Mahmoud Nabil, Isel Grau, Ricardo Grau-Crespo, Said Hamad, Juan A. Anta
Interpreting the impedance response of perovskite solar cells (PSCs) is challenging due to the complex coupling of ionic and electronic motion. While drift-diffusion (DD) modelling is a reliable method, its mathematical complexity makes directly extracting physical parameters from experimental data infeasible. This work uses DD modelling to generate a large synthetic dataset of impedance spectra for a standard TiO2/MAPI/spiro configuration. This dataset trains machine learning (ML) models to predict recombination and ionic parameters from impedance measurements. A Gradient Boosting Regressor, using features from a generalized equivalent circuit, showed the best performance. Interpretative analysis indicates that open-circuit impedance experiments best probe recombination losses, while short-circuit conditions are more adequate for extracting ionic features like concentrations and mobilities. The trained ML models were tested on experimental spectra, confirming that the inferred physical parameters could reproduce the data. For the studied configuration, predicted ion concentrations were (1.3–3.3) × 1017 cm−3, ion mobilities were (5–7) × 10−11 cm2V−1s−1, and surface recombination velocities were 7–9 and 23–40 ms−1. This approach provides insights into the physical information extractable from impedance measurements and paves the way for ML models to unambiguously derive efficiency-determining parameters for solar cells.
{"title":"Inversion of the Impedance Response Towards Physical Parameter Extraction Using Interpretable Machine Learning","authors":"Mahmoud Nabil, Isel Grau, Ricardo Grau-Crespo, Said Hamad, Juan A. Anta","doi":"10.1002/aenm.202506352","DOIUrl":"https://doi.org/10.1002/aenm.202506352","url":null,"abstract":"Interpreting the impedance response of perovskite solar cells (PSCs) is challenging due to the complex coupling of ionic and electronic motion. While drift-diffusion (DD) modelling is a reliable method, its mathematical complexity makes directly extracting physical parameters from experimental data infeasible. This work uses DD modelling to generate a large synthetic dataset of impedance spectra for a standard TiO<sub>2</sub>/MAPI/spiro configuration. This dataset trains machine learning (ML) models to predict recombination and ionic parameters from impedance measurements. A Gradient Boosting Regressor, using features from a generalized equivalent circuit, showed the best performance. Interpretative analysis indicates that open-circuit impedance experiments best probe recombination losses, while short-circuit conditions are more adequate for extracting ionic features like concentrations and mobilities. The trained ML models were tested on experimental spectra, confirming that the inferred physical parameters could reproduce the data. For the studied configuration, predicted ion concentrations were (1.3–3.3) × 10<sup>1</sup><sup>7</sup> cm<sup>−</sup><sup>3</sup>, ion mobilities were (5–7) × 10<sup>−</sup><sup>1</sup><sup>1</sup> cm<sup>2</sup>V<sup>−</sup><sup>1</sup>s<sup>−</sup><sup>1</sup>, and surface recombination velocities were 7–9 and 23–40 ms<sup>−1</sup>. This approach provides insights into the physical information extractable from impedance measurements and paves the way for ML models to unambiguously derive efficiency-determining parameters for solar cells.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"52 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507676","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}
Efficient and durable solar thermal utilization requires composite phase change materials (CPCMs) that integrate high photothermal efficiency, stable energy storage, and environmental robustness within a scalable architecture. However, most CPCMs rely on energy-intensive processing or carbon-based frameworks, hindering the simultaneous realization of multifunctionality and sustainability. Herein, a series of carbonization-free, interface-engineered bio-based CPCMs are developed by functionalizing the anisotropic microchannel structure of delignified balsa wood with black phosphorene and metal-polyphenol network (tannin-Fe3+). The hybrid interface is further in situ reduced Ag nanoparticles and post-grafted octadecyl chains, creating a robust superhydrophobic surface. Interfacial regulation improves wood-based CPCMs compatibility and stability, delivering a latent heat of ∼175.03 kJ kg−1 with suppressed supercooling. Leveraging directional heat pathways, photothermal–plasmonic coupling, and broadband absorption, the CPCMs achieve a photothermal conversion efficiency of 91.27% and a ∼3.9-fold increase in axial thermal conductivity. The as-prepared CPCMs further integrates flame retardancy, superhydrophobicity, and antimicrobial activity, thereby mitigating dust adhesion and microbial colonization that would otherwise deteriorate the outdoor photothermal performance. As a proof of concept, stable solar–thermal–electric conversion is demonstrated with an output voltage of up to 0.65 V under one-sun irradiation. This work presents a scalable and environmentally friendly wood-based platform for advanced solar thermal energy harvesting.
