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Adjustable Room-Temperature Phosphorescence through Tunable Aggregation of Dopants in Polymers and its Application in Hydrazine Hydrate Detection
IF 19 1区 材料科学
Advanced Functional Materials Pub Date : 2025-03-30 DOI: 10.1002/adfm.202502811
Yawen Zhang, Mingxue Gao, Ruimin Wu, Yunshu Meng, Nan Li, Zhijian Chen, Manman Fang, Jie Yang, Zhen Li
{"title":"Adjustable Room-Temperature Phosphorescence through Tunable Aggregation of Dopants in Polymers and its Application in Hydrazine Hydrate Detection","authors":"Yawen Zhang, Mingxue Gao, Ruimin Wu, Yunshu Meng, Nan Li, Zhijian Chen, Manman Fang, Jie Yang, Zhen Li","doi":"10.1002/adfm.202502811","DOIUrl":"https://doi.org/10.1002/adfm.202502811","url":null,"abstract":"The development of stimulus-responsive phosphorescent materials has attracted increasing attention owing to their advantages in practical applications. However, those responses to toxic and hazardous chemicals remain rare owing to the lack of suitable design strategies. Herein, a new approach to regulate the room-temperature phosphorescence (RTP) effect of doping systems is developed, in which two polar phenothiazine derivatives functionalized with trifluoroacetyl groups act as phosphorescent guests and polymer matrices with different polarities function as hosts. Regulated by the polymer host, the transition from aggregation to dispersion can be realized for guest molecules, resulting in enhanced RTP. Unlike traditional stimulus-responsive materials, the doped system can undergo a dynamic state transition upon exposure to hydrazine hydrate vapor, thereby activating phosphorescence. Building on these findings, an effective model is established to investigate the effects of the transitions between aggregated and dispersed states. A novel stimulus-responsive sensor is developed to detect hazardous hydrazine hydrates.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"12 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736851","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
Identification and Reversible Optical Switching of NV+ Centers in Diamond
IF 19 1区 材料科学
Advanced Functional Materials Pub Date : 2025-03-30 DOI: 10.1002/adfm.202500817
Marcel Dickmann, Lucian Mathes, Ricardo Helm, Vassily Vadimovitch Burwitz, Werner Egger, Johannes Mitteneder, Christoph Hugenschmidt, Peter Sperr, Maik Butterling, Maciej Oskar Liedke, Andreas Wagner, Joachim Dorner, Thomas Schwarz-Selinger, Günther Dollinger
{"title":"Identification and Reversible Optical Switching of NV+ Centers in Diamond","authors":"Marcel Dickmann, Lucian Mathes, Ricardo Helm, Vassily Vadimovitch Burwitz, Werner Egger, Johannes Mitteneder, Christoph Hugenschmidt, Peter Sperr, Maik Butterling, Maciej Oskar Liedke, Andreas Wagner, Joachim Dorner, Thomas Schwarz-Selinger, Günther Dollinger","doi":"10.1002/adfm.202500817","DOIUrl":"https://doi.org/10.1002/adfm.202500817","url":null,"abstract":"Positive nitrogen-vacancy centers (NV<sup>+</sup>) in diamond are predicted to exist in conjunction with neutral (NV<sup>0</sup>) and negative (NV<sup>−</sup>) centers. However, the existence of NV<sup>+</sup> has only been indirectly inferred through a shift of the Fermi level. Evidence of NV<sup>+</sup> coexisting with NV<sup>0</sup> and NV<sup>–</sup> in diamond has not yet been observed. In this paper, positron annihilation spectroscopy in combination with in situ light illumination is applied, in order to investigate the presence of NV<sup>+</sup> centers in nitrogen implanted and subsequently annealed diamond. Switching of NV<sup>+</sup> to NV<sup>0</sup> centers is observed with a threshold photon energy of 1.234(8) eV. In complete darkness, a decay of NV<sup>0</sup> centers with a decay time of 1.73(22) h can be detected. In conclusion, previously converted NV<sup>0</sup> centers are metastable and partially decay in darkness, leading to the reformation of NV<sup>+</sup> centers.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"131 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736911","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
