Hui Peng, Danyang Wang, Xin Wang, Wenxing Miao, Jingtian Zeng, Bo Tao, Yue Li, Ying Tang, Guofu Ma
The stability of aqueous Z inc (Zn) ion energy storage devices is significantly compromised by the instability at the electrode/electrolyte interface, which can result in the growth of Zn dendrites, self‐corrosion, and various other side reactions. Regulating the Zn‐ion (Zn2+) solvation structure through electrolyte additives has been proved to be effective strategy in stabilizing the Zn anode, but the influence of free water on the solvation structure is often lacking in‐depth exploration. Herein, the piperazine‐N,N‐bis(2‐hydroxypropanesulfonic acid) sodium salt (POPSO‐Na) is presented as a multifunctional electrolyte additive, which enhances the stability of the Zn anode by modulating the deposition and stripping environment of Zn2⁺ and limiting the presence of free water in the electrolyte during cycling. Theoretical calculation and experimental results demonstrate that the POPSO‐Na additive can not only replace the structural water around Zn2+ to destroy the original solvation sheath, but also form reverse micelle interface structure to hinder the proton transition and constrain the free water in the electrolyte. Thus, the Zn||Zn battery utilizing the ZnSO4+POPSO‐Na electrolyte exhibits an impressive cycle life of 1600 h at a current density of 1 mA cm−2, achieving an average Coulomb efficiency (CE) of ≈100%, which is significantly better than that observed with the ZnSO4 electrolyte. Moreover, the Zn||Cu battery with ZnSO4+POPSO‐Na electrolyte achieves high stability even after cycling for over 2000 h.
{"title":"Coupling Solvation Structure Regulation and Interface Engineering via Reverse Micelle Strategy Toward Highly Stable Zn Metal Anode","authors":"Hui Peng, Danyang Wang, Xin Wang, Wenxing Miao, Jingtian Zeng, Bo Tao, Yue Li, Ying Tang, Guofu Ma","doi":"10.1002/adfm.202417695","DOIUrl":"https://doi.org/10.1002/adfm.202417695","url":null,"abstract":"The stability of aqueous Z inc (Zn) ion energy storage devices is significantly compromised by the instability at the electrode/electrolyte interface, which can result in the growth of Zn dendrites, self‐corrosion, and various other side reactions. Regulating the Zn‐ion (Zn<jats:sup>2+</jats:sup>) solvation structure through electrolyte additives has been proved to be effective strategy in stabilizing the Zn anode, but the influence of free water on the solvation structure is often lacking in‐depth exploration. Herein, the piperazine‐<jats:italic>N</jats:italic>,<jats:italic>N</jats:italic>‐bis(2‐hydroxypropanesulfonic acid) sodium salt (POPSO‐Na) is presented as a multifunctional electrolyte additive, which enhances the stability of the Zn anode by modulating the deposition and stripping environment of Zn<jats:sup>2</jats:sup>⁺ and limiting the presence of free water in the electrolyte during cycling. Theoretical calculation and experimental results demonstrate that the POPSO‐Na additive can not only replace the structural water around Zn<jats:sup>2+</jats:sup> to destroy the original solvation sheath, but also form reverse micelle interface structure to hinder the proton transition and constrain the free water in the electrolyte. Thus, the Zn||Zn battery utilizing the ZnSO<jats:sub>4</jats:sub>+POPSO‐Na electrolyte exhibits an impressive cycle life of 1600 h at a current density of 1 mA cm<jats:sup>−2</jats:sup>, achieving an average Coulomb efficiency (CE) of ≈100%, which is significantly better than that observed with the ZnSO<jats:sub>4</jats:sub> electrolyte. Moreover, the Zn||Cu battery with ZnSO<jats:sub>4</jats:sub>+POPSO‐Na electrolyte achieves high stability even after cycling for over 2000 h.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"37 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642943","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}
Wensun Zhu, Shitan Xu, Shoumeng Yang, Yang Yang, Xianhong Rui
Sodium‐ion batteries have drawn worldwide attention as ideal candidates for the upcoming generation of large‐scale electrical energy storage devices due to the low cost and abundance of sodium. Due to its unique electrochemical and chemical properties, sodium‐ion batteries hold the promise of breaking geographical and environmental constraints, achieving efficient sodium storage under low‐temperature conditions. However, low‐temperature sodium‐ion batteries, especially for their electrode materials, still face numerous challenges, such as the sluggish electrochemical reaction kinetics, poor material stability, significant volume changes leading to the pulverization of materials and the rapid degradation of battery performance. Here, it is focused on the modification methods for electrode materials, the research progress on cathode and anode materials of low‐temperature sodium‐ion batteries is summarized systematically and the other components of the electrodes are discussed briefly, and the shortcomings of the current research and possible future research directions are discussed thoroughly.