高效和持久的太阳能热利用需要复合相变材料（CPCMs）在可扩展的架构内集成高光热效率，稳定的能量存储和环境鲁棒性。然而，大多数cpcm依赖于能源密集型加工或碳基框架，阻碍了多功能和可持续性的同时实现。本研究通过黑色磷烯和金属-多酚网络（单宁- fe3 +）功能化去木质素轻木的各向异性微通道结构，开发了一系列无碳化、界面工程的生物基cpcm。杂化界面进一步在原位还原银纳米颗粒和接枝十八烷基链，创造了一个强大的超疏水表面。界面调节提高了木质cpcm的兼容性和稳定性，提供了约175.03 kJ kg - 1的潜热，抑制了过冷。利用定向热通道、光热-等离子体耦合和宽带吸收，cpcm实现了91.27%的光热转换效率和约3.9倍的轴向导热系数。所制备的CPCMs进一步集成了阻燃性、超疏水性和抗菌活性，从而减轻了灰尘粘附和微生物定植，否则会降低室外光热性能。作为概念验证，在一次太阳照射下，稳定的太阳能-热电转换的输出电压高达0.65 V。这项工作为先进的太阳能热能收集提供了一个可扩展和环保的木质平台。
{"title":"Interface-Engineered Wood-Based Composite Phase Change Materials Integrating Superhydrophobic, Flame-Retardant, and Antimicrobial Properties for Sustainable Solar–Electric Energy Conversion","authors":"Yang Meng, Feng Wu, Yuchan Li, Zhe Xiang, Mengyuan Luo, Xinxin Sheng, Delong Xie","doi":"10.1002/aenm.70872","DOIUrl":"https://doi.org/10.1002/aenm.70872","url":null,"abstract":"Efficient and durable solar thermal utilization requires composite phase change materials (CPCMs) that integrate high photothermal efficiency, stable energy storage, and environmental robustness within a scalable architecture. However, most CPCMs rely on energy-intensive processing or carbon-based frameworks, hindering the simultaneous realization of multifunctionality and sustainability. Herein, a series of carbonization-free, interface-engineered bio-based CPCMs are developed by functionalizing the anisotropic microchannel structure of delignified balsa wood with black phosphorene and metal-polyphenol network (tannin-Fe<sup>3+</sup>). The hybrid interface is further in situ reduced Ag nanoparticles and post-grafted octadecyl chains, creating a robust superhydrophobic surface. Interfacial regulation improves wood-based CPCMs compatibility and stability, delivering a latent heat of ∼175.03 kJ kg<sup>−1</sup> with suppressed supercooling. Leveraging directional heat pathways, photothermal–plasmonic coupling, and broadband absorption, the CPCMs achieve a photothermal conversion efficiency of 91.27% and a ∼3.9-fold increase in axial thermal conductivity. The as-prepared CPCMs further integrates flame retardancy, superhydrophobicity, and antimicrobial activity, thereby mitigating dust adhesion and microbial colonization that would otherwise deteriorate the outdoor photothermal performance. As a proof of concept, stable solar–thermal–electric conversion is demonstrated with an output voltage of up to 0.65 V under one-sun irradiation. This work presents a scalable and environmentally friendly wood-based platform for advanced solar thermal energy harvesting.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"47 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507440","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}
Jinpeng Cao, Hang Zhang, Kaifeng Yu, Hongbo Qu, Bo Liu, Qing Wang, Feifei Zhang, Junmin Yan
Neutral zinc-iron flow batteries (ZIFBs) are promising candidates for grid-scale energy storage due to their safety, low cost, and sustainability. However, their cycle stability and energy density are restricted by zinc dendrite growth, hydrogen evolution, and more positive Zn anode potential in neutral media compared to alkaline conditions. Herein, we propose a ligand-coordination strategy using tetrasodium iminodisuccinate (IDs) to rationally tune the redox behavior of Zn2+. The formation of a stable [H4Zn(C8H7NO8)2]2− complex converts the conversional Zn(H2O)62+ structure into a chelate-dominated configuration, inducing an outer-sphere electron transfer pathway by preventing direct Zn-electrode interactions. Meanwhile, it results in a significant negative shift in redox potential of 350 mV (from −0.814 to −1.164 V vs. SHE), enabling a record-high cell voltage of 1.63 V in neutral ZIFBs. The stabilized coordination environment facilitates highly reversible Zn plating/stripping while suppressing hydrogen evolution, dendrite formation and other side reactions. As a result, such high-voltage ZIFB demonstrates a remarkable energy efficiency of 88.77% at 40 mA cm−2 and excellent cycling stability over 320 cycles, advancing durable and high-performance neutral ZIFBs.
