{"title":"Enhancing Lithium-Mediated Nitrogen Reduction with Porous Polymer Fibers Featuring Lithium-Ion Affinity","authors":"Dongwoo Shin, Ahee Choi, Dong-Yeob Han, Gwangsu Bak, Suhwan Yoo, Yeongbae Jeon, Soojin Park, Yun Jeong Hwang","doi":"10.1002/adfm.202416484","DOIUrl":"https://doi.org/10.1002/adfm.202416484","url":null,"abstract":"The interaction between the electrolyte and working electrode surface affects the cascade of reactions involving Li deposition, N<sub>2</sub>, and proton carriers and consequently the NH<sub>3</sub> production from Li-mediated nitrogen reduction reaction (Li-NRR). Efficient Li-NRR at low Li concentrations is particularly challenging because of low current density and uneven Li metal and lithium nitride plating. Here, the enhanced electrochemical production of NH<sub>3</sub> for a low Li concentration of 0.5 <span>m</span> are demonstrated by employing 3D porous polymer fibers featuring Li<sup>+</sup>-affinity on Cu electrodes. Raman and IR spectroscopic analyses exhibit that the polymeric fibers composed of carboxyl and hydroxyl groups can form Li-binding complexes and decrease interactions with solvents and anions in the electrolyte. The electrochemical analyses support that this polymeric porous structure serves to retain Li<sup>+</sup> near the electrode, expanding the active surface area and increasing current density. The Li-affinitive polymer fibers are effective even at a low Li salt concentration of 0.5 <span>m</span> to improve NH<sub>3</sub> yield and Faradaic efficiency. This study underscores the importance of porous morphology, Li affinity, and its analytical methods in understanding Li-NRR.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"8 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929554","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}
Federico Paolucci, Federica Bianco, Francesco Giazotto, Stefano Roddaro
{"title":"Active Electron Cooling of Graphene","authors":"Federico Paolucci, Federica Bianco, Francesco Giazotto, Stefano Roddaro","doi":"10.1002/adfm.202418456","DOIUrl":"https://doi.org/10.1002/adfm.202418456","url":null,"abstract":"In the emergent field of quantum technology, the ability to manage heat at the nanoscale and in cryogenic conditions is crucial for enhancing device performance in terms of noise, coherence, and sensitivity. Here, active cooling and refrigeration of the electron gas in graphene are demonstrated, by taking advantage of nanoscale superconducting tunnel contacts able to pump or extract heat directly from the electrons in the device. These structures achieved a top <i>cooling</i> of electrons in graphene of ∼15.5 mK at a bath temperature of ∼448 mK, demonstrating the viability of the proposed device architecture. These experimental findings are backed by a detailed thermal model that accurately replicated the observed behavior. Alternative cooling schemes and perspectives are discussed in light of the reported results. Finally, graphene electron cooling could find application in superconducting hybrid quantum technologies, such as radiation detectors, logic gates and qubits.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"21 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929558","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}
Ping Cai, Can Song, Yating Du, Jianbin Wang, Jing Wang, Lixian Sun, Feng Gao, Qifan Xue
{"title":"Recent Progress of Solution-Processed Thickness-Insensitive Cathode Interlayers for High-Performance Organic Solar Cells","authors":"Ping Cai, Can Song, Yating Du, Jianbin Wang, Jing Wang, Lixian Sun, Feng Gao, Qifan Xue","doi":"10.1002/adfm.202422023","DOIUrl":"https://doi.org/10.1002/adfm.202422023","url":null,"abstract":"Organic solar cells (OSCs) have shown great applications potential in flexible/wearable electronics, indoor photovoltaics and so on. The efficiencies of single-junction OSCs have exceeded 19%, making the commercialization of OSCs brighter. Large-area printing fabrication is a key way to the commercialization of OSCs, and solution-processed thickness-insensitive cathode interlayers (CILs) are urgently needed for large-area printing fabrication. High electron mobility of cathode interfacial materials (CIMs) is critical to enable thickness-insensitive CILs. N-type self-doped characteristics can endow organic CIMs with high electron mobility. Different type of n-type self-doped CIMs show different applicability in conventional OSCs and inverted OSCs. External n-type dopants can further increase electron mobility of hybrid blends. Particularly, ZnO doped with organic dyes can achieve superior photoconductivity in inverted OSCs. This review focuses on solution-processed thickness-insensitive CILs for high-performance OSCs. In conventional OSCs, n-type self-doped small molecules and polymers, and external n-doped hybrid blends as thickness-insensitive CILs are summarized. In inverted OSCs, n-type self-doped small-molecular electrolytes and polyelectrolytes, PEI-/PEIE-based polyelectrolytes, and external n-doped hybrid blends (including organic-organic and ZnO-organic) are summarized for thickness-insensitive CILs. The relationships between particular functions of CILs and chemical structures of CIMs are highlighted. Finally, summary and outlook of solution-processed thickness-insensitive CILs are provided.