Yi Feng, Xianwei Lv, Haoyu Wang, Hao Wang, Fengxiao Yan, Lei Wang, Huiying Wang, Jin-Tao Ren, Zhong-Yong Yuan
{"title":"*H Species Regulation of Heterostructured Cu2O/NiO Nanoflowers Boosting Tandem Nitrite Reduction for High-Efficiency Ammonia Production","authors":"Yi Feng, Xianwei Lv, Haoyu Wang, Hao Wang, Fengxiao Yan, Lei Wang, Huiying Wang, Jin-Tao Ren, Zhong-Yong Yuan","doi":"10.1002/adfm.202425687","DOIUrl":"https://doi.org/10.1002/adfm.202425687","url":null,"abstract":"Ambient electrocatalytic reduction of NO<sub>2</sub><sup>−</sup> to NH<sub>3</sub> (NO<sub>2</sub>RR) provides a reliable route for migrating NO<sub>2</sub><sup>−</sup> pollutants and simultaneously generating valuable NH<sub>3.</sub> However, the NO<sub>2</sub>RR involves multistep electron transfer and complex intermediates, rendering the achievement of high NH<sub>3</sub> selectivity a major challenge. In this contribution, heterostructured Cu<sub>2</sub>O/NiO nanoflowers are explored for incorporating the advantages of dual active sites as a highly active and selective NO<sub>2</sub>RR catalyst. Combined theoretical calculations and in situ FTIR/EPR spectroscopy analysis, it is revealed the synergistic effect of Cu<sub>2</sub>O and NiO to promote the NO<sub>2</sub>RR energetics of Cu<sub>2</sub>O/NiO heterostructure electrocatalyst through a tandem catalysis pathway, where Cu<sub>2</sub>O activates the initial absorption and deoxygenation of NO<sub>2</sub><sup>−</sup> for boosting <sup>*</sup>NO formation, while the generated <sup>*</sup>NO on Cu<sub>2</sub>O is then transferred on NiO substrate with abundant active hydrogen for NH<sub>3</sub> conversion. Moreover, the heterostructure formation enhances <sup>*</sup>H retention capacity, promoting <sup>*</sup>H consumed in NO<sub>2</sub>RR and inhibiting inter-<sup>*</sup>H species binding. As a result, Cu<sub>2</sub>O/NiO equipped in a flow cell displays a superior NH<sub>3</sub> yield rate of 128.2 mg h<sup>−1</sup> cm<sup>−2</sup> and Faradaic efficiency of 97.1% at a high current density of −1.25 A cm<sup>−2</sup>. Further, this designed tandem system is proven to be adaptable for other electrochemical NH<sub>3</sub> production reactions including NO<sub>3</sub><sup>−</sup> reduction.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"7 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640942","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}
Jianwei Zheng, Jingwu Zheng, Xinqi Zhang, Pengfei Yue, Wei Cai, Haibo Chen, Liang Qiao, Yao Ying, Jing Yu, Juan Li, Wangchang Li, Shenglei Che
{"title":"Microwave Absorption Properties and Characterization of Porous Permanent/Soft Magnetic Composite Iron Nitride with Heterogeneous Interfaces","authors":"Jianwei Zheng, Jingwu Zheng, Xinqi Zhang, Pengfei Yue, Wei Cai, Haibo Chen, Liang Qiao, Yao Ying, Jing Yu, Juan Li, Wangchang Li, Shenglei Che","doi":"10.1002/adfm.202424988","DOIUrl":"https://doi.org/10.1002/adfm.202424988","url":null,"abstract":"Iron nitride-based composites with different morphologies and magnetic properties are obtained by controlling the nitriding process, thus constructing heterogeneous interfaces conducive to microwave absorption. During the low-temperature nitridation process for synthesizing the permanent magnetic Fe<sub>16</sub>N<sub>2</sub> phase, a stable soft magnetic Fe<sub>4</sub>N phase tends to form on the surface of particles. Consequently, the porous structured Fe<sub>16</sub>N<sub>2</sub>/Fe<sub>4</sub>N composites composed of nano-units are prepared by spray pyrolysis and nitriding processes. The microwave-absorbing mechanisms of permanent/soft magnetic composite iron nitride with porous structure has been elucidated by analyzing the microstructure and electromagnetic properties of samples with varying contents of permanent and soft magnetic materials. The composite of permanent and soft magnetic materials not only creates a heterogeneous interface but also generates a magnetic exchange coupling effect, which improves the impedance matching and increases the interface polarization and dipolar polarization. Eventually, through the coordinated action of excellent dielectric and magnetic loss, good microwave absorption properties are achieved: the minimum reflection loss (RL<sub>min</sub>) is −48.27 dB and the widest effective absorption bandwidth (EAB<sub>max</sub>) is 4.08 GHz with the matching thickness of 1.3 mm. This study provides new insight for further exploration of the application of nano-magnetic materials in the field of microwave absorption.