Fully Electrically Controlled Low Resistance-Area Product and Enhanced Tunneling Magnetoresistance in the Van Der Waals Multiferroic Tunnel Junction
IF 19 1区 材料科学
Advanced Functional Materials Pub Date : 2025-03-30 DOI: 10.1002/adfm.202423855
Xiao-Hui Guo, Jia Zhang, Kai-Lun Yao, Lin Zhu
{"title":"Fully Electrically Controlled Low Resistance-Area Product and Enhanced Tunneling Magnetoresistance in the Van Der Waals Multiferroic Tunnel Junction","authors":"Xiao-Hui Guo, Jia Zhang, Kai-Lun Yao, Lin Zhu","doi":"10.1002/adfm.202423855","DOIUrl":"https://doi.org/10.1002/adfm.202423855","url":null,"abstract":"The development of next-generation spin nanomemory systems faces the challenge of achieving nonvolatile electrical control of magnetic states in magnetic tunnel junctions. Here, a strategy is proposed using trilayer van der Waals heterostructures combining an A-type antiferromagnetic YBr<sub>2</sub> bilayer and a ferroelectric Al<sub>2</sub>Se<sub>3</sub> monolayer. Nonvolatile modulation of the ferroelectric polarization direction of Al<sub>2</sub>Se<sub>3</sub> can flip the interlayer magnetic coupling of YBr<sub>2</sub> between ferromagnetic and antiferromagnetic states. The interlayer magnetic phase transition is caused by the band structure shift and interfacial charge transfer induced by the polarization field. The TiTe<sub>2</sub>/2L-YBr<sub>2</sub>/Al<sub>2</sub>Se<sub>3</sub>/TiTe<sub>2</sub> multiferroic devices achieve a fully electrically controlled tunneling magnetoresistance with a ratio of up to 11550% and an exceptionally low resistance-area product of 0.28 Ω µm<sup>2</sup> by establishing a good P-type Ohmic contact between the TiTe<sub>2</sub> electrode and the central heterojunction. There is also a perfect spin filtering effect. This work provides new perspectives for the development of low-power, fast-response, nonvolatile and fully electrically controlled spintronic memory devices.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"22 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736850","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
Making Photoresponsive Metal–Organic Frameworks an Effective Class of Heterogeneous Photocatalyst
IF 19 1区 材料科学
Advanced Functional Materials Pub Date : 2025-03-30 DOI: 10.1002/adfm.202421318
Rui Liu, Hao Wu, Hoi Ying Chung, Yun Hau Ng
{"title":"Making Photoresponsive Metal–Organic Frameworks an Effective Class of Heterogeneous Photocatalyst","authors":"Rui Liu, Hao Wu, Hoi Ying Chung, Yun Hau Ng","doi":"10.1002/adfm.202421318","DOIUrl":"https://doi.org/10.1002/adfm.202421318","url":null,"abstract":"A highly effective photocatalyst is the core component of photocatalytic energy conversion. Recently, photoresponsive metal–organic frameworks (MOFs) photocatalysts have exhibited convincing potential and become the hotspot research direction because of their dramatic advantages in enhancing light-harvesting capability, charge transfer efficiency, and catalytic performance of surface reactions in a photocatalytic system. In-depth interpretations of the photoresponsive MOFs-based photocatalysts have been constructed, and more insightful understandings of these materials can be obtained by advanced characterizations and accurate theoretical studies, which provide a solid platform to predict the mechanism and applications in photocatalysis. This review summarizes the recent advances in photoresponsive MOF-based photocatalysts for solar-to-chemical energy conversion. A general background of photoresponsive MOF photocatalysts