Advanced Functional Materials最新文献

Unraveling the Role of Open Metal Sites and Their Capping Ligands in MOFs Stability and Liquid-Phase Separation

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2025-04-26 DOI: 10.1002/adfm.202505730

Chunmei Jia, Qazi Mohammad Junaid, Guo-Ying Han, Yu Gai, Francisco G. Cirujano, Xiao Feng

{"title":"Unraveling the Role of Open Metal Sites and Their Capping Ligands in MOFs Stability and Liquid-Phase Separation","authors":"Chunmei Jia, Qazi Mohammad Junaid, Guo-Ying Han, Yu Gai, Francisco G. Cirujano, Xiao Feng","doi":"10.1002/adfm.202505730","DOIUrl":"https://doi.org/10.1002/adfm.202505730","url":null,"abstract":"The stability of metal–organic frameworks (MOFs) is crucial for their practical applications. Open metal sites (OMS), essential active sites in various applications, also significantly impact stability, yet their role remains insufficiently understood. This study investigates MOF-808, a zirconium-based MOF with six OMS per cluster, revealing its higher stability in liquid water compared to gaseous water. Coordination of formic acid at OMS notably enhances water stability, while recrystallization experiments elucidate the mechanisms of instability in gaseous water. Thermal stability is determined by the decomposition temperature of capping ligands on OMS. In liquid-phase adsorption of high-value bio-oil compound creosol, uptake results demonstrate that capping ligand polarity modulates pore hydrophilicity/hydrophobicity, affecting adsorption selectivity. Remarkably, MOF-808 capped with pentafluorobenzoic acid achieves 100% selective pore occupancy during adsorption. This study highlights OMS as critical to MOF stability and emphasizes the role of capping ligands in improving stability and tuning adsorption properties. It underscores nonstructural ligand modifications as a powerful strategy to enhance MOF performance, broadening their application potential in challenging environments.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"9 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875815","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}

引用次数: 0

Mixed-Dimensional 0D-DNA-2D Heterostructures Beyond van der Waals: A DNA-Templated Strategy for Optoelectronic Tunability

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2025-04-26 DOI: 10.1002/adfm.202502140

Kai Chen, Haosen Miao, Stoichko Dimitrov, Matteo Palma

{"title":"Mixed-Dimensional 0D-DNA-2D Heterostructures Beyond van der Waals: A DNA-Templated Strategy for Optoelectronic Tunability","authors":"Kai Chen, Haosen Miao, Stoichko Dimitrov, Matteo Palma","doi":"10.1002/adfm.202502140","DOIUrl":"https://doi.org/10.1002/adfm.202502140","url":null,"abstract":"The assembly of nanomaterials of different dimensionality into mixed-dimensional heterostructures can allow circumventing individual nanomaterials intrinsic limitations toward the development of novel hybrids for a variety of technological applications. Critical to this end is the ability to control the interface of the single components in terms of spatial separation and chemical nature, in order to optimize their synergistic coupling, tailor their optoelectronic properties, and potentially impart novel functionalities. Herein the controlled assembly and optoelectronic tunability of 0D-2D heterostructures is demonstrated, employing DNA as a linking and template moiety for the modular assembly of metal sulfide nanoparticles (NPs) on MoS2, with nanoscale control over their separation and ability to concomitantly assemble different kind of NPs on the same DNA template linker. The developed aqueous solution-processable approach permits the systematic modulation of charge carrier doping and trion formation in the transition metal dichalcogenide (TMD) in a non-destructive manner. Moreover, it allowed to tailor the photoinduced electrical response -with ultrahigh detectivity- of NPs-TMD phototransistors to different wavelengths, thanks to the concomitant presence of different nanoparticles by design. These are key requirements for optimal and scalable implementation of low-dimensional materials and their heterostructures in optoelectronic devices.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"30 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875819","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}

引用次数: 0

Regulating the Interphase Strain in High‐Entropy Oxide Thin Films – An Approach to Attaining Giant Energy Storage Capability under Moderate Electric Fields

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2025-04-26 DOI: 10.1002/adfm.202502853