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"6 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640949","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}
Qingjie Guo, Qian Chen, Wei Jiang, Bin Lu, Mingming Tian, Ruobai Liu, Xinyu Chen, Zhuoyi Li, Lulu Cao, Fangyuan Zhu, Wen Zhang, Jun Du, Zhongming Zeng, Jinlan Wang, Zhaocong Huang, Yongbing Xu, Ke Xia, Ya Zhai
{"title":"Deterministic Magnetization Switching with Controllable Chirality in Single Sperimagnetic NiFeTb Layers","authors":"Qingjie Guo, Qian Chen, Wei Jiang, Bin Lu, Mingming Tian, Ruobai Liu, Xinyu Chen, Zhuoyi Li, Lulu Cao, Fangyuan Zhu, Wen Zhang, Jun Du, Zhongming Zeng, Jinlan Wang, Zhaocong Huang, Yongbing Xu, Ke Xia, Ya Zhai","doi":"10.1002/adfm.202503229","DOIUrl":"https://doi.org/10.1002/adfm.202503229","url":null,"abstract":"Field-free magnetization switching with low critical current density is a fundamental pursuit for spin-orbit torque (SOT) devices. Here, a novel strategy is provided that utilizes the sperimagnetism of NiFeTb to achieve current-induced field-free magnetization switching with high efficiency and controllable chirality. The critical current density required for field-free magnetization switching is as low as 2.8 × 10<sup>6</sup> A cm<sup>−2</sup>, an order of magnitude lower than that in conventional heavy metal-based magnetic heterostructures. The ultralow critical current density is attributed to the exceptional soft magnetism, the nucleation-dominant switching characteristic of NiFeTb, and the strong spin Hall effect associated with the large spin-orbital coupling of Tb 4<i>f</i> electrons. Notably, the switching chirality can be designed by manipulating the history of the in-plane magnetic field. The field-free and chirality-controlled magnetization switching in NiFeTb is facilitated by the symmetry-broken sperimagnetic structural arrangement. Utilizing the rich intermediate resistance states and non-volatility of the device, neural network computation is simulated. The findings reveal sperimagnetic rare-earth-transition metal alloys as vital candidates for multifunctional, ultra-low-power storage and computing applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"33 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640978","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}
Idit Goldfracht, Majd Machour, Inbal Michael, Maria Bulatova, Janette Zavin, Shulamit Levenberg
{"title":"3D Bioprinting of Thick Adipose Tissues with Integrated Vascular Hierarchies (Adv. Funct. Mater. 12/2025)","authors":"Idit Goldfracht, Majd Machour, Inbal Michael, Maria Bulatova, Janette Zavin, Shulamit Levenberg","doi":"10.1002/adfm.202570071","DOIUrl":"https://doi.org/10.1002/adfm.202570071","url":null,"abstract":"<p><b>Tissue Engineering</b></p><p>This image illustrates the advanced 3D bioprinting process used to fabricate thick, vascularized adipose tissue constructs. It shows the precise deposition of cell-laden bioinks forming an intricate vascular network within adipose tissue, enabling the creation of perfusable, hierarchical vascular structures for regenerative medicine applications. More details can be found in article number 2410311 by Shulamit Levenberg and co-workers.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"35 12","pages":""},"PeriodicalIF":18.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/adfm.202570071","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143639159","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}