{"title":"Advanced Electrode Materials for Low‐Temperature Na Storage","authors":"Wensun Zhu, Shitan Xu, Shoumeng Yang, Yang Yang, Xianhong Rui","doi":"10.1002/adfm.202419173","DOIUrl":"https://doi.org/10.1002/adfm.202419173","url":null,"abstract":"Sodium‐ion batteries have drawn worldwide attention as ideal candidates for the upcoming generation of large‐scale electrical energy storage devices due to the low cost and abundance of sodium. Due to its unique electrochemical and chemical properties, sodium‐ion batteries hold the promise of breaking geographical and environmental constraints, achieving efficient sodium storage under low‐temperature conditions. However, low‐temperature sodium‐ion batteries, especially for their electrode materials, still face numerous challenges, such as the sluggish electrochemical reaction kinetics, poor material stability, significant volume changes leading to the pulverization of materials and the rapid degradation of battery performance. Here, it is focused on the modification methods for electrode materials, the research progress on cathode and anode materials of low‐temperature sodium‐ion batteries is summarized systematically and the other components of the electrodes are discussed briefly, and the shortcomings of the current research and possible future research directions are discussed thoroughly.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"6 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642890","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}
Anion exchange membrane fuel cells (AEMFCs) are advantageous for reducing or even eliminating the dependency on platinum resources, as the alkaline environment allows the use of non‐precious metal catalysts for oxygen reduction reaction at the cathode. However, the intrinsic activity of hydrogen oxidation reaction (HOR) catalysts in alkaline environments is 2 to 4 orders of magnitude lower than in acidic environments, which becomes the major challenge for AEMFCs. This review examines the current developments in the intrinsic activity of alkaline HOR catalysts and systematically summarizes the hydrogen activation mechanism with a focus on potential influencing factors and enhancement strategies. Furthermore, it offers insights into the prospects for developing more efficient alkaline HOR catalysts.
阴离子交换膜燃料电池(AEMFC)具有减少甚至消除对铂资源依赖的优势,因为碱性环境允许使用非贵金属催化剂在阴极进行氧还原反应。然而,碱性环境中氢氧化反应催化剂的内在活性比酸性环境中低 2 到 4 个数量级,这成为 AEMFCs 面临的主要挑战。本综述探讨了碱性 HOR 催化剂内在活性的最新进展,并系统总结了氢活化机理,重点介绍了潜在的影响因素和增强策略。此外,它还对开发更高效的碱性氢氧化还原催化剂的前景提出了见解。
{"title":"Intrinsic Activity: A Critical Challenge of Alkaline Hydrogen Oxidation Reaction","authors":"Xiaoyun Song, Qimei Yang, Kaisheng Zou, Zhenyang Xie, Jian Wang, Wei Ding","doi":"10.1002/adfm.202414570","DOIUrl":"https://doi.org/10.1002/adfm.202414570","url":null,"abstract":"Anion exchange membrane fuel cells (AEMFCs) are advantageous for reducing or even eliminating the dependency on platinum resources, as the alkaline environment allows the use of non‐precious metal catalysts for oxygen reduction reaction at the cathode. However, the intrinsic activity of hydrogen oxidation reaction (HOR) catalysts in alkaline environments is 2 to 4 orders of magnitude lower than in acidic environments, which becomes the major challenge for AEMFCs. This review examines the current developments in the intrinsic activity of alkaline HOR catalysts and systematically summarizes the hydrogen activation mechanism with a focus on potential influencing factors and enhancement strategies. Furthermore, it offers insights into the prospects for developing more efficient alkaline HOR catalysts.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"21 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642970","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}
Mark W. Young, Colter E. Oroke, Bruce E. Kirkpatrick, Michael R. Blatchley, Peter J. Dempsey, Kristi S. Anseth
