Jiachengjun Luo, Hushan Chand, Rafael Luque, Alina M. Balu, Gianvito Vilé
{"title":"Structured, Shaped, or Printed Single-Atom Catalysts and Their Applications","authors":"Jiachengjun Luo, Hushan Chand, Rafael Luque, Alina M. Balu, Gianvito Vilé","doi":"10.1002/adfm.202424514","DOIUrl":"https://doi.org/10.1002/adfm.202424514","url":null,"abstract":"Structured catalysts, characterized by continuous, highly porous architectures, have long been recognized for their ability to enhance thermal stability, mechanical robustness, and operational efficiency in catalytic processes. Nevertheless, the use of single-atom catalysts (SACs), renowned for their exceptional atomic efficiency, in structured, shaped, or printed forms remains an emerging challenge, primarily due to the difficulties in maintaining atomic dispersion and ensuring stability under processing and reaction conditions. This review explores recent developments in the design and use of structured single-atom catalysts (collectively referred to as stru-SACs herein), focusing on their unique properties and the potential benefits of combining the atomic precision of SACs with engineered architectures. The composition of structured supports, ranging from traditional materials, such as ceramics and metals, to advanced materials, such as graphene, carbon, and aerogels, are examined. Additionally, functional active sites, innovative fabrication strategies, and advanced characterization techniques required to probe the atomic-scale environments of stru-SACs are discussed. The applications of stru-SACs are reviewed across thermocatalysis, photocatalysis, and electrocatalysis, with an emphasis on how the electronic and structural characteristics of these materials enhance the catalytic performance. Finally, current challenges and future perspectives of stru-SACs are outlined.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"131 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133682","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":"Chelated Linkage and Framework Isomerism Effect Toward Robust Zn‐Salen MCOFs for Dual‐Channel Overall H2O2 Photosynthesis","authors":"Yue Chen, Tao Yang, Yaowei Jin, Jiaxin Li, Junlin Gu, Xiaojing Sun, Yingying Zou, Rui Liu, Guangfeng Wei, Chengzhong Yu, Aiguo Kong","doi":"10.1002/adfm.202508520","DOIUrl":"https://doi.org/10.1002/adfm.202508520","url":null,"abstract":"It remains challenging to synthesize effective and photocorrosion‐tolerated organic photocatalysts for two‐electron oxygen reduction reaction (2e⁻ ORR) and water oxidation reaction (2e⁻ WOR). Herein, two isomeric Zn‐Salen metal covalent organic frameworks (Zn‐Salen‐MCOFs) with kgd‐v or hcb topology are designed as robust and efficient photocatalysts for dual‐channel H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub> photosynthesis. Zn‐Salen‐MCOF with kgd‐v topology shows a higher H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub> photocatalytic production rate of 6617/3438 µmol gcat.<jats:sup>−1</jats:sup> h<jats:sup>−1</jats:sup> in pure water with/without additional O<jats:sub>2</jats:sub> or air saturation, together with long‐time continuous H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub> photosynthesis performance (100 h). The framework isomerism effect and the chelated linkages contribute to the improved H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub> photosynthesis efficiency and stability of it. A three‐step 2e⁻ WOR with the initial H<jats:sub>2</jats:sub>O adsorption over the ZnO<jats:sub>2</jats:sub>N<jats:sub>2</jats:sub> unit and a four‐step 2e⁻ ORR reaction mechanism with the key H<jats:sub>ad</jats:sub> adsorption at the pyrazinic N site are proposed. This study paves the way for developing robust MCOF‐based photocatalysts for dual‐channel H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub> production based on chelated linkage and framework isomerism effect.