{"title":"Regulating Oxygen Vacancies to Enhance Dipole and Interface Polarization for Highly Efficient Electromagnetic Wave Absorption in SiC@MnO2 Nanocomposites","authors":"Yukun Miao, Anguo Cui, Chang Wang, Zhongning Tian, Ting Wang, Jinyuan Liu, Qianqian Jia, Zhenjiang Li, Meng Zhang","doi":"10.1002/adfm.202503394","DOIUrl":"https://doi.org/10.1002/adfm.202503394","url":null,"abstract":"At present, atomic-scale defect engineering has become a primary strategy for precisely regulating the inherent properties associated with the electronic structure of semiconductors. However, concurrent phenomena and factors during the introduction of defects constrain researchers’ understanding of the correlation between desired defects in various transition metal oxides, electromagnetic parameters, and electromagnetic wave absorption. In this study, MnO<sub>2</sub> nanoneedle arrays are pre-prepared on the surface of SiC nanowire-based carriers via a hydrothermal method, subsequently, oxygen vacancy is successfully introduced into the as-fabricated sample by a simple calcination process. By precisely adjusting the heat-treatment temperature, the oxygen vacancy accumulation-induced in situ phase transformation from MnO<sub>2</sub> to Mn<sub>3</sub>O<sub>4</sub>, creating intrinsic heterointerfaces. Under the synergistic effects of vacancy-induced dipole polarization and interfacial polarization of derived MnO<sub>2</sub>@Mn<sub>3</sub>O<sub>4</sub> heterogenerous interface, the optimal sample exhibits a minimum reflection loss (RL<sub>min</sub>) of −47.96 dB at a matching thickness of 1.90 mm, along with a favorable effective absorption bandwidth (EAB) of 6.40 GHz covering the entire Ku band at a matching thickness of 2.02 mm. This work pionners a defect-driven phase transition strategy to elucidate the relationship between oxygen vacancy concentration, heterostructure interface properties, and EMW absorption capabilities, paving the way for practical application of defect engineering in EMW absorption.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"37 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640976","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}
{"title":"Adaptive Vision Sensor Based on Nonlinear Negative Photoconductivity Behavior","authors":"Chenxing Jin, Jingwen Wang, Wanrong Liu, Yunchao Xu, Xiaofang Shi, Ruihan Li, Jia Sun, Junliang Yang","doi":"10.1002/adfm.202501284","DOIUrl":"https://doi.org/10.1002/adfm.202501284","url":null,"abstract":"In-sensor adaptive visual systems represent a promising technology applicable across various fields. This method significantly enhances image quality while reducing system complexity, thereby holding substantial scientific significance and practical applications. This study emulates a light-triggered depolarization neuromorphic response utilizing an In<sub>2</sub>O<sub>3</sub>/C8-BTBT heterojunction transistor device equipped with ion-gel gating. When the heterojunction device is exposed to UV light, electrons in the In<sub>2</sub>O<sub>3</sub> layer recombine with holes in the C8-BTBT layer, leading to a rapid decrease in photocurrent and resulting in a significant negative photoresponse. The device is capable of simulating spike-dependent inhibitory currents and multilevel storage capabilities. Moreover, the proposed device is employed in constructing a UV-adaptive retina, facilitating in-sensor adaptive computational imaging by leveraging its unique dependence on UV intensity and temporal characteristics, thereby significantly enhancing the visualization of image details.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"40 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640948","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}
