Xia Hu, Fei Yang, Junshu Sun, Ting Liu, Peng Guo, Junwei Han, Linjie Zhi","doi":"10.1016/j.ensm.2026.105552","DOIUrl":"10.1016/j.ensm.2026.105552","url":null,"abstract":"<div><div>Micro-silicon (μSi) is a promising high-capacity anode material for sulfide solid-state lithium batteries; however, repeated lithiation/delithiation induces severe chemo-mechanical degradation, accompanied by electrode-scale full electrochemical sintering, localized stress concentration, crack propagation, and interfacial contact loss. Herein, we construct a homogeneous organic-inorganic hybrid solid electrolyte interphase (H-SEI) network throughout the μSi electrode to enable confined electrochemical sintering via interphase engineering. Unlike conventional gradient SEI architectures, the interconnected H-SEI network simultaneously integrates high mechanical modulus and is proposed to promote interfacial interactions with both silicon and sulfide solid electrolyte. The homogeneous interphase reduces the formation of high-volume-expansion crystalline Li<sub>15</sub>Si<sub>4</sub>, redistributes lithiation-induced stress, and confines electrochemical sintering at the microparticle scale, preventing its propagation across the electrode. Meanwhile, the uniformly distributed organic components maintain intimate and stable Si/LPSCl contact during long-term electrochemical cycling. Benefiting from the synergistic regulation of electrochemical sintering and interfacial stability, the H-SEI-modified μSi electrode delivers a high areal capacity of 2.15 mAh cm<sup>-2</sup>, ultralong cycling stability over 1400 cycles with an ultralow average capacity decay rate of 0.032% per cycle, and excellent rate capability of 958 mAh g<sup>-1</sup> at 8.75 A g<sup>-1</sup>. This work provides an effective interphase engineering strategy for regulating electrochemical sintering and chemo-mechanical evolution in micro-silicon anodes, offering new insights into the development of durable sulfide solid-state lithium batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"91 ","pages":"Article 105552"},"PeriodicalIF":19.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149085231","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electrolyte solvation structure governs ion transport and interfacial reactions in sodium-ion batteries, yet conventional strategies rely on high salt concentrations to induce anion participation, leading to high cost, increased viscosity, and sluggish kinetics. Here, we propose a coordination-engineered low-concentration electrolyte (CE-LCEs) based on solvation-network regulation to simultaneously enhance transport and interfacial stability. Combined experiments and theoretical calculations reveal the regulatory mechanism of CE-LCEs. Multicomponent ether solvents disrupt molecular ordering, increasing structural disorder and lowering migration activation energy across a wide temperature range. Meanwhile, a weakly solvating ether reconstructs the solvent network, reduces coordination solvent density, and breaks rigid solvation configurations. This regulation transitions the coordination structure from “solvent-dominated coordination” to “anion-participating coordination”. As a result, the electrolyte maintains good fluidity at −50°C and delivers a high ionic conductivity of 2.07 mS cm⁻¹, together with a low migration activation energy and excellent stability from −50 to 60°C. Benefiting from these properties, 1 Ah NFPP||HC pouch cells exhibit outstanding electrochemical performance from −45 to 60°C, achieving 80.34% capacity retention after 2000 cycles at 25°C (2 A), 97.33% retention after 200 cycles at −40°C (0.5 A), and retaining 49.86% of initial capacity (25 °C) even at −50°C.