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"27 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929520","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":"A High-Sensitivity, Broadband (1A,1B)-3 Single-Crystal Composite Ultrasonic Transducer","authors":"Yu Lei, Ziyan Gao, Guohong Gan, Wei Bai, Yang Wei, Bing Wang, Xiaoting Yuan, Zewei Hou, Jiawang Hong, Shuxiang Dong","doi":"10.1002/adfm.202417084","DOIUrl":"https://doi.org/10.1002/adfm.202417084","url":null,"abstract":"Piezocomposite ultrasonic transducers (PUTs) are extensively used in diverse technological fields, however, PUTs based on conventional 1–3 piezocomposite containing only one type of piezo pillars have met a bottleneck in further performance enhancement. Herein, based on the [011]-oriented relaxor ferroelectric Pb(In<sub>1/3</sub>Nb<sub>2/3</sub>)O<sub>3</sub>-Pb(Mg<sub>1/3</sub>Nb<sub>2/3</sub>)O<sub>3</sub>-PbTiO<sub>3</sub> (PIN-PMN-PT) crystal, a novel (1<sub>A</sub>,1<sub>B</sub>)-3 piezocomposite structure containing two types of single-crystal pillars- high <i>d</i><sub>33</sub>, <i>k</i><sub>t</sub> pillars with square cross-section (termed as 1<sub>A</sub>) and high dhgh pillars with rectangular cross-section (termed as 1<sub>B</sub>), alternately arranging in epoxy resin and forming a 5 × 9 array are reported. The combination effect and synergistic action of two different piezo-pillars in the piezocomposite notably broaden the working bandwidth, improve the sound sensitivity, and also produce a suppression effect to undesirable transverse vibration modes. Experimental results validate the performance enhancements of (1<sub>A</sub>,1<sub>B</sub>)-3 composite-based PUT: the increases in –3 dB transmitting, receiving bandwidth, and receiving sensitivity are 71.4%, 28.6%, and 26.6%, respectively, in comparison to conventional 13 single-crystal composite-based PUT. Moreover, its hydrostatic figure of merit (HFOM) dhgh (=4084.9 × 10<sup>−15</sup> m<sup>2</sup> N<sup>−1</sup>) is 177.3% higher than that of commercial single crystal 13 piezocomposites. The proposed design strategy represents a promising development direction of next-generation bandwidth and high-sensitivity ultrasonic transducers.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"21 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929555","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}
Yikun Chen, Xinqiang Wang, Wen-Gang Cui, Yong Gao, Hongge Pan, Yan Wang, Renchao Che
{"title":"Multiple Schottky Contacts Motivated via Defects to Tune the Response Ability of Electromagnetic Waves","authors":"Yikun Chen, Xinqiang Wang, Wen-Gang Cui, Yong Gao, Hongge Pan, Yan Wang, Renchao Che","doi":"10.1002/adfm.202417215","DOIUrl":"https://doi.org/10.1002/adfm.202417215","url":null,"abstract":"Metal-organic framework (MOF) derivatives employed as novel microwave-absorbing materials (MAMs) have garnered significant attention due to their diverse in situ or ex situ coordinated components and the flexibility in nano-microstructure fabrication. A well-designed heterointerface can provide an optimal balance between impedance and high-loss capability. However, precisely tuning semiconductor-metal-carbon heterostructures remains a huge challenge. Herein, a multi-component NiS/Co<sub>3</sub>S<sub>4</sub>/NiCo@CNTs/NC nanohybrid with hollow structure is elaborately fabricated using a convenient solvothermal method followed by high-temperature pyrolysis, forming a unique heterostructure with multiple Schottky contacts. This nanohybrid demonstrates a remarkable reflection loss value of −75.9 dB at thickness of 2.6 mm. The transcendent microwave absorption (MA) capacity is primarily attributed to the intense polarization relaxation process and superb impedance-matching properties of the semiconductor/metal/carbon hybrid structure with Schottky barriers. In addition, the built-in electric field established at the Schottky heterointerfaces increases the electron transport capabilities. Notably, the controllable introduction of numerous defects into the carbon layer intensifies the interfacial polarization effect at the Schottky heterointerfaces of the nanohybrid. This study offers innovative insights into the mechanisms of polarization loss and the development of high-performance MAMs.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"80 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929556","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}