As a model of the intestinal epithelium, intestinal stem cells (ISCs) are grown and differentiated as monolayers on materials where stochastic organization of the crypt and villi cells occurs. An allyl sulfide crosslinked photoresponsive hydrogel with a shear modulus of 1.6 kPa is developed and functionalized with GFOGER, Bm‐binder peptide ligands for monolayer growth of ISCs. The allyl sulfide chemistry allows in situ control of mechanics in the presence of growing ISC monolayers and structured irradiation affords spatial regulation of the hydrogel properties. Specifically, ISC monolayers grown on 1.6 kPa substrates are in situ softened to 0.29 kPa, using circular patterns 50, 75, and 100 µm in diameter, during differentiation, resulting in control over the size and arrangement of de novo crypts and monolayer cellularity. These photoresponsive materials should be useful in applications ranging from studying crypt evolution to drug screening and transport across tissues of changing cellular composition. Spatiotemporal softening enables control over the size and arrangement of de novo crypts within intestinal monolayers.
{"title":"Synthetic Photoresponsive Hydrogels Enable In Situ Control Over Murine Intestinal Monolayer Differentiation and Crypt Formation","authors":"Mark W. Young, Colter E. Oroke, Bruce E. Kirkpatrick, Michael R. Blatchley, Peter J. Dempsey, Kristi S. Anseth","doi":"10.1002/adfm.202413778","DOIUrl":"https://doi.org/10.1002/adfm.202413778","url":null,"abstract":"As a model of the intestinal epithelium, intestinal stem cells (ISCs) are grown and differentiated as monolayers on materials where stochastic organization of the crypt and villi cells occurs. An allyl sulfide crosslinked photoresponsive hydrogel with a shear modulus of 1.6 kPa is developed and functionalized with GFOGER, Bm‐binder peptide ligands for monolayer growth of ISCs. The allyl sulfide chemistry allows in situ control of mechanics in the presence of growing ISC monolayers and structured irradiation affords spatial regulation of the hydrogel properties. Specifically, ISC monolayers grown on 1.6 kPa substrates are in situ softened to 0.29 kPa, using circular patterns 50, 75, and 100 µm in diameter, during differentiation, resulting in control over the size and arrangement of de novo crypts and monolayer cellularity. These photoresponsive materials should be useful in applications ranging from studying crypt evolution to drug screening and transport across tissues of changing cellular composition. Spatiotemporal softening enables control over the size and arrangement of de novo crypts within intestinal monolayers.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"38 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642889","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}
Yiwei Sun, Wei Zhang, Zhiwen Luo, Can Zhu, Yiqun Zhang, Zheng Shu, Cailiang Shen, Xiaxi Yao, Yuanyin Wang, Xianwen Wang
Implant‐related infections are characterized by the formation of bacterial biofilms. Current treatments have various drawbacks. Nanozymes with enzyme‐like activity can produce highly toxic substances to kill bacteria and remove biofilms without inducing drug resistance. However, it is difficult for current monometallic nanozymes to function well in complex biofilm environments. Therefore, the development of multimetallic nanozymes with efficient multienzyme activities is crucial. In the present study, bimetallic nanozyme, ZnO‐CuS nanoflowers with peroxidase (POD), glutathione oxidase (GSH‐Px), and catalase (CAT) activity are successfully synthesized via calcination and loaded into F127 hydrogels for the treatment of implant‐related infections. The ability of ZnO‐CuS nanoflowers to bind bacteria is key for efficient antimicrobial activity. In addition, ZnO‐CuS nanoflowers with H2O2 disrupt the metabolism of MRSA, including arginine synthesis, nucleotide excision repair, energy metabolism, and protein synthesis. ZnO‐CuS/F127 hydrogel in combination with H2O2 has been demonstrated to be effective in clearing biofilm infection and facilitating the switch of M1 macrophages to M2‐repairative phenotype macrophages for the treatment of implant infections in mice. Furthermore, ZnO‐CuS/F127 hydrogels have favorable biosafety, and their toxicity is negligible. ZnO‐CuS/F127 hydrogel has provided a promising biomedical strategy for the healing of implant‐related infections, highlighting the potential of bimetallic nanozymes for clinical applications.