{"title":"Coordination−engineered low−concentration electrolytes via solvation network regulation for wide temperature high−rate sodium ion pouch batteries","authors":"Haomiao Zhao, Pengyu Li, Gaojing Xia, Pujun Zhang, Shu Zhang, Mengqiang Wu","doi":"10.1016/j.ensm.2026.105519","DOIUrl":"10.1016/j.ensm.2026.105519","url":null,"abstract":"<div><div>Electrolyte solvation structure governs ion transport and interfacial reactions in sodium-ion batteries, yet conventional strategies rely on high salt concentrations to induce anion participation, leading to high cost, increased viscosity, and sluggish kinetics. Here, we propose a coordination-engineered low-concentration electrolyte (CE-LCEs) based on solvation-network regulation to simultaneously enhance transport and interfacial stability. Combined experiments and theoretical calculations reveal the regulatory mechanism of CE-LCEs. Multicomponent ether solvents disrupt molecular ordering, increasing structural disorder and lowering migration activation energy across a wide temperature range. Meanwhile, a weakly solvating ether reconstructs the solvent network, reduces coordination solvent density, and breaks rigid solvation configurations. This regulation transitions the coordination structure from “solvent-dominated coordination” to “anion-participating coordination”. As a result, the electrolyte maintains good fluidity at −50°C and delivers a high ionic conductivity of 2.07 mS cm⁻¹, together with a low migration activation energy and excellent stability from −50 to 60°C. Benefiting from these properties, 1 Ah NFPP||HC pouch cells exhibit outstanding electrochemical performance from −45 to 60°C, achieving 80.34% capacity retention after 2000 cycles at 25°C (2 A), 97.33% retention after 200 cycles at −40°C (0.5 A), and retaining 49.86% of initial capacity (25 °C) even at −50°C.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"91 ","pages":"Article 105519"},"PeriodicalIF":19.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149159499","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-10-01Epub Date: 2026-10-08DOI: 10.1016/j.ensm.2026.105585
Tao Shen, Yile Chang, Mengyu Xie, Xiujing Wen, Zhaoyang Han, Jie Zhang, Linhong Zhuang, Chaoqun Su, Yihan Yang, Jirong Mou, Jishi Wei, Andreu Cabot, Dawei Yang
Lithium-sulfur batteries (LSBs) are promising candidates for next-generation energy storage because of their high theoretical energy density and the natural abundance of sulfur. However, their practical application remains limited by polysulfide shuttling, sluggish sulfur redox kinetics, and kinetic barriers associated with Li2S nucleation and decomposition. Conventional strategies primarily rely on regulating material composition and structure, whereas the dynamic evolution of charge, orbital, and spin states during sulfur conversion has received comparatively less attention. Electromagnetic-field regulation provides an emerging route to directly influence these electronic degrees of freedom and thereby modulate reaction kinetics. This review discusses the fundamental mechanisms by which electric and magnetic fields regulate sulfur redox chemistry in LSBs. Electric-field effects are considered in terms of interfacial charge redistribution, built-in electric fields (BIEFs), ion migration, and field-induced modulation of electronic states, with particular attention to orbital polarization and energy-level changes associated with the Stark effect. Magnetic-field regulation is discussed from the complementary perspectives of mass transport and electronic spin, including magnetohydrodynamic effects, magnetic ordering, spin polarization, and Zeeman-induced changes in electronic states. Representative studies are used to illustrate how these effects influence polysulfide adsorption and conversion, Li+ transport, and Li2S nucleation, growth, and decomposition. Finally, we identify the major challenges in establishing quantitative field-electronic-state-kinetics relationships and highlight opportunities for designing materials with intrinsic electric and magnetic functionalities. This framework provides a basis for moving electromagnetic regulation of LSBs from phenomenological performance enhancement toward mechanistically guided electronic-state engineering.