Jinshuai Liu, Song Chen, Wenshuo Shang, Jizhen Ma, Jintao Zhang
{"title":"In Situ Formation of 3D ZIF-8/MXene Composite Coating for High-Performance Zinc-Iodine Batteries","authors":"Jinshuai Liu, Song Chen, Wenshuo Shang, Jizhen Ma, Jintao Zhang","doi":"10.1002/adfm.202422081","DOIUrl":"https://doi.org/10.1002/adfm.202422081","url":null,"abstract":"Aqueous Zn batteries have garnered a great deal of attention owing to environmental benefits, intrinsic safety, and cost-effectiveness. However, the commercial viability of these batteries is hindered by Zn anode issues, including dendrite formation and side reactions. Herein, the authors modulate the deposition behavior of Zn<sup>2+</sup> ions through a 3D ZIF-8@MXene (Z@M) composite coating. The Z@M coating can effectively reduce the contact area with the electrolyte, inhibiting the hydrogen evolution reaction and Zn corrosion. Notably, theoretical calculations and in situ experimental observations of Zn deposition reveal that the dual coordination mechanism of MXene and ZIF-8 significantly improves the adsorption energy of Zn atoms. This improved capacity to capture Zn<sup>2+</sup> ions will promote the desolvation of hydrated Zn<sup>2+</sup> ions, resulting in a dendrite-free deposition process. Therefore, in a symmetry cell, the Z@M-Zn anode demonstrates an impressive cycle life of 1050 h at 1 mA cm<sup>−2</sup>. When applies in an aqueous Zn-I<sub>2</sub> battery, the Z@M-Zn anode demonstrates a remarkable lifespan of over 2400 cycles at 5 C. This work provides a straightforward approach to designing reversible Zn anode, offering promising potential for broader applications across various metal-based anode systems.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"28 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929559","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":"Oxygen Edge-Sharing Strategy in P2-Type Na0.67MnO2 Cathodes: Synergistic Enhancement of Intercalation Kinetics and Air Stability","authors":"Yuanming Liu, Shiyu Wang, Weijie Fu, Shuyun Yao, Yingjie Ji, Jingxian Li, Lanlan Shi, Xiaojun Wang, Feike Zhang, Jinghua Yang, Ruilong Liu, Jiangzhou Xie, Zhiyu Yang, Yi-Ming Yan","doi":"10.1002/adfm.202420682","DOIUrl":"https://doi.org/10.1002/adfm.202420682","url":null,"abstract":"Mn-based layered oxides have garnered significant attention as cathode materials for energy storage due to their environmental benignity and high theoretical specific capacity. However, practical applications remain constrained by sluggish Na<sup>+</sup> intercalation kinetics and poor structural stability. In this study, it is engineered that the Mn-O-B unit through an oxygen edge-sharing strategy to modulate Mn─O covalency in P2-type Na<sub>0.67</sub>MnO<sub>2</sub>, thereby achieving high specific capacity and structural stability. Both experimental results and density functional theory (DFT) calculations reveal that increased TM-O covalency facilitates Na<sup>+</sup> diffusion in P2-type Na<sub>0.67</sub>MnO<sub>2</sub> while simultaneously enhancing air stability. The as-prepared P2-type Na<sub>0.67</sub>MnB<sub>0.05</sub>O<sub>2</sub> exhibits a specific capacitance of 452 F g<sup>−1</sup> at 1 A g<sup>−1</sup>, maintaining 96.75% capacity retention after 8800 cycles. This work elucidates the critical role of oxygen edge-sharing in optimizing interactions between transition metal and oxygen atoms, establishing a relationship between Mn─O structure and functional properties. These findings advance the development of high-performance energy storage technologies.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"36 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929557","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":"Closed-Loop Recyclable High-Performance Aerogels Derived from Polystyrene","authors":"Yufei Xiong, Chang-lin Wang, Lijie Dong, Željko Tomović","doi":"10.1002/adfm.202420472","DOIUrl":"https://doi.org/10.1002/adfm.202420472","url":null,"abstract":"Upcycling of low valuable plastic waste into materials with enhanced properties helps progress toward establishing a plastics circular economy. Furthermore, implementing recyclability as a core design criterium for newly formed materials can significantly increase their impact on sustainability, yet rarely explored. In this work, the upcycling of polystyrene (PS) waste is presented into closed-loop recyclable high-performance aerogels. Through a simple post-functionalization process, PS is aminated to generate a polyfunctional amine, which is then reacted with aldehydes to form a recyclable cross-linked imine network. This network is subsequently dried to produce poly(styrene-imine) aerogels (PSAs). The resulting PSAs exhibit excellent thermally insulating properties, along with low density, outstanding mechanical strength, and intrinsic hydrophobicity. More importantly, these aerogels show quantitative depolymerization under acidic aqueous conditions, back to their original precursors which can be recovered in high yield and purity and reused for the synthesis of fresh aerogels with nearly identical material properties, thus achieving closed-loop recycling. This work presents an efficient method for upcycling of chemically non-recyclable plastics into recyclable and high value-added advanced aerogel materials, offering a new pathway for establishing a circular economy for plastics.