Hao Luo, Yunlong Sun, Haotian Wen, Richard Webster, Yasuhiro Sakamoto, Zizheng Song, Yating Ran, Chenlu Jiang, Siyuan Zhang, Zibin Chen, Shery L. Y. Chang, Danyang Wang

{"title":"Regulating the Interphase Strain in High‐Entropy Oxide Thin Films – An Approach to Attaining Giant Energy Storage Capability under Moderate Electric Fields","authors":"Hao Luo, Yunlong Sun, Haotian Wen, Richard Webster, Yasuhiro Sakamoto, Zizheng Song, Yating Ran, Chenlu Jiang, Siyuan Zhang, Zibin Chen, Shery L. Y. Chang, Danyang Wang","doi":"10.1002/adfm.202502853","DOIUrl":"https://doi.org/10.1002/adfm.202502853","url":null,"abstract":"In recent years, high‐entropy dielectrics have demonstrated superior performance in capacitive energy storage devices. However, the impressive energy storage density of these materials typically necessitates ultrahigh external electric fields, which restricts the range of their practical applications. In this work, an interphase strain engineering strategy is developed, i.e., through the modulation of the deposition temperatures and post‐deposition cooling rates, an appropriate amount of pyrochlore nanocolumns is introduced into high‐entropy oxide epitaxial films, exerting a nontrivial level of interphase strain on adjacent perovskite lattices. This interphase strain transforms the dispersive polar nanodomains into a compact polar slush state, enabling a delicate balance between spontaneous polarization and breakdown strength. Ultimately, the (Bi0.5Na0.5)(Ti0.2Sn0.2Hf0.2Fe0.2Nb0.2)O3 (BNTSHFN) high‐entropy oxide thin film in this work exhibits a giant recoverable energy density of 93 J cm−3 and a high efficiency of 83% under a moderate electric field of 3.6 MV cm−1. This work provides an innovative idea for designing high‐entropy capacitive energy storage devices with promising potential in real‐world scenarios.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"15 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875856","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}

引用次数: 0

Conjugated Oligomer-Based NIR-II Chemiluminescence Nanosensor for In Vivo Imaging

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2025-04-26 DOI: 10.1002/adfm.202424286

Ling Li, Xinyi Zhang, Yuxin Ren, Benkai Bao, Meiqi Li, Mengpan Zhang, Junqing Wang, Jian Wang, Yanli Tang

{"title":"Conjugated Oligomer-Based NIR-II Chemiluminescence Nanosensor for In Vivo Imaging","authors":"Ling Li, Xinyi Zhang, Yuxin Ren, Benkai Bao, Meiqi Li, Mengpan Zhang, Junqing Wang, Jian Wang, Yanli Tang","doi":"10.1002/adfm.202424286","DOIUrl":"https://doi.org/10.1002/adfm.202424286","url":null,"abstract":"Chemiluminescence imaging has become a promising optical imaging method because of its advantages such as no excitation source and minimal background autofluorescence. However, chemiluminescent nanosensors with second near-infrared (NIR-II) window emission are rarely reported. Here, a NIR-II chemiluminescence nanosensor OLBB-CLS is designed by adopting the CRET (chemiluminescence resonance energy transfer) – FRET (fluorescent resonance energy transfer) combined strategy, which consists of OFBTL, BTD540-C8, BBTD725-C8 and DSPE-PEG2000. OFBTL, a chemiluminescent conjugated oligomer with D-A-D (donor-acceptor-donor) molecular structure, acts as a chemiluminescent probe of 1O2 and the donor of CRET. BTD540-C8, as an energy receptor of CRET and an energy donor of FRET, can absorb the energy of chemiluminescence and transfer the energy to NIR-II molecule BBTD725-C8, thus producing NIR-II fluorescence. Notably, there is a great overlap between the chemiluminescence spectrum of OFBTL and the absorption spectrum of BTD540-C8, enabling efficient CRET between them. Also, an excellent overlap occurs between the emission spectrum of BTD540-C8 and the absorption spectrum of BBTD725-C8, allowing effective FRET. The nanosensor OLBB-CLS demonstrates remarkable biosafety and can achieve in vivo NIR-II chemiluminescent imaging for ROS-related disease with a high signal-to-noise ratio. This study paves the way for the design of NIR-II chemiluminescence probes for in vivo imaging.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"3 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875824","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}