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"49 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133480","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":"Understanding Voltage Decay and Hysteresis in Li‐Rich Layered Oxide Cathodes","authors":"Hongfei Zheng, Liguang Wang, Jun Lu","doi":"10.1002/adfm.202503578","DOIUrl":"https://doi.org/10.1002/adfm.202503578","url":null,"abstract":"Li‐rich layered oxide cathodes (LLOs) with anionic redox are promising to boost the energy density of lithium batteries beyond 500 Wh kg<jats:sup>−1</jats:sup>. However, their commercialization has long been hampered by inherent drawbacks, particularly voltage decay and hysteresis, which reduce energy density and efficiency, shorten battery life, and challenge battery management. To address these issues, a prerequisite is establishing a comprehensive understanding of voltage‐related phenomena correlated with anionic redox reactions (ARR), which remains elusive despite extensive research. Therefore, in this review, the proposed mechanisms are systematically summarized and the fundamental origins of voltage decay and hysteresis are identified, together with elucidating their relationship with ARR. Voltage decay is mainly attributed to irreversible TM migration and phase transition, whose driving force involves factors like lattice strain accumulation and oxygen loss. A relatively unified theory, the asymmetric non‐equilibrium reaction path during ARR, is identified as the fundamental origin of voltage hysteresis. This path includes sequential electrochemical reactions and chemical processes (sluggish electronic and atomic structural rearrangements, such as TM migration and ligand‐to‐metal charge transfer). Recent achievements and effective solutions for these voltage issues are also elaborated. After deeply understanding voltage decay and hysteresis, inspiring insights for mitigation strategies and forward‐looking remarks are provided.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"18 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133546","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}
Lujiao Wang, Song Yang, Tao Zhou, Siyu Yang, Pengyu Bi, Jiangyi Zhou, Qi Wang, Hai Qiao
{"title":"n‐Butanol Enables OMVs as Heat‐Responsive Nanometer Ultrasound Contrast Agents for Tumor Imaging","authors":"Lujiao Wang, Song Yang, Tao Zhou, Siyu Yang, Pengyu Bi, Jiangyi Zhou, Qi Wang, Hai Qiao","doi":"10.1002/adfm.202505161","DOIUrl":"https://doi.org/10.1002/adfm.202505161","url":null,"abstract":"Extracellular vesicles, such as <jats:italic>Escherichia coli</jats:italic> outer membrane vesicles (OMVs), have been widely explored as carriers for contrast agents, yet their application in ultrasound imaging remains limited. In this study, heat‐responsive nB‐OMVs are developed by loading n‐butanol into OMVs (nB‐OMVs). Upon heating, the decreased solubility of n‐butanol triggered phase separation within the vesicles, resulting in enhanced ultrasound signals, including fundamental, harmonic, and subharmonic components. Experimental results demonstrated that nB‐OMVs retained the native morphology of OMVs, along with their tumor‐targeting accumulation and tumor growth inhibition capabilities. nB‐OMVs injection induces red blood cell extravasation into tumors, under near‐infrared (NIR) irradiation, these extravasated RBCs acted as photothermal mediators, generating a localized thermal environment that activated intratumoral nB‐OMVs and further amplified the ultrasound signal. In B‐mode and contrast‐enhanced ultrasound (CEUS) imaging, tumor grayscale intensities increased by 4.6‐ and 8.5‐fold, respectively. This work provides a promising strategy for ultrasound‐based tumor imaging using extracellular vesicles.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"9 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133498","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":"Multipath Synergistic Immune Activation of Hydrogels Delivering STING Agonist and siXkr8 for Long‐Lasting Colorectal Cancer Therapy","authors":"Ning Yang, Xiaolong Feng, Lixuan Yin, Hongjie Bi, Zirang Fu, Xinyue Shao, Zongyan He, Yutong Wang, Tian Zhang, Yiran Liu, Jiazhen Hou, Yuanchao Xie, Tianqun Lang","doi":"10.1002/adfm.202506362","DOIUrl":"https://doi.org/10.1002/adfm.202506362","url":null,"abstract":"Colorectal cancer (CRC) poses a significant threat to global public health, and immunotherapy has emerged as a promising