Chuan Xiang, Di Xue, Hongyu Liu, Qi Wang, Xingyu Jiang, Cheng Shi, Chi Yan, Jianlong Xu, Zi Wang, Lizhen Huang, Lifeng Chi
{"title":"Organic Photonic Synapses with UV–Vis–NIR Broadband Perception Based on Organic Electrochemical Transistors","authors":"Chuan Xiang, Di Xue, Hongyu Liu, Qi Wang, Xingyu Jiang, Cheng Shi, Chi Yan, Jianlong Xu, Zi Wang, Lizhen Huang, Lifeng Chi","doi":"10.1021/acsami.5c07976","DOIUrl":"https://doi.org/10.1021/acsami.5c07976","url":null,"abstract":"Organic photonic synaptic devices have shown immense potential for emulating the visual perception function of the human retina. In particular, organic electrochemical transistors (OECTs) with photoresponse ability are considered promising choices because of their advantages in low-voltage operation, mechanical flexibility, and biocompatibility. However, current research is limited, and deeper investigations into the materials, devices, and their perception capability are needed. Herein, we introduce a solid-state organic electrochemical transistor based on an organic bulk heterojunction film, which exhibits a broadband response from ultraviolet to near-infrared (365–850 nm) and can simulate fundamental biological synaptic behaviors across multiple wavelengths. Moreover, the device can emulate the learning, forgetting, and relearning processes, as well as the image recognition and memory functions. By employing a trichromatic perception simulation based on convolutional operations, the device successfully achieves image preprocessing capabilities, demonstrating the promising potential of our OECT-based photonic synapses in artificial visual perception systems.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"42 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144229238","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Bin Liu, Yixin Wang, Yikun Ji, Mingjun Zou, Peng Wang, Shujuan Liu, Qian Ye, Feng Zhou
{"title":"Fabrication of Microgel-Functionalized Metal–Organic Framework Composite Polyurethane/Hydrogel Coatings with Enhanced Antifouling Performance","authors":"Bin Liu, Yixin Wang, Yikun Ji, Mingjun Zou, Peng Wang, Shujuan Liu, Qian Ye, Feng Zhou","doi":"10.1021/acsami.5c05228","DOIUrl":"https://doi.org/10.1021/acsami.5c05228","url":null,"abstract":"Antifouling coatings are a key component of marine antifouling strategies, offering a competitive solution to combat biofouling. However, many coatings face significant limitations stemming from insufficient mechanical properties and weak antibacterial performance. Herein, the composite coatings (PMETAC@Ag-MOF/PU/GEL) were prepared by integrating polyurethane/hydrogel (PU/GEL) composites as the polymer matrix and microgel-functionalized metal–organic frameworks (PMETAC@Ag-MOF) as nanofillers. The prepared composite coatings PMETAC@Ag-MOF/PU/GEL combine the excellent mechanical properties of polyurethane with the hydratability of hydrogels and demonstrate enhanced mechanical properties, swelling resistance, and lubrication compared to the original coating. Importantly, it effectively reduces microbial attachment and improves the corrosion resistance of the coating through the slow release of Ag<sup>+</sup>, achieving over 99% bacterial elimination and reducing microalgae attachment by 98%. The improved dispersibility provided by methacryloxyethyltrimethylammonium chloride (METAC) of hydrogels, coupled with the protective film formed by the 2-mercaptobenzothiazole (MBT) of MOFs, significantly improve corrosion resistance of the coating by creating a barrier between the substrate and corrosive environment. Notably, MBT, as a ligand, is incorporated into the structure of MOFs, moderating the release of the antifouling agent and extending the coating’s corrosion resistance over time.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"10 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144229220","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Natalie Munding, Christina Schlagheck, Jochen Wittbrodt, Anthony D. Ho, Yoshinori Takashima, Motomu Tanaka