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"5 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929562","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":"2D Ruddlesden-Popper Perovskites/PVDF-TrFE Photodetector for Anti-Interference Vision System Derived from Ferroelectric Polarization Modulation","authors":"Xinglong Zhang, Enliu Hong, Xiaojun Tan, Jie Liu, Anquan Jiang, Xiaosheng Fang","doi":"10.1002/adfm.202424848","DOIUrl":"https://doi.org/10.1002/adfm.202424848","url":null,"abstract":"2D Ruddlesden-Popper (RP) perovskites have garnered increasing attention for their excellent photoresponse, characterized by high carrier mobility, tunable bandgaps, high optical absorption, and molecular asymmetry. Herein, centimeter scale single crystal 2D hybrid perovskites, BA<sub>2</sub>PbBr<sub>4</sub> (BPB) is synthesized, using quasi-static cooling method and composited with ferroelectric PVDF-TrFE(PT) film to construct a multi-field coupling photodetector (PD) via van der Waals force contact. Ferroelectric tests show that the PT film exhibits a saturated polarization strength of 3.6 µC cm<sup>−2</sup>, allowing the ferroelectric localized field to modulate the band structure of PT and enhance the photocurrent. The Heterojunction systems exhibit ultra-high responsivity (15.3 A W<sup>−1</sup>) and detectivity (1.99 × 10<sup>13</sup> Jones) under 390 nm illumination at 3 V bias, with a performance improvement of over 10<sup>2</sup> times compared to BPB PDs. Furthermore, the hybrid PDs exhibit highly stable <i>I–t</i> curve with a photocurrent retention rate of 97.4%. Leveraging this feature, a large-area imaging device is designed at the centimeter level scale, enabling multifunctional vision applications accurate letter imaging process and anti-interference number detection. The work presents a valuable insight in design of future autonomous driving vision systems.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"125 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929762","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}
Min Wu, Lei Liu, Youqiang Xing, Ze Wu, Peng Huang, Bingjue Li
{"title":"Plasmonic Nanodiamond – Microneedle Bioinspired System for Ultrarapid Sampling and Quantum Sensing of Melanoma-Related MiRNA","authors":"Min Wu, Lei Liu, Youqiang Xing, Ze Wu, Peng Huang, Bingjue Li","doi":"10.1002/adfm.202422305","DOIUrl":"https://doi.org/10.1002/adfm.202422305","url":null,"abstract":"MicroRNA (miRNA) in interstitial fluid (ISF) is a promising biomarker for early disease diagnosis, but its quantification is challenging due to low sampling efficiency and weak signals. Here, inspired by the osmotic pressure-driven feeding mechanism of sea anemones, a novel is designed that plasmonic nanodiamonds – microneedles (PND-MNs) bioinspired system for ultrarapid sampling and quantum sensing of melanoma-related miRNA. Specifically, high-osmotic hydrogel microneedles, prepared by immersing in LiCl solution, exhibit a substantial swelling ratio for rapid ISF enrichment, extracting 0.92 ± 0.14 mg within 5 min. Concurrently, by coating fluorescent nanodiamonds (FNDs) with hollow composite metal Au-Ag NPs, precise modulation of the fluorescence intensity of nitrogen vacancy color centers (NV-center) in FNDs has been achieved. This innovative quantum sensing technology significantly enhances the fluorescence signal in the PND-MNs bioinspired system, amplifying it by a factor of 16, reducing the detection limit of miRNA to an unprecedented 0.68 f<span>m</span> (to the knowledge, no method based on fluorescent microneedles for detecting biomarkers has surpassed this level). Furthermore, the PND-MNs bioinspired system, employing backpropagation neural network (BPNN), achieves high accuracy in recognizing miRNA concentrations (R<sup>2</sup> = 0.9986). By combining rapid sampling, signal enhancement, and machine learning, it holds promise for detecting ISF biomarkers, offering significant clinical applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"12 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929516","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}