中性锌铁液流电池（zifb）因其安全、低成本和可持续性而成为电网规模储能的有希望的候选者。然而，与碱性条件相比，它们的循环稳定性和能量密度受到锌枝晶生长、析氢和中性介质中更正的锌阳极电位的限制。在此，我们提出了一种使用亚氨基二磺酸四钠（IDs）的配位策略来合理调节Zn2+的氧化还原行为。稳定的[H4Zn(C8H7NO8)2]2 -配合物的形成将Zn(H2O)62+结构转化为螯合物主导的构型，通过阻止Zn-电极的直接相互作用诱导了外球电子转移途径。同时，它导致350 mV的氧化还原电位显著负移（与SHE相比，从- 0.814 V变为- 1.164 V），使中性zifb的电池电压达到创纪录的1.63 V。稳定的配位环境有利于高可逆的锌镀/剥离，同时抑制析氢、枝晶形成和其他副反应。因此，这种高压ZIFB在40 mA cm - 2下的能量效率达到了88.77%，并且在320次循环中具有出色的循环稳定性，从而推进了耐用和高性能的中性ZIFB。
{"title":"Chelation Mediated Outer-Sphere Electron Transfer for High-Voltage and Long-Lifespan Neutral Zinc-Iron Flow Batteries","authors":"Jinpeng Cao, Hang Zhang, Kaifeng Yu, Hongbo Qu, Bo Liu, Qing Wang, Feifei Zhang, Junmin Yan","doi":"10.1002/aenm.70849","DOIUrl":"https://doi.org/10.1002/aenm.70849","url":null,"abstract":"Neutral zinc-iron flow batteries (ZIFBs) are promising candidates for grid-scale energy storage due to their safety, low cost, and sustainability. However, their cycle stability and energy density are restricted by zinc dendrite growth, hydrogen evolution, and more positive Zn anode potential in neutral media compared to alkaline conditions. Herein, we propose a ligand-coordination strategy using tetrasodium iminodisuccinate (IDs) to rationally tune the redox behavior of Zn<sup>2+</sup>. The formation of a stable [H<sub>4</sub>Zn(C<sub>8</sub>H<sub>7</sub>NO<sub>8</sub>)<sub>2</sub>]<sup>2−</sup> complex converts the conversional Zn(H<sub>2</sub>O)<sub>6</sub><sup>2+</sup> structure into a chelate-dominated configuration, inducing an outer-sphere electron transfer pathway by preventing direct Zn-electrode interactions. Meanwhile, it results in a significant negative shift in redox potential of 350 mV (from −0.814 to −1.164 V vs. SHE), enabling a record-high cell voltage of 1.63 V in neutral ZIFBs. The stabilized coordination environment facilitates highly reversible Zn plating/stripping while suppressing hydrogen evolution, dendrite formation and other side reactions. As a result, such high-voltage ZIFB demonstrates a remarkable energy efficiency of 88.77% at 40 mA cm<sup>−2</sup> and excellent cycling stability over 320 cycles, advancing durable and high-performance neutral ZIFBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"4 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507677","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}
Jesse J. Hinricher, Katarzyna P. Sokol, Philipp Simons, Kun Joong Kim, Michael Foshey, Yunsheng Tian, Thorben Prein, Lincoln J. Miara, Elsa Olivetti, Wojciech Matusik, Jennifer L. M. Rupp
Global energy demand is projected to grow 30% within the next three decades, driven primarily by population growth and urbanization, leading to greater material needs in energy, and necessitates a new regime of accelerated research via a fundamentally improved strategy. In this perspective, we examine traditional ceramic synthesis methods for high-throughput synthesis and optimization, and highlight requirements and opportunities of synthesis routes for rapid alterations in the future. Such a strategy relies on flexible direct liquid precursor-to-solid film methods rather than traditional, but slower, solid-state methods. Application of computer-aided decision making takes in variables at all levels of fabrication and operates on both material and device characteristics to initialize and optimize the search for higher-performance devices, not just narrow materials optimization. Collectively, we provide a blueprint for accelerated ceramic materials and device improvements of next-generation materials research targeting energy storage.