{"title":"One-Step Surface Functionalization of Hydrogel-Based, Stimulus-Responsive 3D Microstructures for Human Stem Cells","authors":"Natalie Munding, Christina Schlagheck, Jochen Wittbrodt, Anthony D. Ho, Yoshinori Takashima, Motomu Tanaka","doi":"10.1021/acsami.5c08146","DOIUrl":"https://doi.org/10.1021/acsami.5c08146","url":null,"abstract":"To regulate the maintenance and differentiation of stem and progenitor cells, a variety of hydrogels have been developed and applied as two-dimensional (2D) cell culture substrates that can provide well-defined mechanical cues by adjusting the stiffness. Recently, cell-laden hydrogels have been drawing attention as the three-dimensional (3D) cellular environments that can be patterned or printed by extrusion of the cell–polymer mixtures. Hydrogels also serve as 3D microstructures that can stimulate cells both mechanically and geometrically. For flexible, modular functionalization, the coupling of different extracellular matrix (ECM) proteins to side walls and curved surfaces is necessary. However, widely used heterobifunctional photo-cross-linkers encounter a problem because the light cannot reach into the scaffolds uniformly. In this study, we overcame this problem by integrating monomers with <i>N</i>-hydroxysuccinimide (NHS) groups into the copolymer hydrogels with tunable stiffness via careful adjustment of solvent miscibility. This enabled one-step surface functionalization with extracellular matrix proteins such as fibronectin, laminin, and gelatin, replacing photoactivation or laborious multistep functionalization. On the 2D hydrogel substrates functionalized with fibronectin, we found that more than 80% of human mesenchymal stem cells (hMSCs) were viable, and about 60% of them maintained proliferation capacity. These data confirmed that the introduction of NHS monomers caused no cytotoxic effect. We further designed and fabricated 3D microstructures containing various wall and bottom architectures using 3D printed stamps. The uniform functionalization of side walls and bottom surfaces with ECM proteins enabled us to accommodate hMSCs inside the 3D scaffolds, which was in stark contrast to commonly used photo-cross-linkers. The 3D scaffolds showed reversible swelling and deswelling by the addition and removal of soluble guest molecules in the presence of hMSCs, suggesting that the one-step functionalization method established in this study can be applied for a variety of hydrogel-based 3D microstructures for various cell types.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"16 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144218920","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Agnes C. Morrissey, Federica Sbordone, William Sprake, Lukas Michalek, Domenique Ghijzen, Bart van de Worp, Neomy Zaquen, Laura Delafresnaye, Prasanna Egodawatta, Christopher Barner-Kowollik
{"title":"Bioinspired Metal Binding Interfaces for Continuous Metal Removal from Water","authors":"Agnes C. Morrissey, Federica Sbordone, William Sprake, Lukas Michalek, Domenique Ghijzen, Bart van de Worp, Neomy Zaquen, Laura Delafresnaye, Prasanna Egodawatta, Christopher Barner-Kowollik","doi":"10.1021/acsami.5c06671","DOIUrl":"https://doi.org/10.1021/acsami.5c06671","url":null,"abstract":"Herein, we introduce a water flow system that combines adhesion with the selective complexation of metal ions from aqueous solutions, enabling the removal of multiple metal ions from polluted water. Specifically, we utilize a bioinspired polymeric system based on <span>l</span>-3,4-dihydroxyphenylalanine (<span>l</span>-DOPA) carrying a terpyridine functionality that efficiently coats stone wool fibers in a continuous flow coating process, enabling the in-line generation of water purification cartridges. We assess the carefully characterized coated fibers for their metal removal capacities in single metal solutions as well as multi-metal solutions to determine binding affinities via inductively coupled plasma mass spectrometry (ICP-MS). The findings of these studies reveal that chromium (Cr), copper (Cu), and lead (Pb) are adsorbed efficiently by the ligand-coated stone wool fibers. Moreover, we investigated the long-term application of the coated fibers, which displayed no saturation for the removal of Cu over 15 column volumes, making the introduced coating system an excellent candidate for applications in urban stormwater management.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"26 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144218921","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yifan Wu, Ran Wei, Jie Jiang, Ling Ren, Xiaodong Tang, Yu Guo