{"title":"Out-of-Plane CuSe/WS2 Heterostructure Array as a High-Performance Electrode Material in Ammonium Ion Supercapacitor in Harsh Environment of Extreme Temperature","authors":"Monika Sharma, Shiv Prakash Singh, Pritam Deb","doi":"10.1002/adfm.202424005","DOIUrl":"https://doi.org/10.1002/adfm.202424005","url":null,"abstract":"Ammonium-ion supercapacitor (AISC), being technology innovation for next generation energy storage devices has been limited in practical application. Conventional in-plane structure leads to short circuit and less participated electro-active sites in the redox process. However, out-of-plane heterostructure array provides rapid charge transport across vertically arranged nanoflakes, and forms less heat pockets due to less contact area between vertically arranged ensembles and in-plane nanoflake, making them suitable for advanced energy storage applications. Here, the energy storage performances of AISC based on out-of-plane heterostructure array is studied, which provides large surface area with ample active sites for rapid charge transport at the surfaces of vertically arrayed nanoflakes. The developed electrode material achieves a high specific capacitance of 555.6 F g<sup>−1</sup> and capacitance retention of 82.3% after 5500 cycles. The assembled quasi-solid-state supercapacitor achieves high energy-power densities, and significant capacitance retention after 5000 cycles. The assembled device can illuminate different colored LEDs and power the scientific calculator. Importantly, the developed heterostructure array can dissipate heat and inhibit short circuit due to limited overlap between 2D CuSe ensemble and 2D WS<sub>2</sub> nanoflake. Hence, the device can endure a wide range of temperatures with remarkable energy and power densities even in harsh environments of differential temperatures.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"16 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640947","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}
{"title":"Enabling Long-Life All-Solid-State Sodium Metal Batteries via in situ Construction of a Stable Solid Electrolyte Interphase","authors":"Fangxin Ling, Jiefeng Diao, Yu Yao, Ruilin Bai, Zhen Li, Mingze Ma, Zhiyun Li, Huijuan Huang, Shaolong Zhu, Xianhong Rui, Yu Shao, Graeme Henkelman, Yan Yu","doi":"10.1002/adfm.202419970","DOIUrl":"https://doi.org/10.1002/adfm.202419970","url":null,"abstract":"Suppressing the interface deterioration and sodium dendrites growth is crucial for achieving long-life polyethylene oxide (PEO)-based all-solid-state sodium metal batteries. Herein, we systematically screen Sb<sub>2</sub>S<sub>3</sub> for use as a PEO-based solid-state electrolyte (PSE) additive through theoretical calculations, and in situ construct a highly stable solid electrolyte interphase (SEI) enriched with Na<sub>2</sub>S and Na<sub>3</sub>Sb. This SEI, characterized by its low reduction reaction activity, high ionic conductivity, and strong Na affinity, significantly inhibits interfacial side reactions, accelerates ion transport, and facilitates smooth Na<sup>+</sup> deposition. Moreover, the incorporation of Sb<sub>2</sub>S<sub>3</sub> effectively enhances the mechanical robustness, ionic transference number, and ionic conductivity of the composite solid-state electrolyte film (Sb<sub>2</sub>S<sub>3</sub>@PSE), thereby mitigating the sodium dendrites formation. Consequently, remarkable electrochemical performances for the Sb<sub>2</sub>S<sub>3</sub>@PSE symmetric battery (achieving 5200 h at 0.1 mA cm<sup>−2</sup>, 520 times longer than that of pristine PSE), and the Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub>|Sb<sub>2</sub>S<sub>3</sub>@PSE|Na full battery with high-capacity retention of 91% after 1000 cycles, are demonstrated. This work, which emphasizes the in situ construction of a stable SEI, provides significant guidance to suppress interface degradation for long-life solid-state metal batteries.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"55 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640973","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}