引用次数: 0

Microenvironments‐Targeted Nanomaterials for Atherosclerosis Therapy

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2025-04-26 DOI: 10.1002/adfm.202421512

Chunli Song, Hao Ling, Guanqing Yang, Jianxun Ding

{"title":"Microenvironments‐Targeted Nanomaterials for Atherosclerosis Therapy","authors":"Chunli Song, Hao Ling, Guanqing Yang, Jianxun Ding","doi":"10.1002/adfm.202421512","DOIUrl":"https://doi.org/10.1002/adfm.202421512","url":null,"abstract":"Atherosclerosis significantly contributes to cardiovascular disease. Traditional treatments for atherosclerosis, such as pharmacological interventions and surgical procedures, have demonstrated limited efficacy and often yield unsatisfactory results. Consequently, safe and effective therapeutic strategies are urgently needed. The atherosclerotic microenvironments, characterized by inflammation driven by foam cells, damaged endothelial cells, recruited leukocytes, lipoproteins, and inflammatory mediators, play a key role in disease progression. By leveraging the biological components and physicochemical properties of these microenvironments, researchers have developed microenvironments‐targeted nanomaterials as a promising approach to treat atherosclerosis. These nanomaterials aim to address and eliminate inflammatory processes. Their functions include repairing endothelial damage, reducing lipoprotein accumulation, inhibiting leukocyte chemotaxis, suppressing foam cell formation, delaying plaque rupture, and preventing thrombosis within the plaque. This review highlights the therapeutic mechanisms and effects of nanomaterials targeting key processes in atherosclerotic microenvironments. Finally, the challenges and prospects of nanomaterial‐based therapies for atherosclerosis are discussed to inspire the development of nanomaterials that modulate atherosclerotic microenvironments, potentially leading to promising clinical applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"3 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875845","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}

引用次数: 0

Topological Magnetism: Materials and Devices

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2025-04-26 DOI: 10.1002/adfm.202425483

Jingyan Zhang, Jiawang Xu, Yunchi Zhao, Pengwei Dou, Jiaji Yang, Jie Qi, Haifeng Du, Ying Zhang, Shiming Zhou, Baogen Shen, Shouguo Wang

{"title":"Topological Magnetism: Materials and Devices","authors":"Jingyan Zhang, Jiawang Xu, Yunchi Zhao, Pengwei Dou, Jiaji Yang, Jie Qi, Haifeng Du, Ying Zhang, Shiming Zhou, Baogen Shen, Shouguo Wang","doi":"10.1002/adfm.202425483","DOIUrl":"https://doi.org/10.1002/adfm.202425483","url":null,"abstract":"The emerging interest in topological magnetism has ignited exciting vitality in the field of spintronics, thereby offering a promising route for breaking Moore's law constraints and establishing an efficient information storage model. Unlike the conventional 2D storage cell based on macroscopic magnetization, magnetic skyrmions—the representative of topological magnetism—are considered candidates for realizing 3D memory, such as “racetrack memory,” facilitating the development of topological spintronics. Since the discovery of skyrmion‐hosting materials, extensive studies on topological magnetic materials are conducted, although challenges have arisen with rapid research progress. Herein, the recent progress in topological spintronics, including material and device design, is reviewed. Beyond bulk magnets, research on topological magnetism is focused on low‐dimensional materials, including magnetic films and 2D magnetic materials, which are promising candidates for magnetic storage devices. Furthermore, the design of new structures, such as in lattice or composition asymmetry engineering, to expand the family of topological magnetic materials is essential. In addition to skyrmions, various topological magnetic structures such as antiskyrmions, merons, and 3D complex structures are detailed. Furthermore, topological magnetism manipulation and related principal devices are discussed. This review provides an opportunity to generate more interest and deepen the discussion of topological magnetism.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"8 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875857","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}

引用次数: 0

Electrochemical Self‐Assembly of Boron‐Based Cathode‐Electrolyte Interphase to Stabilize 4.65 V LiCoO2

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2025-04-26 DOI: 10.1002/adfm.202504165

Hengyu Ren, Xiaohu Wang, Wangyang Ding, Chunyu Xu, Wenguang Zhao, Haocheng Ji, Haocong Yi, Zhaohuang Zhan, Yongli Song, Lin Zhou, Qinghe Zhao, Feng Pan