is provided initially. A brief discussion of the possible roles of photoresponsive MOFs in photocatalysis is then provided. After that, the advanced characterization techniques for photoresponsive MOF photocatalysts are presented. After obtaining a fundamental understanding of photoresponsive MOF-based photocatalysts, their multifold applications are highlighted. Finally, the future challenges and perspectives of photoresponsive MOF photocatalysts are proposed. This review is expected to motivate the exploration of novel photoresponsive MOF-based photocatalysts and drive future development in this burgeoning field.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"11 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736908","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
Strontium Hexacyanoferrate Nanomedicine Alleviates Ischemic Cardiomyopathy by Regulating Pyroptosis
IF 19 1区 材料科学
Advanced Functional Materials Pub Date : 2025-03-30 DOI: 10.1002/adfm.202417939
Xi Li, Yu Yao, Xiangyi Ren, Liying Wang, Minfeng Huo, Jianlin Shi
{"title":"Strontium Hexacyanoferrate Nanomedicine Alleviates Ischemic Cardiomyopathy by Regulating Pyroptosis","authors":"Xi Li, Yu Yao, Xiangyi Ren, Liying Wang, Minfeng Huo, Jianlin Shi","doi":"10.1002/adfm.202417939","DOIUrl":"https://doi.org/10.1002/adfm.202417939","url":null,"abstract":"Ischemic cardiomyopathy remains high mortality and morbidity worldwide due to dysfunctional cell metabolism and programmed death of cardiomyocytes. Restoration of the blocked blood flows is a major therapeutic approach against ischemic cardiomyopathy, which, unfortunately, may cause the burst of oxidative species damaging tissues (ischemic/reperfusion injury, IR). Cardiac antioxidation and revascularization are two major therapeutic aims in treating cardiac IR as well as myocardial infarction (MI). In the present work, strontium hexacyanoferrate (SrHF) nanoparticles are synthesized for alleviating both the cardiac pathologies of MI and IR concurrently. SrHF features high antioxidative catalytic activity, mimicking superoxide dismutase and catalase in eliminating reactive oxygen species for cardiac protection. In vivo, investigation confirms that SrHF has significantly alleviated myocardial functional deterioration and enhanced cardiomyocyte survival. Mechanistic studies demonstrate that SrHF can effectively inhibit cardiac programmed pyroptosis and pathological remodeling through antioxidation and enhance angiogenesis by bioactive strontium ions. The present work provides a promising therapeutic strategy in treating ischemic cardiac pathologies, providing a fundamental basis for clinical translation and application toward cardiovascular diseases.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"36 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143737170","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
Designing Metastable P3-type Layered Negative Electrodes with High Na Vacancy Concentration for High-Power Sodium-Ion Batteries
IF 19 1区 材料科学
Advanced Functional Materials Pub Date : 2025-03-30 DOI: 10.1002/adfm.202417830
Alok K. Pandey, Benoît D.L. Campéon, Saad Zafar, Toru Ishigaki, Tsubasa Koyama, Masanobu Nakayama, Naoaki Yabuuchi
{"title":"Designing Metastable P3-type Layered Negative Electrodes with High Na Vacancy Concentration for High-Power Sodium-Ion Batteries","authors":"Alok K. Pandey, Benoît D.L. Campéon, Saad Zafar, Toru Ishigaki, Tsubasa Koyama, Masanobu Nakayama, Naoaki Yabuuchi","doi":"10.1002/adfm.202417830","DOIUrl":"https://doi.org/10.1002/adfm.202417830","url":null,"abstract":"Titanium-based layered oxides exhibit promising characteristics for negative electrode applications for sodium-ion batteries (SIBs) owing to their low operating potential and stable redox behavior. However, challenges persist in synthesizing