{"title":"ZnO‐CuS/F127 Hydrogels with Multienzyme Properties for Implant‐Related Infection Therapy by Inhibiting Bacterial Arginine Biosynthesis and Promoting Tissue Repair","authors":"Yiwei Sun, Wei Zhang, Zhiwen Luo, Can Zhu, Yiqun Zhang, Zheng Shu, Cailiang Shen, Xiaxi Yao, Yuanyin Wang, Xianwen Wang","doi":"10.1002/adfm.202415778","DOIUrl":"https://doi.org/10.1002/adfm.202415778","url":null,"abstract":"Implant‐related infections are characterized by the formation of bacterial biofilms. Current treatments have various drawbacks. Nanozymes with enzyme‐like activity can produce highly toxic substances to kill bacteria and remove biofilms without inducing drug resistance. However, it is difficult for current monometallic nanozymes to function well in complex biofilm environments. Therefore, the development of multimetallic nanozymes with efficient multienzyme activities is crucial. In the present study, bimetallic nanozyme, ZnO‐CuS nanoflowers with peroxidase (POD), glutathione oxidase (GSH‐Px), and catalase (CAT) activity are successfully synthesized via calcination and loaded into F127 hydrogels for the treatment of implant‐related infections. The ability of ZnO‐CuS nanoflowers to bind bacteria is key for efficient antimicrobial activity. In addition, ZnO‐CuS nanoflowers with H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub> disrupt the metabolism of <jats:italic>MRSA</jats:italic>, including arginine synthesis, nucleotide excision repair, energy metabolism, and protein synthesis. ZnO‐CuS/F127 hydrogel in combination with H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub> has been demonstrated to be effective in clearing biofilm infection and facilitating the switch of M1 macrophages to M2‐repairative phenotype macrophages for the treatment of implant infections in mice. Furthermore, ZnO‐CuS/F127 hydrogels have favorable biosafety, and their toxicity is negligible. ZnO‐CuS/F127 hydrogel has provided a promising biomedical strategy for the healing of implant‐related infections, highlighting the potential of bimetallic nanozymes for clinical applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"25 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642892","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}
Xin Ge, Zixuan Huang, Biao Shi, Pengyang Wang, Zhen Liu, You Gao, Xiaona Du, Ying Zhao, Xiaodan Zhang
Transforming perovskite solar cells into commercial production requires advanced scalable deposition technology. However, the deposition of high-quality perovskite thin films using the blade coating method presents challenges, especially in controlling the nucleation and crystallization of perovskite. In this work, an effective approach is proposed for controlling nucleation and crystallization by simultaneously incorporating two kinds of ionic liquid, namely 1H-imidazole acetate (IMAc), and 1-buty-3-methylimidazolium tetrafluoroborate (BMIMBF4), into the precursor solution. This innovative strategy initiates π–π interactions between IM and BMIM cations, thereby enhancing the interaction between cations and the Pb-I framework. The competitive mechanism of interaction with Pb-I framework effectively suppresses the formation of unfavorable mesophase, thereby enabling a single crystallization pathway from NMP + PbI2 to α-perovskite. Consequently, this method effectively reduces defects and enhances the crystal quality of α-perovskite film. Based on this strategy, the power conversion efficiency of the p-i-n wide bandgap perovskite device prepared by the blade coating method, is increased to 21.31%, representing one of the highest efficiencies achieved with this technology for 1.68 eV bandgap FACs-based perovskites. Thus, this approach emerges as a feasible breakthrough strategy that may unleash the full potential of perovskite solar cells.