{"title":"Desert Beetle Inspired Heterogeneous Electrode for Large Current Density Hydrogen Evolution Reaction","authors":"Yingjia Sun, Chunhui Zhang, Ziwei Guo, Kesong Liu, Lei Jiang, Cunming Yu","doi":"10.1002/adfm.202425150","DOIUrl":"https://doi.org/10.1002/adfm.202425150","url":null,"abstract":"The hydrogen (H<sub>2</sub>) evolution reaction (HER) is a pivotal process in the production of green H<sub>2</sub>, which will play a crucial role in future sustainable energy systems. Despite extensive efforts to optimize catalyst activity, great challenges related to H<sub>2</sub> mass transfer at the electrode interface still impede the improvement of HER efficiency. Here, a catalytic system inspired is designed by the desert-beetle's hydrophilic/hydrophobic patterned back, a natural structure capable of condensing and transporting fog droplets. This catalytic system is composed of superaerophobic (SAB) electrocatalytic catalyst dots surrounded with superaerophilic (SAL) coating, which can efficiently enhance the gaseous and dissolved H<sub>2</sub> mass transfer to achieve exceptional HER performance. Such a desert beetle-inspired structure using platinum (Pt) as catalyst achieves an excellent current density of HER (−1252 mA cm<sup>−2</sup>) at −0.5 V versus RHE, which is 2 times higher than the conventional Pt electrode (−408.5 mA cm<sup>−2</sup>). The overpotential required to achieve −10 mA cm<sup>−2</sup> is only −7 mV, compared to −25 mV on the conventional electrode. This catalytic system is also applicable to various catalysts (e.g., Re-Co, Co-Cu, Co-Mo, Cu-Mo, and Ni-Mo), which exhibit a minimum 200% current density increase, as compared with their conventional electrode structures.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"24 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640974","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}
Seok Hyun Song, Kyoung Sun Kim, Seokjae Hong, Jong Hyeok Seo, Ji-Hwan Kwon, Minjeong Gong, Jung-Je Woo, Inchul Park, Kyu-Young Park, Dong-Hwa Seo, Chunjoong Kim, Hyeokjun Park, Seung-Ho Yu, Hyungsub Kim
{"title":"Realizing Li Concentration and Particle Size Gradients in Ni-Rich Cathode for Superior Electrochemical Performance in Oxygen-Deficient Atmospheres","authors":"Seok Hyun Song, Kyoung Sun Kim, Seokjae Hong, Jong Hyeok Seo, Ji-Hwan Kwon, Minjeong Gong, Jung-Je Woo, Inchul Park, Kyu-Young Park, Dong-Hwa Seo, Chunjoong Kim, Hyeokjun Park, Seung-Ho Yu, Hyungsub Kim","doi":"10.1002/adfm.202424823","DOIUrl":"https://doi.org/10.1002/adfm.202424823","url":null,"abstract":"To extend the lifespan of Ni-rich layered oxide cathodes, doping, coating, and particle-morphology optimization strategies have been explored, though these approaches often result in reduced reversible capacity. In this study, a novel LiNi<sub>0.92</sub>Co<sub>0.04</sub>Mn<sub>0.04</sub>O<sub>2</sub> cathode is introduced featuring gradients in Li concentration and particle size at the secondary-particle level. By controlling the oxygen partial pressure during synthesis, enhanced cycle stability is achieved without compromising the capacity of this unique structure. Contrary to common knowledge, the superior performance of cathode materials synthesized under oxygen-deficient conditions is reported, delivering a remarkable capacity of 226.7 mAh g<sup>−1</sup> and robust cycle retention of 87.23% after 200 cycles. These electrodes achieve 85.08% capacity retention at 2 C/0.1 C, demonstrating excellent rate performance. Comprehensive diffraction and microscopy analyses identify secondary particles with Li-excess structures on their surfaces (characterized by larger primary particles) and stoichiometric structures in the core (featuring smaller primary particles). This dual-gradient structure enhances performance by suppressing surface reactions and stabilizing the bulk. Furthermore, the electrodes retain pristine microstructure during electrochemical cycling, minimize lattice contraction (3.86%), and suppress H2-to-H3 transitions. This study highlights the potential of using Li concentration gradients to mitigate surface side reactions, paving the way for the development of durable, high-capacity, and cost-effective cathodes.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"327 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640951","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}