{"title":"3D-Printed Tantalum Scaffolds Regulates the SDF-1α/CXCR4 Signaling Axis through Spatial Configuration To Enhance the Repair of Osteoporotic Bone Defects","authors":"Yifan Wu, Ran Wei, Jie Jiang, Ling Ren, Xiaodong Tang, Yu Guo","doi":"10.1021/acsami.5c04816","DOIUrl":"https://doi.org/10.1021/acsami.5c04816","url":null,"abstract":"Osteoporosis with large bone defects lacks effective reconstruction methods. Consequently, to improve reconstruction efficiency, a deeper understanding of the molecular mechanisms of osteoporotic bone defect repair is a “bottleneck problem” that needs to be resolved. Via proliferation, adhesion, osteogenic differentiation, and animal experiments, we found that 3D-printed tantalum (Ta) scaffolds could upregulate the expression of TNF-α, an upstream signal of SDF-1α/CXCR4, and that the expression of TNF-α could also differ with changes to the scaffolds’ spatial configuration. Through <i>in vitro</i> and <i>in vivo</i> experiments, this study demonstrated that Ta could upregulate the SDF-1α/CXCR4 signaling pathway through its spatial structure, thereby promoting the repair of osteoporotic bone defects. These research outcomes present an approach for treating osteoporotic bone defects and establish a theoretical foundation for manufacturing 3D-printed Ta prosthetic structures.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"39 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144229219","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Beyza Nur Günaydin, Süleyman Çelik, Selim Tanrıseven, Ali Osman Çetinkaya, Fevzi Çakmak Cebeci, Meral Yüce, Hasan Kurt
{"title":"High-Performance Plasmonic Hafnium Nitride Nanocavity and Nanodisk Arrays for Enhanced Refractometric Sensing","authors":"Beyza Nur Günaydin, Süleyman Çelik, Selim Tanrıseven, Ali Osman Çetinkaya, Fevzi Çakmak Cebeci, Meral Yüce, Hasan Kurt","doi":"10.1021/acsami.5c02241","DOIUrl":"https://doi.org/10.1021/acsami.5c02241","url":null,"abstract":"We report on the deposition and thorough characterization of plasmonic hafnium nitride (HfN) thin films, along with the fabrication of HfN nanocavity and nanodisk arrays for refractometric sensing in the visible–near-infrared (Vis–NIR) range. By optimizing reactive RF magnetron sputtering parameters, we achieved high-quality HfN thin films with tunable properties, confirmed through extensive structural, compositional, and optical analyses: grazing-incidence X-ray diffraction, Raman spectroscopy, X-ray photoelectron spectroscopy, Hall-effect measurements, and variable angle spectroscopic ellipsometry. Our optimized HfN films display a gold-like color with metallic behavior down to ∼360 nm, high free-carrier concentration, and minimal energy losses. Using electron-beam lithography, we patterned HfN nanocavity and nanodisk arrays on fused silica substrates. The nanocavity arrays exhibit a grating-coupled surface plasmon polariton (SPP) tunable by adjusting the lattice periodicity, yielding a bulk refractive index sensitivity of up to 636 nm·RIU<sup>–1</sup> and a figure of merit (FOM) of 17.3. In nanodisk arrays, coupling between LSPR and diffractive orders leads to surface lattice resonances (SLRs), giving rise to narrower spectral line widths and a quality factor exceeding 60. Both array types show significant spectral red-shifts in response to incremental changes in surrounding media refractive indices, demonstrating strong promise for high-performance refractometric sensing. These findings highlight that HfN─a CMOS-compatible, mechanically stable, and cost-effective alternative to noble metals─enables tunable plasmonic devices for biosensing and photonic applications. By bridging a key gap in the exploration of refractory transition metal nitrides, this work emphasizes the potential of HfN in next-generation plasmonic platforms.