{"title":"Roadmap for High-Throughput Ceramic Materials Synthesis and Discovery for Batteries","authors":"Jesse J. Hinricher, Katarzyna P. Sokol, Philipp Simons, Kun Joong Kim, Michael Foshey, Yunsheng Tian, Thorben Prein, Lincoln J. Miara, Elsa Olivetti, Wojciech Matusik, Jennifer L. M. Rupp","doi":"10.1002/aenm.202506213","DOIUrl":"https://doi.org/10.1002/aenm.202506213","url":null,"abstract":"Global energy demand is projected to grow 30% within the next three decades, driven primarily by population growth and urbanization, leading to greater material needs in energy, and necessitates a new regime of accelerated research via a fundamentally improved strategy. In this perspective, we examine traditional ceramic synthesis methods for high-throughput synthesis and optimization, and highlight requirements and opportunities of synthesis routes for rapid alterations in the future. Such a strategy relies on flexible direct liquid precursor-to-solid film methods rather than traditional, but slower, solid-state methods. Application of computer-aided decision making takes in variables at all levels of fabrication and operates on both material and device characteristics to initialize and optimize the search for higher-performance devices, not just narrow materials optimization. Collectively, we provide a blueprint for accelerated ceramic materials and device improvements of next-generation materials research targeting energy storage.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"29 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507678","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}
CJ Sturgill, Manish Kumar, Nima Karimitari, Iva Milisavljevic, Coby S. Collins, Aaron Hegler, Hsin-Yun Joy Chao, Santosh Kiran Balijepalli, Scott T. Misture, Christopher Sutton, Morgan Stefik
Wadsley Defects
Wadsley缺陷
{"title":"Role of Wadsley Defects and Cation Disorder to Enhance MoNb12O33 Diffusion (Adv. Energy Mater. 12/2026)","authors":"CJ Sturgill, Manish Kumar, Nima Karimitari, Iva Milisavljevic, Coby S. Collins, Aaron Hegler, Hsin-Yun Joy Chao, Santosh Kiran Balijepalli, Scott T. Misture, Christopher Sutton, Morgan Stefik","doi":"10.1002/aenm.70770","DOIUrl":"https://doi.org/10.1002/aenm.70770","url":null,"abstract":"<b>Wadsley Defects</b>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"4 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507804","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}
Sodium-ion batteries have attracted renewed interest in recent years and are widely studied as a complementary power source to Li-ion batteries for large-scale stationary energy storage and small electric vehicles. Compared with Li-ion batteries, Na-ion batteries offer several advantages, including elemental abundance, lower cost, improved safety, and better low-temperature performance. An in-depth understanding of Na-ion batteries across multiple length and time scales has further accelerated the rapid development of this technology. Among the various advanced characterization techniques used to study Na-ion batteries, neutron scattering has gained significant traction in recent years. It has become a powerful and versatile tool for probing structure, morphology, and sodium-ion dynamics over a wide range of length and time scales. In this article, we will briefly review the development of neutron scattering technology and highlight recent advances in applying neutron-based techniques—including neutron diffraction, total scattering, small-angle scattering, quasi-elastic/inelastic scattering, and neutron imaging—to Na-ion battery materials. We also provide perspectives on future technique developments, particularly in the realm of in situ and operando neutron scattering characterization, and discuss how these approaches could further enhance our understanding of Na-ion battery systems.