alternative to its treatment. Nevertheless, owing to the tumor immunosuppressive microenvironment (TIME), the efficacy of single‐agent immunotherapy remains limited. Herein, CSZ@Gel is designed by co‐loading cyclic diguanosine (CDG) and siXkr8 in zeolitic imidazolate framework‐8 (ZIF‐8) nanoparticles and subsequently integrating them into α‐tocopherol polyethylene glycol succinate (TPGS) hydrogels. ZIF‐8 is found to undergo degradation under acidic conditions releasing its cargo and Zn<jats:sup>2+</jats:sup> to induce cell pyroptosis. CDG triggers the activation of the stimulator of interferon genes (STING) pathway, leading to enhanced release of proinflammatory cytokines release, dendritic cell (DC) maturation and CD8<jats:sup>+</jats:sup> T cell infiltration. siXkr8 inhibits the expression of scramblase mXkr8 and decreases the phosphatidylserine translocation to the cell surface, thus decreasing immature DCs and regulatory T cells (Tregs) and reversing TIME. In a murine CRC model, CSZ@Gel exhibits significant tumor growth suppression effects, extends the median survival time of mice to more than 60 days, and significantly inhibits CRC recurrence after resection by long‐term synergistic anti‐tumor immune activation. These findings suggest that CSZ@Gel provides an innovative drug delivery platform with clinical translation potential through comprehensive strategies for sustained CRC immunotherapy.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"39 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133507","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}
Lei Wang, Mengqiu Huang, Longjun Rao, Yuetong Qian, Zhikai Yan, Xue He, Wenbin You, Renchao Che
{"title":"Atomically Polarization Regulation in Molybdenum Disulfide Nanosheets via Phase Transition Engineering for Superior Electromagnetic Wave Dissipation","authors":"Lei Wang, Mengqiu Huang, Longjun Rao, Yuetong Qian, Zhikai Yan, Xue He, Wenbin You, Renchao Che","doi":"10.1002/adfm.202507569","DOIUrl":"https://doi.org/10.1002/adfm.202507569","url":null,"abstract":"Disentangling the limitations of dipole activity at the atomic scale in the dielectric materials is key to boosting the intrinsic polarization ability and electromagnetic (EM) energy dissipation. Herein, an atomic structure regulation in molybdenum disulfide (MoS<jats:sub>2</jats:sub>) nanosheets (NSs) connected by multi‐wall carbon nanotubes (MoS<jats:sub>2</jats:sub>‐MWCNTs) is studied to explore the correlation between the local atomic structure and polarization properties at the atomic scale. Induced by the phase transition engineering, 1T‐phase dominated MoS<jats:sub>2</jats:sub> NSs with centrosymmetric D3d point groups are evolved from the 2H‐phase structure. Atomic‐scale and visualized electric field distribution in the MoS<jats:sub>2</jats:sub> NSs are verified by the advanced integrated differential phase contrast technology and related scanning transmission electron microscopy (iDPC‐STEM) imaging. Periodic atomic structure in the 1T‐phase MoS<jats:sub>2</jats:sub> is constructed to enhance symmetrical electric field distribution and those phase interlaced regions promoted a significant increase in dielectric relaxation. Benefiting the boosted dielectric ability and polarization behaviors, 1T‐phase dominated MoS<jats:sub>2</jats:sub>@MWCNTs (TMC) exhibit superior EM wave energy dissipation with the minimum reflection loss (RL<jats:sub>min</jats:sub>) value of −74.3 dB at only 1.7 mm thickness. Changes in atomic structure and electric field study in the MoS<jats:sub>2</jats:sub> NSs help to further elucidate their polarization mechanism and to explore the for studying the mixed‐phase 2D functional nanosheets.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"135 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133508","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}
Jiawei Zhu, Xiaorui Wang, Runtao Li, Tian Zhang, Lei An, Xuejiao Song, Xiaochen Dong, Yu Cai