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"9 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144229215","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Microenvironment-Responsive Xanthotoxol–Copper Nanozyme for MRSA-Infected Wound Healing","authors":"Yinyin Chen, Xinyue Wu, Shiyu Wang, Qiuju Wu, Chen Liang, Wei Fan, Hui Wang, Aimin Wu, Xianxiang Wang","doi":"10.1021/acsami.5c05402","DOIUrl":"https://doi.org/10.1021/acsami.5c05402","url":null,"abstract":"Methicillin-resistant <i>Staphylococcus aureus</i> (<i>MRSA</i>) infections, oxidative stress, and excessive inflammation present significant challenges for wound healing. The natural product xanthotoxol (XT) demonstrates strong antibacterial and anti-inflammatory properties; however, its therapeutic efficacy is limited by poor water solubility. To address this limitation, we have modified XT using polyethylenimine (PEI) to enhance its solubility and have developed a Cu-based composite material, XT-PEI-Cu, which possesses glutathione lyase (GSH-X)-like activity and is specifically designed to respond to the wound microenvironment. During the initial bacterial infection phase, the acidic wound microenvironment activates the glutathione lyase (GSH-X)-like activity of XT-PEI-Cu, significantly depleting bacterial intracellular glutathione (GSH) to achieve potent antibacterial efficacy. As healing progresses to the remodeling phase, the neutralized microenvironment triggers a functional shift, where XT-PEI-Cu scavenges excess reactive oxygen species (ROS) efficiency, polarizes macrophages toward an anti-inflammatory phenotype, reduces the secretion of inflammatory cytokines, and promotes angiogenesis and collagen deposition, thereby facilitating the healing of infected wounds. This study presents a strategy for enhancing the use of natural products in the treatment of <i>MRSA</i>-related wound healing.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"10 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144229237","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xiangwei He, Jianping Xu, Shaobo Shi, Lina Kong, Xiaosong Zhang, Lan Li
{"title":"Enhancing the Performance of Broadband Sb2Se3/Ga2O3 Self-Powered Photodetectors via Modulation of Ga2O3 Surface States and Their Application in All-Day Corona Detection","authors":"Xiangwei He, Jianping Xu, Shaobo Shi, Lina Kong, Xiaosong Zhang, Lan Li","doi":"10.1021/acsami.5c06657","DOIUrl":"https://doi.org/10.1021/acsami.5c06657","url":null,"abstract":"The technology for photodetection and localization of corona discharge typically necessitates the integration of various photodetectors (PDs) with different photoresponse bands and relies on external power supplies. A self-powered PD was fabricated utilizing the Sb<sub>2</sub>Se<sub>3</sub>/Ga<sub>2</sub>O<sub>3</sub> heterojunction, exhibiting a broadband photoresponse from solar-blind ultraviolet (SBUV) to visible (Vis) and near-infrared (NIR) bands. The surface states of Ga<sub>2</sub>O<sub>3</sub> nanorod array (NR) films were modulated by treatment with hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) solution for different periods of time to suppress the interface recombination of photogenerated carriers in type-I heterojunctions. The H<sub>2</sub>O<sub>2</sub> treatment resulted in increased hydroxyl groups (−OH) and decreased oxygen vacancies in Ga<sub>2</sub>O<sub>3</sub> NRs. The −OH can facilitate oxygen molecule (O<sub>2</sub>) adsorption in Ga<sub>2</sub>O<sub>3</sub> NRs and form O<sub>2</sub><sup>–</sup> to consume photogenerated holes to reduce the recombination of photogenerated carriers. However, the decrease of oxygen vacancies will cause a decline in the concentration of electrons in Ga<sub>2</sub>O<sub>3</sub> NRs to hinder the carrier transport. Ultimately, the optimized Al/Sb<sub>2</sub>Se<sub>3</sub>/Ga<sub>2</sub>O<sub>3</sub>/FTO PD, subjected to H<sub>2</sub>O<sub>2</sub> treatment for 4 min, demonstrated responsivities of 3.3, 130, and 180 mA/W under 254, 525, and 850 nm light illumination without applying a bias voltage, respectively. The utilization of oxygen adsorption and desorption processes to regulate the recombination of photogenerated carriers at the interface is an effective strategy for improving the performance of I-type heterojunction self-powered PDs. An approach was conceptually proposed for all-day real-time corona discharge monitoring in high-voltage transmission lines by utilizing the broadband photoresponse characteristic of PDs. The SBUV photoresponse was applied for the capture of SBUV light signals generated by corona discharge. The photoresponse in Vis and NIR light bands was employed to provide background information on corona discharge in both strong light conditions during daytime and weak light conditions during nighttime. The results provide a low power and miniaturized solution for the digitalization of the Power Internet of Things (IoT) and enable real-time monitoring of high-voltage transmission lines.