{"title":"Neutron Scattering in Sodium-Ion Battery Research: Progress and Prospects","authors":"Jue Liu, Lilin He, Naresh C. Osti, Yuxuang Zhang","doi":"10.1002/aenm.202506774","DOIUrl":"https://doi.org/10.1002/aenm.202506774","url":null,"abstract":"Sodium-ion batteries have attracted renewed interest in recent years and are widely studied as a complementary power source to Li-ion batteries for large-scale stationary energy storage and small electric vehicles. Compared with Li-ion batteries, Na-ion batteries offer several advantages, including elemental abundance, lower cost, improved safety, and better low-temperature performance. An in-depth understanding of Na-ion batteries across multiple length and time scales has further accelerated the rapid development of this technology. Among the various advanced characterization techniques used to study Na-ion batteries, neutron scattering has gained significant traction in recent years. It has become a powerful and versatile tool for probing structure, morphology, and sodium-ion dynamics over a wide range of length and time scales. In this article, we will briefly review the development of neutron scattering technology and highlight recent advances in applying neutron-based techniques—including neutron diffraction, total scattering, small-angle scattering, quasi-elastic/inelastic scattering, and neutron imaging—to Na-ion battery materials. We also provide perspectives on future technique developments, particularly in the realm of in situ and operando neutron scattering characterization, and discuss how these approaches could further enhance our understanding of Na-ion battery systems.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1998 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507679","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}
The decomposition of sulfide-based electrolytes (SEs), notably Li3PS4 (LPS), at the electrode interface during battery cycling significantly hinders their practical application in all-solid-state batteries (ASSBs). However, the underlying mechanism through which chemical bonding modification enhances the electrochemical stability of SEs without compromising other properties remains unclear. Herein, we investigate the effect of introducing highly electronegative elements Q (Q ═ N, O, F) into LPS to strengthen chemical bonds and optimize lithium-ion (Li+) migration pathways in LPSQ electrolytes. Our results reveal that N and O facilitate the formation of PS3Q polyanions, whereas F tends to exist as LiF. All LPSQ systems exhibit an extended electrochemical stability window than pristine LPS, substantially enhancing their compatibility with high-voltage LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes. The strengthened chemical bonding environment further proves beneficial for both electronic and ionic conductivities, leading to superior performance in Li|LPSQ|Li symmetric batteries. Furthermore, by achieving an optimal balance between electronic and ionic conductivity, LPSN enables stable long-term cycling for over 300 cycles at 1C in LiIn||NCM811 full battery, while maintaining high Coulombic efficiency and minimal interfacial degradation. These findings provide guidelines for dopant selection in SE design and offer perspectives on SE engineering aimed at enhancing the high-voltage stability of ASSBs.