{"title":"Lymphocyte‐Mimicking Sonosensitizers Boost Cancer Immunotherapy via Sequential Ultrasound Activation","authors":"Jiawei Zhu, Xiaorui Wang, Runtao Li, Tian Zhang, Lei An, Xuejiao Song, Xiaochen Dong, Yu Cai","doi":"10.1002/adfm.202509057","DOIUrl":"https://doi.org/10.1002/adfm.202509057","url":null,"abstract":"Effective initiation of the cancer‐immunity cycle is the core challenge of tumor immunotherapy, which relies on the coordinated antigen release and immunostimulation. To address this issue, this work introduced a novel lymphocyte‐mimicking sonosensitizer using Mn‐doped hollow Prussian blue nanoparticle (Mn‐HP) for cancer sonodynamic therapy (SDT) to efficiently evoke anticancer immunity. The prepared Mn‐HP have unique architecture to amplify ultrasonic cavitation effects, boosting spatially controlled reactive oxygen species (ROS) production. Through the effective combination of the Mn‐HP and lymphocytes, the Lymphocyte‐mimicking sonosensitizer (Lymphocytes‐Mn‐HP, LM) with the “Homing effect” is constructed. The sequenced dual‐ultrasound strategy employs high‐power ultrasound (2.0 W cm<jats:sup>−2</jats:sup>) stimulation (excessive ROS) for tumor antigen release and low‐power ultrasound (0.5 W cm<jats:sup>−2</jats:sup>) stimulation (moderate ROS) for lymph node to active immune cells, enabling precise spatial‐temporal controlled ROS generation while preserving immune function. Both in vitro and in vivo studies demonstrated significant tumor suppression through initiating the cancer‐immunity cycle, offering a transformative paradigm for SDT‐immunotherapy integration.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"34 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133509","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":"High‐Areal‐Capacity Manganese‐Based Redox Flow Batteries via Sodium Diphosphate‐Modified Electrolyte","authors":"Xin Liu, Zhang Chen, Chengyu Zhang, Changsheng Ding, Haitao Feng, Yuanyuan Cui, Yanfeng Gao","doi":"10.1002/adfm.202509495","DOIUrl":"https://doi.org/10.1002/adfm.202509495","url":null,"abstract":"Manganese (Mn)‐based redox flow batteries (RFBs) have emerged as promising candidates for large‐scale energy storage owing to their high redox potential (Mn<jats:sup>2+</jats:sup>/Mn<jats:sup>3+</jats:sup>: 1.58 V vs SHE), cost‐effectiveness, and sustainability. Nevertheless, Mn‐based RFBs face a critical challenge: the undesired formation of crystalline MnO<jats:sub>2</jats:sub> through Mn<jats:sup>3+</jats:sup> disproportionation and irreversibility of MnO<jats:sub>2</jats:sub> deposits on electrode surfaces severely diminish accessible reaction sites and restrict achievable areal capacity. Herein, it is demonstrated that ligand chelation‐mediated structural transformation of MnO<jats:sub>2</jats:sub> by sodium diphosphate (Na<jats:sub>4</jats:sub>P<jats:sub>2</jats:sub>O<jats:sub>7</jats:sub>, PPi) modulates MnO<jats:sub>2</jats:sub> deposition behavior. The PPi coordinate with Mn<jats:sup>2+</jats:sup> to form a stable [Mn(HPO<jats:sub>4</jats:sub>)<jats:sub>2</jats:sub>(H<jats:sub>2</jats:sub>O)<jats:sub>2</jats:sub>]<jats:sup>2−</jats:sup> chelate, which facilitates the incorporation of defective O and P into the evolving MnO<jats:sub>2</jats:sub> structure, effectively disrupting its crystallographic ordering and converting MnO<jats:sub>2</jats:sub> from crystalline to amorphous configuration. The amorphous MnO<jats:sub>2</jats:sub> tends to flow into the electrolyte instead of depositing on the electrode due to the electrostatic interplay, thereby resulting in a breakthrough areal capacity of 91.5 mAh cm<jats:sup>−2</jats:sup> (300 cycles @ 99.7% CE) and 141.8 mAh cm<jats:sup>−2</jats:sup> (150 cycles @ 98.2% CE, the highest reported values), representing a 10‐fold enhancement compared to additive‐free counterparts. The ligand chelation modification of MnO<jats:sub>2</jats:sub> provides a new pathway for developing high‐areal‐capacity Mn‐based RFBs.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"34 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133543","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}
Ziyi Lu, Rundong Chen, Gaoxiong Liu, Bingquan Xia, Kun Fan, Teng Liu, Yang Xia, Shantang Liu, Bo You