{"title":"Electromagnetic-field regulation of sulfur redox chemistry in lithium-sulfur batteries: From mass transport to orbital and spin states","authors":"Tao Shen, Yile Chang, Mengyu Xie, Xiujing Wen, Zhaoyang Han, Jie Zhang, Linhong Zhuang, Chaoqun Su, Yihan Yang, Jirong Mou, Jishi Wei, Andreu Cabot, Dawei Yang","doi":"10.1016/j.ensm.2026.105585","DOIUrl":"10.1016/j.ensm.2026.105585","url":null,"abstract":"<div><div>Lithium-sulfur batteries (LSBs) are promising candidates for next-generation energy storage because of their high theoretical energy density and the natural abundance of sulfur. However, their practical application remains limited by polysulfide shuttling, sluggish sulfur redox kinetics, and kinetic barriers associated with Li<sub>2</sub>S nucleation and decomposition. Conventional strategies primarily rely on regulating material composition and structure, whereas the dynamic evolution of charge, orbital, and spin states during sulfur conversion has received comparatively less attention. Electromagnetic-field regulation provides an emerging route to directly influence these electronic degrees of freedom and thereby modulate reaction kinetics. This review discusses the fundamental mechanisms by which electric and magnetic fields regulate sulfur redox chemistry in LSBs. Electric-field effects are considered in terms of interfacial charge redistribution, built-in electric fields (BIEFs), ion migration, and field-induced modulation of electronic states, with particular attention to orbital polarization and energy-level changes associated with the Stark effect. Magnetic-field regulation is discussed from the complementary perspectives of mass transport and electronic spin, including magnetohydrodynamic effects, magnetic ordering, spin polarization, and Zeeman-induced changes in electronic states. Representative studies are used to illustrate how these effects influence polysulfide adsorption and conversion, Li<sup>+</sup> transport, and Li<sub>2</sub>S nucleation, growth, and decomposition. Finally, we identify the major challenges in establishing quantitative field-electronic-state-kinetics relationships and highlight opportunities for designing materials with intrinsic electric and magnetic functionalities. This framework provides a basis for moving electromagnetic regulation of LSBs from phenomenological performance enhancement toward mechanistically guided electronic-state engineering.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"91 ","pages":"Article 105585"},"PeriodicalIF":19.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149150721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Anode-free metal batteries (AFMBs) are promising high-energy-density systems because they remove the initially assembled metal anode and use cathode-derived metal as the only cyclable inventory. This concept has been extended from lithium to sodium, potassium, and zinc batteries, offering opportunities for both high energy density and resource-abundant chemistries. However, their practical development is hindered by low Coulombic efficiency, unstable interfaces, nonuniform metal deposition, and rapid capacity decay. These failures arise from the coupled constraints of zero excess metal inventory, hostless metal deposition, and dynamic interface reconstruction. In this review, we establish a spatiotemporal framework to understand and regulate anode-free metal batteries. The temporal degradation chain is first divided into initial nucleation, repeated plating and stripping, and end-of-life dead metal accumulation. Key descriptors such as nucleation overpotential, metal affinity, ion transport limitation, SEI fracture, tortuosity, and active-metal inventory loss are discussed. Spatial regulation strategies are then summarized according to their dominant functions at different failure stages, including current collector modification, artificial interphase engineering, electrolyte and solvation design, and solid-state electrolyte development. Chemistry-specific challenges across Li, Na, K, and Zn systems are further compared. Finally, practical benchmarking criteria are discussed to guide the transition from materials-level optimization to cell-level design.
{"title":"Spatiotemporal regulation of anode-free metal batteries from lithium to beyond","authors":"Shaolong Zhu, Yubin Feng, Ruilin Bai, Xianhong Rui, Yu Yao, Zhaolin Chen, Yan Yu","doi":"10.1016/j.ensm.2026.105560","DOIUrl":"10.1016/j.ensm.2026.105560","url":null,"abstract":"<div><div>Anode-free metal batteries (AFMBs) are promising high-energy-density systems because they remove the initially assembled metal anode and use cathode-derived metal as the only cyclable inventory. This concept has been extended from lithium to sodium, potassium, and zinc batteries, offering opportunities for both high energy density and resource-abundant chemistries. However, their practical development is hindered by low Coulombic efficiency, unstable interfaces, nonuniform metal deposition, and rapid capacity decay. These failures arise from the coupled constraints of zero excess metal inventory, hostless metal deposition, and dynamic interface reconstruction. In this review, we establish a spatiotemporal framework to understand and regulate anode-free metal batteries. The temporal degradation chain is first divided into initial nucleation, repeated plating and stripping, and end-of-life dead metal accumulation. Key descriptors such as nucleation overpotential, metal affinity, ion transport limitation, SEI fracture, tortuosity, and active-metal inventory loss are discussed. Spatial regulation strategies are then summarized according to their dominant functions at different failure stages, including current collector modification, artificial interphase engineering, electrolyte and solvation design, and solid-state electrolyte development. Chemistry-specific challenges across Li, Na, K, and Zn systems are further compared. Finally, practical benchmarking criteria are discussed to guide the transition from materials-level optimization to cell-level design.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"91 ","pages":"Article 105560"},"PeriodicalIF":19.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149084619","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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