{"title":"Highly Electronegative Anions Doping Effects in Sulfide-Based Electrolytes: Toward High-Voltage All-Solid-State Batteries","authors":"Yujun Li, Wei Hao, Xinyang Yue, Tinghu Liu, Tong Duan, Jiangkai Kong, Siyuan Shen, Junjian Zhao, Xiaoya He, Yakun Liu, Zheng Liang, Song Du","doi":"10.1002/aenm.70855","DOIUrl":"https://doi.org/10.1002/aenm.70855","url":null,"abstract":"The decomposition of sulfide-based electrolytes (SEs), notably Li<sub>3</sub>PS<sub>4</sub> (LPS), at the electrode interface during battery cycling significantly hinders their practical application in all-solid-state batteries (ASSBs). However, the underlying mechanism through which chemical bonding modification enhances the electrochemical stability of SEs without compromising other properties remains unclear. Herein, we investigate the effect of introducing highly electronegative elements Q (Q ═ N, O, F) into LPS to strengthen chemical bonds and optimize lithium-ion (Li<sup>+</sup>) migration pathways in LPSQ electrolytes. Our results reveal that N and O facilitate the formation of PS<sub>3</sub>Q polyanions, whereas F tends to exist as LiF. All LPSQ systems exhibit an extended electrochemical stability window than pristine LPS, substantially enhancing their compatibility with high-voltage LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) cathodes. The strengthened chemical bonding environment further proves beneficial for both electronic and ionic conductivities, leading to superior performance in Li|LPSQ|Li symmetric batteries. Furthermore, by achieving an optimal balance between electronic and ionic conductivity, LPSN enables stable long-term cycling for over 300 cycles at 1C in LiIn||NCM811 full battery, while maintaining high Coulombic efficiency and minimal interfacial degradation. These findings provide guidelines for dopant selection in SE design and offer perspectives on SE engineering aimed at enhancing the high-voltage stability of ASSBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"14 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147506965","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}
Layered high-Ni (Ni ≥ 0.9) cathodes are being developed to endure high-voltage operations above 4.5 V for unlocking unprecedented energy density, but they still suffer from exacerbated chemomechanical and electrochemical degradation primarily due to excessive lattice strain, oxygen loss, and phase distortion during prolonged cycling. Herein, we design a high-Ni, Co-free cathode, which features an entropy-assisted core–shell layered/spinel dual-phase, coupled with a Ni-valence gradient framework, via a multi-component complex doping involved co-precipitation strategy. The coherent structural ordering from surface spinel phase to bulk layered phase, driven by the Ni-enriched core/Mn-enriched shell arrangement, and the entropy-assistance and valence-gradient layout, hugely prevents mechanical degradation, surface side-reactions, and oxygen loss, delivering a pseudo strain-free cathode. Thanks to these appealing merits, the cathode breaks through current voltage limitations while maintaining an optimal balance between capacity and sustainability, enabling the stable high-voltage operation up to 4.9 V. Moreover, an exceptional cyclability under strenuous conditions is achieved in practical Ah-level pouch-type cells employing graphite and metallic Li anodes, operating at ultrahigh voltages of 4.65 and 4.8 V, respectively. Besides, the oxygen loss-triggered phase transitions upon heating are markedly delayed. More significantly, our contribution here propels the tremendous advancement of high-Ni, Co-free cathodes to the commercializable levels.
{"title":"Dual-Phase Engineering Coupled With Valence Gradient and Entropy Assistance Unlocking 4.9 V-Tolerant Co-Free High-Ni Cathodes","authors":"Longwei Liang, Yahui Chen, Jiahui Ye, Qingyun Zhang, Hongqiang Xi, Youfeng Tian, Linrui Hou, Changzhou Yuan","doi":"10.1002/aenm.70868","DOIUrl":"https://doi.org/10.1002/aenm.70868","url":null,"abstract":"Layered high-Ni (Ni ≥ 0.9) cathodes are being developed to endure high-voltage operations above 4.5 V for unlocking unprecedented energy density, but they still suffer from exacerbated chemomechanical and electrochemical degradation primarily due to excessive lattice strain, oxygen loss, and phase distortion during prolonged