{"title":"Electrochemical Self‐Assembly of Boron‐Based Cathode‐Electrolyte Interphase to Stabilize 4.65 V LiCoO2","authors":"Hengyu Ren, Xiaohu Wang, Wangyang Ding, Chunyu Xu, Wenguang Zhao, Haocheng Ji, Haocong Yi, Zhaohuang Zhan, Yongli Song, Lin Zhou, Qinghe Zhao, Feng Pan","doi":"10.1002/adfm.202504165","DOIUrl":"https://doi.org/10.1002/adfm.202504165","url":null,"abstract":"The cathode‐electrolyte interphase (CEI) is vital for the stability of LiCoO2 (LCO) beyond 4.55 V (vs Li/Li+). Herein, the full coverage of boron‐based CEI is achieved on LCO surface via utilizing the self‐wetting synthesis of boric acid (i.e., B‐LCO), accompanying with the subsequent electrochemical self‐assembly process upon cycles. Initially, the B‐LCO is coated with borate deposits (size of 10–20 nm), then it melts and fully covers the surface upon sintering, leading to the full coverage of boron‐based artificial CEI, which directly reduces the side reactions induced by highly oxidative Co4+/On− (0 < n < 2). Significantly, during cycling, the in situ interfacial reactions between the surface boron‐based species and LiF promote the formation of crystalline LiB6O9F components, showing the mechanically robust and highly Li+ conductive characteristics. Due to the synergism of robust CEI and structurally tough surface rocksalt (RS) phase, not only the more reversible phase transition and uniform Li+ (de)lithiation are achieved, but also the particle cracks and surface deterioration issues are effectively inhibited. As a result, the B‐LCO||Li cells show excellent cycle stability, with a high retention of 84.0% in 500 cycles in 3–4.65 V.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"8 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875859","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}

引用次数: 0

Off-Stoichiometry Engineering of the Electrical and Optical Properties of SrNbO3 Using Oxide Molecular Beam Epitaxy

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2025-04-26 DOI: 10.1002/adfm.202419990

Jasnamol Palakkal, Alexey Arzumanov, Ruiwen Xie, Zhiyuan Li, Niloofar Hadaeghi, Thomas Wagner, Tianshu Jiang, Yating Ruan, Gennady Cherkashinin, Leopoldo Molina Luna, Hongbin Zhang, Lambert Alff

{"title":"Off-Stoichiometry Engineering of the Electrical and Optical Properties of SrNbO3 Using Oxide Molecular Beam Epitaxy","authors":"Jasnamol Palakkal, Alexey Arzumanov, Ruiwen Xie, Zhiyuan Li, Niloofar Hadaeghi, Thomas Wagner, Tianshu Jiang, Yating Ruan, Gennady Cherkashinin, Leopoldo Molina Luna, Hongbin Zhang, Lambert Alff","doi":"10.1002/adfm.202419990","DOIUrl":"https://doi.org/10.1002/adfm.202419990","url":null,"abstract":"The highly conducting and transparent inorganic perovskites SrBO3 with V, Nb, Mo, and their mixtures at the B-site have recently attracted the attention of the oxide electronics community as novel alternative transparent conducting oxides. For different applications, from solar cells to transparent electronics, it is desirable to tune the optical transmission window in the ultraviolet, visible, and infrared (IR) range. The conventional approach is substitutional design at the A- and/or B-site. Here, a method of engineering the off-stoichiometry of the perovskite SrNbO3 is used, opening new pathways to broaden the range of applications without adding additional elements. For oxide molecular beam epitaxy (MBE) grown SrNbO3 on GdScO3 substrates, it shows that controlled Sr deficiency shifts the plasma edge from ∼2 eV in the visible range into the near-IR region, 1.37 eV (similar to stoichiometric SrVO3). The epitaxial growth using MBE allows going beyond the limitations of phase stability set by thermodynamics. This work includes controlled vacancy sites as quasi-substitutional virtual elements and advances the stoichiometry engineering of perovskite oxides using an oxide MBE.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"78 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875814","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}