single-phase Na<i><sub>x</sub></i>Cr<i><sub>x</sub></i>Ti<sub>1–</sub><i><sub>x</sub></i>O<sub>2</sub> materials with reduced sodium content (<i>x</i> &lt; 0.58) due to structural instability. In this study, an unconventional approach utilizing potassium analogues to design high Na vacancy concentration compounds is proposed. By exploiting the larger ionic size of K<sup>+</sup> ions, a P3-type K<sub>0.5</sub>Cr<sub>0.5</sub>Ti<sub>0.5</sub>O<sub>2</sub> layered material with lower alkali ion concentrations (<i>x</i> = 0.50) is stabilized. Subsequently, through a facile room-temperature K<sup>+</sup>/Na<sup>+</sup> ion-exchange process, sodium-deficient metastable P3-type Na<sub>0.5</sub>Cr<sub>0.5</sub>Ti<sub>0.5</sub>O<sub>2</sub> is successfully synthesized. A similar K<sup>+</sup>/Li<sup>+</sup> ion-exchange process is also applied to synthesize O3-type Li<sub>0.5</sub>Cr<sub>0.5</sub>Ti<sub>0.5</sub>O<sub>2</sub>. X-ray diffraction combined with electron microscopy reveals the formation of metastable single-phase P3-type Na<sub>0.5</sub>Cr<sub>0.5</sub>Ti<sub>0.5</sub>O<sub>2</sub> and metastable O3-type Li<sub>0.5</sub>Cr<sub>0.5</sub>Ti<sub>0.5</sub>O<sub>2</sub> with a unique layer arrangement. The high Na vacancy concentration in P3-type Na<sub>0.5</sub>Cr<sub>0.5</sub>Ti<sub>0.5</sub>O<sub>2</sub> results in an increased initial capacity of 125 mA h g<sup>−1</sup> at 10 mA g<sup>−1</sup>. Additionally, Na<sub>0.5</sub>Cr<sub>0.5</sub>Ti<sub>0.5</sub>O<sub>2</sub> exhibits Na<sup>+</sup>/vacancy disordering and high electronic conductivity, enabling a high-rate charge capability without sodium plating. This work provides new insights into the design of metastable layered materials for durable and safe sodium battery applications with fast-charge capability.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"183 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736846","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
An Optically Modulated Hydrogel Synapse for Multilevel Information Decryption
IF 19 1区 材料科学
Advanced Functional Materials Pub Date : 2025-03-30 DOI: 10.1002/adfm.202502784
Rui Zhou, Huasheng Tian, Hongyang Zhao, Li Ke, Haoyu Wu, Yaqing Liu, Jingcheng Hao
{"title":"An Optically Modulated Hydrogel Synapse for Multilevel Information Decryption","authors":"Rui Zhou, Huasheng Tian, Hongyang Zhao, Li Ke, Haoyu Wu, Yaqing Liu, Jingcheng Hao","doi":"10.1002/adfm.202502784","DOIUrl":"https://doi.org/10.1002/adfm.202502784","url":null,"abstract":"The increasing significance of data security promotes the development of multilevel information encryption and decryption techniques. However, the realization of logical outputs modulated by multiple stimuli is challenging in the design of advanced functional materials. Herein, a multilevel information decryption system with a combination of visual and digital outputs that responds to dual-optical inputs is developed based on a hydrogel-based synaptic device. ammonium molybdate nanoparticles and calcium alginate supramolecular networks is incorporated into a polyacrylamide hydrogel to enable optically regulated color change and ionic conductivity. Under UV irradiation, the reduction of the nanoparticles allows the hydrogel to change color as visual outputs. Meanwhile, the ionic conductivity of the hydrogel can be modulated by near-infrared (NIR) optical pulses to emulate the synaptic plasticity of biological synapses, producing NIR-mediated digital outputs. As a demonstration, a multilevel decryption strategy is provided using a hydrogel array that combines digital information decoding with visual information camouflage. Moreover, the short-term plasticity of the hydrogel synapse endows the system with time-dependent decryption, which improves information security and reduces the risk of data leakage. This study contributes to advancing multilevel decryption systems by providing an effective technique for integrating digital and visual decryption in hydrogel materials.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"4 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736854","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