cycling. Herein, we design a high-Ni, Co-free cathode, which features an entropy-assisted core–shell layered/spinel dual-phase, coupled with a Ni-valence gradient framework, via a multi-component complex doping involved co-precipitation strategy. The coherent structural ordering from surface spinel phase to bulk layered phase, driven by the Ni-enriched core/Mn-enriched shell arrangement, and the entropy-assistance and valence-gradient layout, hugely prevents mechanical degradation, surface side-reactions, and oxygen loss, delivering a pseudo strain-free cathode. Thanks to these appealing merits, the cathode breaks through current voltage limitations while maintaining an optimal balance between capacity and sustainability, enabling the stable high-voltage operation up to 4.9 V. Moreover, an exceptional cyclability under strenuous conditions is achieved in practical Ah-level pouch-type cells employing graphite and metallic Li anodes, operating at ultrahigh voltages of 4.65 and 4.8 V, respectively. Besides, the oxygen loss-triggered phase transitions upon heating are markedly delayed. More significantly, our contribution here propels the tremendous advancement of high-Ni, Co-free cathodes to the commercializable levels.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"60 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507081","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}
Ahui Zhu, Ersha Fan, Xiaodong Zhang, Renjie Chen, Li Li
High-value recycling of retired lithium-ion battery materials is pivotal for the circular economy. The nickel-rich strategy, with its merits in boosting energy density, stands out as a key approach for upcycling spent LiNi0.54Co0.16Mn0.3O2 (SNCM). However, the inherent structural defects of SNCM and the heterogeneous reactions among precursors during regeneration jointly induce irreversible phase transformations, preventing the formation of an ideally ordered layered structure. Therefore, we developed a targeted bidirectional anchoring strategy involving pre-anchoring Al species on both SNCM and Ni(OH)2 surfaces. This method reduces the energy barrier for lithiation in the surface-disordered structures of SNCM and suppresses the structural degradation of nickel-rich intermediate phases, thereby addressing the root cause of structural disorder during upcycling. The upcycled cathode material exhibits a stable layered structure and a distinctive nickel concentration gradient from the surface toward the bulk. It delivers outstanding electrochemical performance, including a reversible capacity of 186.84 mAh g−1 at 0.2C and retaining 90.17% of its initial capacity after 200 cycles at 1C, outperforming current commercial materials. Furthermore, this study provides essential insights into solid-state regeneration and establishes a pathway toward the high-value recycling of degraded lithium-ion batteries, demonstrating great potential for practical application.
退役锂离子电池材料的高价值回收是循环经济的关键。富镍策略具有提高能量密度的优点，是升级回收废LiNi0.54Co0.16Mn0.3O2 （SNCM）的关键方法。然而，SNCM固有的结构缺陷和再生过程中前驱体之间的非均相反应共同诱导了不可逆的相变，阻碍了理想有序层状结构的形成。因此，我们开发了一种有针对性的双向锚定策略，包括在SNCM和Ni(OH)2表面预锚定Al物质。该方法降低了SNCM表面无序结构中的锂化能垒，抑制了富镍中间相的结构降解，从而解决了升级回收过程中结构无序的根本原因。升级后的正极材料具有稳定的层状结构和从表面到本体的独特的镍浓度梯度。它具有出色的电化学性能，包括在0.2C时的可逆容量为186.84 mAh g - 1，在1C下循环200次后保持其初始容量的90.17%，优于目前的商用材料。此外，该研究为固态再生提供了重要的见解，并为降解锂离子电池的高价值回收开辟了一条途径，显示了巨大的实际应用潜力。
{"title":"Bidirectional Lattice Anchoring Enhances Composition Reconfiguration of Spent Lithium-Ion Cathodes","authors":"Ahui Zhu, Ersha Fan, Xiaodong Zhang, Renjie Chen, Li Li","doi":"10.1002/aenm.70869","DOIUrl":"https://doi.org/10.1002/aenm.70869","url":null,"abstract":"High-value recycling of retired lithium-ion battery materials is pivotal for the circular economy. The nickel-rich strategy, with its merits in boosting energy density, stands out as a key approach for upcycling spent LiNi<sub>0.54</sub>Co<sub>0.16</sub>Mn<sub>0.3</sub>O<sub>2</sub> (SNCM). However, the inherent structural defects of SNCM and the heterogeneous reactions among precursors during regeneration jointly induce irreversible phase transformations, preventing the formation of an ideally ordered layered structure. Therefore, we developed a targeted bidirectional anchoring strategy involving pre-anchoring Al species on both SNCM and Ni(OH)<sub>2</sub> surfaces. This method reduces the energy barrier for lithiation in the surface-disordered