引用次数: 0

Revealing Effect of Aggregation Structure of Plant Precursors on Rate Performance of Carbon Anode for Sodium‐Ion Batteries

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2025-04-26 DOI: 10.1002/adfm.202425234

Tianyun Zhang, Tian Zhang, Changhong Zhao, Fujuan Wang, Lirong Zhang, Yu Li, Liyu Zhang, Fen Ran

{"title":"Revealing Effect of Aggregation Structure of Plant Precursors on Rate Performance of Carbon Anode for Sodium‐Ion Batteries","authors":"Tianyun Zhang, Tian Zhang, Changhong Zhao, Fujuan Wang, Lirong Zhang, Yu Li, Liyu Zhang, Fen Ran","doi":"10.1002/adfm.202425234","DOIUrl":"https://doi.org/10.1002/adfm.202425234","url":null,"abstract":"Plant‐based hard carbon is a highly promising anode material for sodium‐ion batteries. Numerous studies have dedicated significant effort to the selection of precursors; however, there has been limited comprehensive research on the low‐rate performance of plant‐based hard carbon. Indeed, the aggregated structure of cellulose and hemicellulose in precursors has been underestimated regarding its influence on the material properties. In this study, the inherent aggregated structure of kapok fiber is optimized. It has been observed that the aggregation structure of the precursor significantly influences the content of highly disordered carbon post‐carbonization, consequently impacting the rate performance of the derived anode material. To address the problems, aluminum ions innovatively are used to support the crushed cellulose‐hemicellulose arrays, and the prepared carbon anode has a capacity retention rate of up to≈70% at a current density increased from 0.05 to 3.2 A g−1. This research not only clarifies the mechanism by which the structure leads to the decline of rate performance but also innovatively introduces the ion coupling method to repair the structure, thereby achieving the optimization of rate performance.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"31 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875855","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}

引用次数: 0

Engineering Supramolecular Composite Hydrogels via “pH‐Induced Ureidopyimidinone (UPy) Tautomerization” Strategy

IF 19 1区材料科学

Advanced Functional Materials Pub Date : 2025-04-26 DOI: 10.1002/adfm.202505578

Min Gao, Xiaoying Hao, Yue Li, Ying Tang, Weipeng Yang, Kaisheng Zhang, Yingxi Lu, Xianfeng Zhou

{"title":"Engineering Supramolecular Composite Hydrogels via “pH‐Induced Ureidopyimidinone (UPy) Tautomerization” Strategy","authors":"Min Gao, Xiaoying Hao, Yue Li, Ying Tang, Weipeng Yang, Kaisheng Zhang, Yingxi Lu, Xianfeng Zhou","doi":"10.1002/adfm.202505578","DOIUrl":"https://doi.org/10.1002/adfm.202505578","url":null,"abstract":"Hydrogels are compelling materials for emerging applications including regenerative medicine, flexible electronics, and soft robotics; however, their mechanical weakness, time‐consuming fabrication, and end‐of‐life disposal pose significant challenges. Herein, a straightforward “pH‐induced tautomerization” strategy is presented for fabricating supramolecular composite hydrogels, which harness physical crosslinking mediated by ureidopyimidinone (UPy) tautomerism to construct a leaf‐like hierarchical meshing structures involving highly dynamic microphase‐separated domains. The resultant hydrogels achieve high mechanical properties, with an ultimate stress of 1.00 ± 0.09 MPa, a strain level of 4219.62 ± 56.32%, a toughness of 11.60 ± 0.29 MJ m−3, and a fracture energy of 28.40 ± 0.76 KJ m−2, which are 3.9‐20 times higher than those of conventional hydrogels with similar matrices. Beyond their superior mechanical properties, these hydrogels offer a remarkable combination of high compressive strength and exceptional ductility, ensuring superior puncture resistance. The uniform distribution of hydrogen bonds endows the material with outstanding fatigue resistance, dynamic self‐healing capabilities, and shape memory performance. Additionally, the physical crosslinking facilitates effortless recycling and regeneration, as the network can be disrupted through alkaline‐induced dissociation of hydrogen bonding and electrostatic repulsion. This “pH‐induced tautomerization” strategy offers a promising route for developing high‐performance, recyclable hydrogels for advanced applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"29 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875858","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}

引用次数: 0