Volatile to Non-Volatile Switching Transition in Chalcogenides
IF 19 1区 材料科学
Advanced Functional Materials Pub Date : 2025-03-30 DOI: 10.1002/adfm.202423940
Zihao Zhao, Mengfei Zhang, Qun Yang, Tamihiro Gotoh, Qingqin Ge, Nannan Shi, Yuting Sun, Jiayi Zhao, Yanping Sui, Ran Jiang, Haibin Yu, Stephen R. Elliott, Zhitang Song, Min Zhu
{"title":"Volatile to Non-Volatile Switching Transition in Chalcogenides","authors":"Zihao Zhao, Mengfei Zhang, Qun Yang, Tamihiro Gotoh, Qingqin Ge, Nannan Shi, Yuting Sun, Jiayi Zhao, Yanping Sui, Ran Jiang, Haibin Yu, Stephen R. Elliott, Zhitang Song, Min Zhu","doi":"10.1002/adfm.202423940","DOIUrl":"https://doi.org/10.1002/adfm.202423940","url":null,"abstract":"Over the past 60 years, three distinct electrical switching behaviors have been discovered in chalcogenides: ovonic threshold switch (OTS), ovonic memory switch (OMS), and phase-change switch (PCS). The first two have been successfully utilized in commercialized 3D Xpoint chips, serving as selector and memory cells, respectively. However, the relationships among these three behaviors remain unclear. Here, it is demonstrated that the Ge-Te binary system exhibits these three switching mechanisms. Specifically, the switching behavior transforms from PCS-like to OTS-like within the composition range from GeTe<sub>8</sub> to GeTe<sub>6</sub>, while the shift from volatile (OTS) to non-volatile switching behavior (OMS) occurs between the compositions GeTe<sub>2</sub> and GeTe. The PCS-to-OTS transition is primarily driven by enhancements in glass-forming ability, with the Turnbull parameter increasing from 0.58 to 0.6, and the crystallization temperature exceeding 145 °C, while the shift from OTS to OMS behavior is largely due to the significantly accelerated crystallization speed, from microseconds to nanoseconds. Most importantly, the GeTe<sub>16</sub> PCS stands out, with a large ON current (0.6 mA), low leakage current (&lt;2.5 × 10<sup>−8</sup> A), high endurance (&gt;6 × 10<sup>9</sup> cycles), and high-temperature back-end-of-line compatibility. The crystalline nature of this PCS material addresses the composition and toxicity issues in conventional OTS materials. Moreover, GeTe<sub>16</sub> PCSs have been successfully integrated with GeTe OMSs, forming selector/memory arrays with a read margin of 0.4 V. These findings not only reveal the mechanisms underlying the volatile to non-volatile transition but also provide an alternative solution for high-density 3D memory, potentially replacing the OTS/OMS stack approach.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"36 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736857","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
Enhancing Oxygen Reduction Reaction in PdHx@Pt Metallenes: Unveiling the Impact of Ligand Beyond Strain Effect
IF 19 1区 材料科学
Advanced Functional Materials Pub Date : 2025-03-30 DOI: 10.1002/adfm.202500522
Zhipeng Feng, Dongxu Jiao, Jinchang Fan, Yu Qiu, Xin Ge, Jiaqi Wang, Xiao Zhao, Wei Zhang, Lirong Zheng, Lei Zhang, Zhigen Yu, Weitao Zheng, Xiaoqiang Cui