structures of SNCM and suppresses the structural degradation of nickel-rich intermediate phases, thereby addressing the root cause of structural disorder during upcycling. The upcycled cathode material exhibits a stable layered structure and a distinctive nickel concentration gradient from the surface toward the bulk. It delivers outstanding electrochemical performance, including a reversible capacity of 186.84 mAh g<sup>−1</sup> at 0.2C and retaining 90.17% of its initial capacity after 200 cycles at 1C, outperforming current commercial materials. Furthermore, this study provides essential insights into solid-state regeneration and establishes a pathway toward the high-value recycling of degraded lithium-ion batteries, demonstrating great potential for practical application.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"15 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507083","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}
The strong metal-support interactions (SMSI) between supported clusters and substrate can drive the local structure reconstructions, which stabilize the supported clusters to avoid migration and aggregation. Such reconstruction and stabilization mechanism are crucial to construct the atomically dispersed catalysts (ADCs), but they are too complex to simulate in most catalyst theoretical studies for a relative long time. Herein, an accurate machine learning potential (MLP) is employed into Monte Carlo simulation on the MnN (1 ≤ N ≤ 7) clusters supported on MoS2 layer. The adsorption, reconstruction and thermodynamic and kinetical stabilization of Mn clusters on perfect and defective MoS2 are compared studied. The results indicate that the S vacancies can effectively anchor Mn clusters and are feasible to control the dual-atom catalysts (DACs) on the MoS2 surface. Besides, Comparative analysis reveals that the Mn2@MoS2-S2V exhibits superior NH3-SCR catalytic activity. The complete reaction process of Mn2@MoS2-S2V following the “Fast-SCR” mechanism and the NO2 reduction pathway is the dominant route, with a rate-determining barrier of 1.03 eV. This work provides a pioneer way to disclose the very complex reconstruction of supported clusters with SMSI in simulation, which is indeed helpful to design real atomic structure of ADCs.
{"title":"The Reconstruction Mechanism and NH3-SCR Kinetics of Mn Clusters on MoS2 by Ab Initio Data Driven Machine Learning Simulations","authors":"Ziyi Wang, Luneng Zhao, Yuan Chang, Chunqiang Zhuang, Hongsheng Liu, Jiaxu Liu, Tao Liu, Junfeng Gao","doi":"10.1002/aenm.70851","DOIUrl":"https://doi.org/10.1002/aenm.70851","url":null,"abstract":"The strong metal-support interactions (SMSI) between supported clusters and substrate can drive the local structure reconstructions, which stabilize the supported clusters to avoid migration and aggregation. Such reconstruction and stabilization mechanism are crucial to construct the atomically dispersed catalysts (ADCs), but they are too complex to simulate in most catalyst theoretical studies for a relative long time. Herein, an accurate machine learning potential (MLP) is employed into Monte Carlo simulation on the Mn<i><sub>N</sub></i> (1 ≤ <i>N</i> ≤ 7) clusters supported on MoS<sub>2</sub> layer. The adsorption, reconstruction and thermodynamic and kinetical stabilization of Mn clusters on perfect and defective MoS<sub>2</sub> are compared studied. The results indicate that the S vacancies can effectively anchor Mn clusters and are feasible to control the dual-atom catalysts (DACs) on the MoS<sub>2</sub> surface. Besides, Comparative analysis reveals that the Mn<sub>2</sub>@MoS<sub>2</sub>-S<sub>2</sub>V exhibits superior NH<sub>3</sub>-SCR catalytic activity. The complete reaction process of Mn<sub>2</sub>@MoS<sub>2</sub>-S<sub>2</sub>V following the “Fast-SCR” mechanism and the NO<sub>2</sub> reduction pathway is the dominant route, with a rate-determining barrier of 1.03 eV. This work provides a pioneer way to disclose the very complex reconstruction of supported clusters with SMSI in simulation, which is indeed helpful to design real atomic structure of ADCs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"476 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507084","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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