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"331 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144218919","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Dry versus Wet Particle Assembly: Toward Solvent-Free Fabrication","authors":"Ignaas S. M. Jimidar, Kai Sotthewes","doi":"10.1021/acsami.5c05262","DOIUrl":"https://doi.org/10.1021/acsami.5c05262","url":null,"abstract":"For over three decades, the continuous demand for miniaturized devices has prompted scientists to explore the fundamental principles of colloidal or particle (10 nm to 10 μm) assembly to construct large ordered structures. So far, most of the assembly has been performed in wet conditions, i.e., in a solution. Over the past decade, solvent-free (or dry) assembly methods have gained more attention, offering a more sustainable alternative. In this perspective, we highlight the promising aspects of the dry assembly method, which is not only easy to use, rapidly performed, and clean but also abandons the use of solvents while ensuring that the quality of the created particle assembly matches or exceeds that of wet particle assemblies. However, challenges remain for ordered multilayers, binary layers, and nonspherical particle assemblies due to strong surface forces and limited control. Learning from strategies used in wet assembly and gaining a deeper fundamental understanding of surface interactions at the micro- and nanoscale could help bridge these gaps. In this perspective, the challenges and opportunities of dry particle assembly are thoroughly explored, providing a roadmap for advancing the solvent-free assembly field and contributing to a more sustainable world.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"1 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144229236","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ling-Yun Li, Ming-Yuan Shen, Jing-Song Wang, Tao Wu, Wen-Cui Li
{"title":"Mitigating Jahn–Teller Effect of Mn-Based Layered Oxide Cathodes for Sodium-Ion Batteries by Regulation of Coordination Chemistry","authors":"Ling-Yun Li, Ming-Yuan Shen, Jing-Song Wang, Tao Wu, Wen-Cui Li","doi":"10.1021/acsami.5c08162","DOIUrl":"https://doi.org/10.1021/acsami.5c08162","url":null,"abstract":"P2-type Mn-based layered oxide cathode materials are competitive candidates for sodium-ion batteries (SIBs), which are expected to be widely used in large-scale electrochemical energy storage applications due to their easy availability. However, MnO<sub>6</sub> octahedra centered around Mn<sup>3+</sup> are inclined to adverse phase transitions and lattice oxygen loss under high operating voltages, which markedly compromise the capacity and cycling stability. Here, a configurational entropy tuning strategy was proposed to optimize the P2-type Na<sub>0.8</sub>Li<sub>0.17</sub>Mg<sub>0.18</sub>Mn<sub>0.66</sub>O<sub>2</sub> (LMM) cathode. The as-synthesized cathode material, Na<sub>0.8</sub>Li<sub>0.17</sub>Ca<sub>0.025</sub>Mg<sub>0.12</sub>Ni<sub>0.05</sub>Mn<sub>0.66</sub>O<sub>2</sub> (LMCNM), conforms to the standard <i>P</i>63/<i>mmc</i> crystal phase. Impressively, this material exhibits a capacity retention rate of 92% after 100 cycles at a 0.4C rate (where 1C = 125 mA h g<sup>–1</sup>) and demonstrates minimal volume change (0.94%) during charge–discharge cycles at higher working voltages (2.0–4.3 V). In situ X-ray powder diffraction (XRD), ex situ X-ray photoelectron spectroscopy (XPS), and computational analyses collectively indicate that through the charging and discharging processes of LMCNM, there is no obvious Jahn–Teller distortion, while there is clear evidence for charge compensation from Mn<sup>3+</sup> to Mn<sup>4+</sup>. Furthermore, partial reversible anionic redox has been achieved through codoping with Ca and Ni to harmonize expressive stability and high capacity.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"36 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144229240","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}