{"title":"Recent Advances in Solar‐Driven Artificial Photocatalytic Synthesis of Urea","authors":"Ziyi Lu, Rundong Chen, Gaoxiong Liu, Bingquan Xia, Kun Fan, Teng Liu, Yang Xia, Shantang Liu, Bo You","doi":"10.1002/adfm.202500944","DOIUrl":"https://doi.org/10.1002/adfm.202500944","url":null,"abstract":"Urea (CO(NH<jats:sub>2</jats:sub>)<jats:sub>2</jats:sub>), a nitrogen‐rich compound, is widely used as nitrogen fertilizer in agriculture, key component in medicine, and raw material in chemical production. The continuously growing demand for urea has spurred an escalation in production. Considering the impacts of byproducts during urea production, it is urgent to explore cost‐effective and environmentally benign urea synthesis methods. Artificial photosynthesis, which utilizes renewable solar power to convert carbon dioxide (CO<jats:sub>2</jats:sub>) and nitrogen (N<jats:sub>2</jats:sub>), not only provides a sustainable alternative for urea synthesis but also reduces carbon emissions and fixes nitrogen simultaneously. This review delves into the C−N coupling pathways, key intermediates, and their detection methodologies in photocatalytic urea production. It also discusses the rational design and selection of targeted photocatalysts toward urea synthesis, highlighting their key characteristics that determine the rate‐limiting steps. Furthermore, it systematically examines the challenges in photocatalytic urea synthesis and evaluates viable solutions to overcome these limitations. By identifying current obstacles and proposing potential strategies, this review aims to advance artificial photosynthesis as a sustainable and eco‐friendly approach for urea production. The insights presented herein seek to bridge fundamental research with practical applications, ultimately fostering progress toward energy‐efficient and environmentally benign nitrogen fixation technologies.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"97 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133545","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}
Yuquan Yang, Ju Hao, Chaojie Lyu, Jinlong Zheng, Yanru Yuan, Chenjing Wang, Kai Li, Hui Ying Yang, Xiaolu Pang
{"title":"Electron Islands‐Induced Interface Engineering in FeP@NiCoP/Mo4P3 for Efficient Hydrogen Evolution Catalysis","authors":"Yuquan Yang, Ju Hao, Chaojie Lyu, Jinlong Zheng, Yanru Yuan, Chenjing Wang, Kai Li, Hui Ying Yang, Xiaolu Pang","doi":"10.1002/adfm.202507225","DOIUrl":"https://doi.org/10.1002/adfm.202507225","url":null,"abstract":"This study employs an “electron island” micro‐interface engineering strategy to construct a NiCoP/Mo<jats:sub>4</jats:sub>P<jats:sub>3</jats:sub> heterostructured catalytic system on a FeP substrate via a synergistic hydrothermal synthesis and low‐temperature phosphorization approach. The unique open hierarchical architecture provides atomic‐scale anchoring sites for small‐sized Mo<jats:sub>4</jats:sub>P<jats:sub>3</jats:sub> quantum dots (QDs), forming a high‐density “electron island‐substrate” micro‐interface network, which drastically increases the population of active micro‐interface sites between the two phases. Concurrently, the discretely distributed QDs induce interfacial charge polarization through quantum confinement effects, generating a robust built‐in electric field at the heterointerfaces that drives directional electron migration. Density functional theory (DFT) calculation shows the interfacial interaction between NiCoP and Mo<jats:sub>4</jats:sub>P<jats:sub>3</jats:sub> can effectively manipulate the electronic architecture and regulate the H* adsorption energy, further decreasing the Gibbs free energy (ΔG<jats:sub>H*</jats:sub>). FeP@NiCoP/Mo<jats:sub>4</jats:sub>P<jats:sub>3</jats:sub> can make full use of the active sites generated at the interface, to give full play to the catalytic properties of heterogeneous structures, which ensures the significantly enhanced hydrogen evolution reaction (HER) catalytic efficiency and excellent long‐term stability in alkaline water and complicated seawater environments. This work provides guidance and direction to maximize the interface effect for designing efficient and stable catalysts.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"64 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133412","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}