{"title":"Enhancing Oxygen Reduction Reaction in PdHx@Pt Metallenes: Unveiling the Impact of Ligand Beyond Strain Effect","authors":"Zhipeng Feng, Dongxu Jiao, Jinchang Fan, Yu Qiu, Xin Ge, Jiaqi Wang, Xiao Zhao, Wei Zhang, Lirong Zheng, Lei Zhang, Zhigen Yu, Weitao Zheng, Xiaoqiang Cui","doi":"10.1002/adfm.202500522","DOIUrl":"https://doi.org/10.1002/adfm.202500522","url":null,"abstract":"Incorporating interstitial non-metal atoms within the crystal lattice of catalysts enables flexible modulation of their electronic structures and catalytic performances. However, the resulting induced tensile strain typically has a detrimental effect on oxygen reduction reaction (ORR) activity. In this study, a series of PdH<sub>x</sub>@Pt metallenes with varying H/Pd ratios, where hydrogen atoms precisely modulate the strain and ligand effects on the Pt skin surface is reported. Notably, PdH<sub>0.35</sub>@Pt metallenes exhibit an extraordinary half-wave potential of 0.933 V and a mass activity (MA) of 7.36 A mg<sub>Pt</sub><sup>−1</sup> at 0.9 V vs reversible hydrogen electrode (RHE) for ORR, outperforming both Pd@Pt metallenes and commercial Pt/C catalysts. Control experiments and density functional theory (DFT) calculations reveal a competitive relationship between strain and ligand effects across different H/Pd ratios, with a dominant positive ligand effect overcoming the negative strain effect at an H/Pd ratio of 0.35. This electronic structure modulation leads to an increased 5d electron density of the surface Pt and a downshift in the e<sub>g</sub><sup>*</sup> band center, thereby weakening the adsorption of oxygen intermediates on the Pt skin surface and resulting in excellent ORR activity.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"40 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143737173","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
Multifunctional Conductive Polymer Modification for Efficient CO2 Electroreduction in Acidic Electrolyte
IF 19 1区 材料科学
Advanced Functional Materials Pub Date : 2025-03-28 DOI: 10.1002/adfm.202425636
Lina Su, Qingfeng Hua, Guang Feng, Yanan Yang, Hao Mei, Yulv Yu, Xiaoxia Chang, Zhiqi Huang
{"title":"Multifunctional Conductive Polymer Modification for Efficient CO2 Electroreduction in Acidic Electrolyte","authors":"Lina Su, Qingfeng Hua, Guang Feng, Yanan Yang, Hao Mei, Yulv Yu, Xiaoxia Chang, Zhiqi Huang","doi":"10.1002/adfm.202425636","DOIUrl":"https://doi.org/10.1002/adfm.202425636","url":null,"abstract":"Electrode-electrolyte interfacial modification by hydrophobic molecules represents a promising strategy for suppressing competing proton reduction in acidic electrocatalytic carbon dioxide reduction reactions (CO<sub>2</sub>RR), meanwhile sacrificing extra overpotential due to increased ohmic resistance. Herein, a multifunctional conductive polymer, polyaniline modified by p-aminobenzenesulfonic acid (ABSA-polyaniline), is constructed between Cu catalyst layer and electrolyte to simultaneously create an ideal microenvironment for CO<sub>2</sub>RR and enhance the charge transfer and ion transport processes at the electrochemical reaction interface. This polymer layer balances the local hydrophobicity, promotes CO<sub>2</sub> adsorption and activation, and regulates the mass transport of K<sup>+</sup>, H<sup>+</sup>, and OH<sup>−</sup> ions, thus significantly enhancing the CO<sub>2</sub>RR kinetics in acidic medium, yielding a high Faraday efficiency (FE = 81%) for multicarbon products at 600 mA cm<sup>−2</sup>. More importantly, compared with commonly used hydrophobic molecules, the conductive nature of ABSA-PANI helps to reduce the ohmic resistance of the electrode, leading to notably lowered cathode overpotential at industrial-grade current density and improve cathode energy efficiency over a wide potential window. This work sheds light on the development of highly efficient acidic CO<sub>2</sub>RR systems, especially for those with low alkali cation concentrations and low CO<sub>2</sub> concentrations.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"33 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723949","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
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