{"title":"Crystallization Control of Blade-Coated Wide Bandgap FACs-Based Perovskite","authors":"Xin Ge, Zixuan Huang, Biao Shi, Pengyang Wang, Zhen Liu, You Gao, Xiaona Du, Ying Zhao, Xiaodan Zhang","doi":"10.1002/adfm.202417493","DOIUrl":"https://doi.org/10.1002/adfm.202417493","url":null,"abstract":"Transforming perovskite solar cells into commercial production requires advanced scalable deposition technology. However, the deposition of high-quality perovskite thin films using the blade coating method presents challenges, especially in controlling the nucleation and crystallization of perovskite. In this work, an effective approach is proposed for controlling nucleation and crystallization by simultaneously incorporating two kinds of ionic liquid, namely 1H-imidazole acetate (IMAc), and 1-buty-3-methylimidazolium tetrafluoroborate (BMIMBF<sub>4</sub>), into the precursor solution. This innovative strategy initiates <i>π</i>–<i>π</i> interactions between IM and BMIM cations, thereby enhancing the interaction between cations and the Pb-I framework. The competitive mechanism of interaction with Pb-I framework effectively suppresses the formation of unfavorable mesophase, thereby enabling a single crystallization pathway from NMP + PbI<sub>2</sub> to α-perovskite. Consequently, this method effectively reduces defects and enhances the crystal quality of α-perovskite film. Based on this strategy, the power conversion efficiency of the p-i-n wide bandgap perovskite device prepared by the blade coating method, is increased to 21.31%, representing one of the highest efficiencies achieved with this technology for 1.68 eV bandgap FACs-based perovskites. Thus, this approach emerges as a feasible breakthrough strategy that may unleash the full potential of perovskite solar cells.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"21 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642790","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}
Hygroscopic metal–organic frameworks (MOFs) are considered as superior moisture sorbents due to their highly adjustable and desired water adsorption/release performance, enabling effective atmospheric water harvesting (AWH) in arid regions. However, the water adsorption capacity, recycling stability, and functionality of current MOFs should be further improved to meet the requirements of practical AWH systems. Here the hydrophilicity at low relative humidity (RH) and cycling stability of MOF‐808 are simultaneously enhanced through the ethylenediaminetetraacetic acid (EDTA)‐mediated post‐modification. Based on the structural reinforcement, EDTA‐modified MOF‐808 (E‐MOF‐808) delivers a stable water uptake capacity of 0.39 g g−1 at 25% RH even after 50 water adsorption–desorption cycles, more than five times that of pristine MOF‐808. In addition, bridging by EDTA with the strong chelating ability, the E‐MOF‐808 can spontaneously capture Cu2+ for further functional improvement. Accordingly, light‐absorbing CuS nanoparticles can be in situ decorated on E‐MOF‐808 for facilitating solar‐driven water release. It is envisioned that this EDTA‐mediated function enhancement should provide valuable insights into the all‐in‐one design of versatile MOFs sorbents.
{"title":"Optimizing Hygroscopic Metal–Organic Frameworks via EDTA‐Mediated Structural Reinforcement and Photothermal Modification","authors":"Mingren Cheng, Xin Lian, Haoyu Bai, Xinsheng Wang, Jian Xu, Moyuan Cao, Xian‐He Bu","doi":"10.1002/adfm.202416241","DOIUrl":"https://doi.org/10.1002/adfm.202416241","url":null,"abstract":"Hygroscopic metal–organic frameworks (MOFs) are considered as superior moisture sorbents due to their highly adjustable and desired water adsorption/release performance, enabling effective atmospheric water harvesting (AWH) in arid regions. However, the water adsorption capacity, recycling stability, and functionality of current MOFs should be further improved to meet the requirements of practical AWH systems. Here the hydrophilicity at low relative humidity (RH) and cycling stability of MOF‐808 are simultaneously enhanced through the ethylenediaminetetraacetic acid (EDTA)‐mediated post‐modification. Based on the structural reinforcement, EDTA‐modified MOF‐808 (E‐MOF‐808) delivers a stable water uptake capacity of 0.39 g g<jats:sup>−1</jats:sup> at 25% RH even after 50 water adsorption–desorption cycles, more than five times that of pristine MOF‐808. In addition, bridging by EDTA with the strong chelating ability, the E‐MOF‐808 can spontaneously capture Cu<jats:sup>2+</jats:sup> for further functional improvement. Accordingly, light‐absorbing CuS nanoparticles can be in situ decorated on E‐MOF‐808 for facilitating solar‐driven water release. It is envisioned that this EDTA‐mediated function enhancement should provide valuable insights into the all‐in‐one design of versatile MOFs sorbents.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"48 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642893","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}
Yihui Gu, Wenjuan Wu, Chaofeng Zhang, Xinrui Li, Xinyu Guo, Yilin Wang, Yufeng Yuan, Bo Jiang, Yongcan Jin
A hydrogel that is expected as a biomedical load‐bearing material remains a substantial challenge. In this work, a multi‐solvent‐induced gradient aggregation state strategy is developed to construct lignin‐based supramolecular hydrogels that feature superstrong, tough, stretchable, and fatigue‐resistant properties. The multi‐solvent high‐temperature annealing induces the gradient crystallization of polyvinyl alcohol and the self‐assembly of lignin. The interior strong hydrogen‐binding and the external weak non‐covalent‐binding forms a gradient aggregation state microstructure and compact macrostructure, where lignin acts as an interfacial molecular bridge. By sharing interconnection points to collaboratively dissipate energy, the developed hydrogels demonstrate high modulus (74.4 MPa), toughness (90 MJ m−3), tear (34,000 J m−2), tensile (24.8 MPa), and compressive strength (60 MPa). Moreover, such lignin‐based supramolecular hydrogels also exhibit extraordinary fatigue resistance, biocompatibility, and reactive oxygen species scavenging activity. This gradient non‐covalent conjoined‐network caused by multi‐solvent high‐temperature annealing provides a new design strategy and potential for developing biomaterials that mimic biomedical load‐bearing materials (e.g., natural tendons and ligaments).
{"title":"Multi‐Solvent‐Induced Gradient Aggregation Rendered Superstrong, Tough, Stretchable, and Fatigue‐Resistant Lignin‐Based Supramolecular Hydrogels","authors":"Yihui Gu, Wenjuan Wu, Chaofeng Zhang, Xinrui Li, Xinyu Guo, Yilin Wang, Yufeng Yuan, Bo Jiang, Yongcan Jin","doi":"10.1002/adfm.202417206","DOIUrl":"https://doi.org/10.1002/adfm.202417206","url":null,"abstract":"A hydrogel that is expected as a biomedical load‐bearing material remains a substantial challenge. In this work, a multi‐solvent‐induced gradient aggregation state strategy is developed to construct lignin‐based supramolecular hydrogels that feature superstrong, tough, stretchable, and fatigue‐resistant properties. The multi‐solvent high‐temperature annealing induces the gradient crystallization of polyvinyl alcohol and the self‐assembly of lignin. The interior strong hydrogen‐binding and the external weak non‐covalent‐binding forms a gradient aggregation state microstructure and compact macrostructure, where lignin acts as an interfacial molecular bridge. By sharing interconnection points to collaboratively dissipate energy, the developed hydrogels demonstrate high modulus (74.4 MPa), toughness (90 MJ m<jats:sup>−3</jats:sup>), tear (34,000 J m<jats:sup>−2</jats:sup>), tensile (24.8 MPa), and compressive strength (60 MPa). Moreover, such lignin‐based supramolecular hydrogels also exhibit extraordinary fatigue resistance, biocompatibility, and reactive oxygen species scavenging activity. This gradient non‐covalent conjoined‐network caused by multi‐solvent high‐temperature annealing provides a new design strategy and potential for developing biomaterials that mimic biomedical load‐bearing materials (e.g., natural tendons and ligaments).","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"8 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642894","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}
Yeon‐Woo Seong, Hoedon Kwon, Changwoo Lee, Hyeonwook Lim, Kwnagsik Jeong, Hee Jun Shin, Mann‐Ho Cho
Ovonic threshold switching (OTS), characterized by a rapid resistance drop in chalcogenide glass, has enabled the realization of memory and selectors. Despite over five decades of development, the challenges in characterizing the transient switching in amorphous materials upon reaching the threshold voltage have hindered the establishment of its underlying mechanism. This study uses femtosecond terahertz spectroscopy and ab initio simulation to elucidate the dynamics of the free‐carrier and IR‐active phonons involved in OTS. Specifically, in Te‐rich amorphous GeTe, the generation of transient phonons is observed within picoseconds, a phenomenon associated with an increased Born effective charge due to the alignment of Te‐centered bonds. The findings demonstrate a correlation between the enhancement of polarizability, due to orbital alignment during the disorder–order structural transition while maintaining a macroscopic amorphous structure, and the switching behavior. These results provide valuable insights into the enigmatic OTS phenomenon.
以掺杂镓玻璃中电阻快速下降为特征的椭圆阈值开关(OTS),使存储器和选择器得以实现。尽管经过了五十多年的发展,但在表征非晶材料达到阈值电压时的瞬态开关时所面临的挑战阻碍了其基本机制的建立。本研究利用飞秒太赫兹光谱和 ab initio 模拟来阐明参与 OTS 的自由载流子和红外活性声子的动力学。具体来说,在富含碲的非晶态 GeTe 中,可在皮秒内观察到瞬态声子的产生,这种现象与碲中心键的排列导致的 Born 有效电荷增加有关。研究结果表明,在保持宏观非晶结构的同时,无序结构转变过程中轨道排列导致的极化能力增强与开关行为之间存在关联。这些结果为研究神秘的 OTS 现象提供了宝贵的见解。
{"title":"Transient Structural Transition in Ovonic Threshold Switching Glass","authors":"Yeon‐Woo Seong, Hoedon Kwon, Changwoo Lee, Hyeonwook Lim, Kwnagsik Jeong, Hee Jun Shin, Mann‐Ho Cho","doi":"10.1002/adfm.202415462","DOIUrl":"https://doi.org/10.1002/adfm.202415462","url":null,"abstract":"Ovonic threshold switching (OTS), characterized by a rapid resistance drop in chalcogenide glass, has enabled the realization of memory and selectors. Despite over five decades of development, the challenges in characterizing the transient switching in amorphous materials upon reaching the threshold voltage have hindered the establishment of its underlying mechanism. This study uses femtosecond terahertz spectroscopy and ab initio simulation to elucidate the dynamics of the free‐carrier and IR‐active phonons involved in OTS. Specifically, in Te‐rich amorphous GeTe, the generation of transient phonons is observed within picoseconds, a phenomenon associated with an increased Born effective charge due to the alignment of Te‐centered bonds. The findings demonstrate a correlation between the enhancement of polarizability, due to orbital alignment during the disorder–order structural transition while maintaining a macroscopic amorphous structure, and the switching behavior. These results provide valuable insights into the enigmatic OTS phenomenon.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"39 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642900","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}
Upgrading the available dielectric materials is the most effective approach to solve the poor quality of signal transmission and heat buildup caused by high density integration. In this work, a design strategy for multilayer 3D porous composite networks is proposed, relying on the self‐assembly effect of “crystal‐like phase” to achieve the synergistic optimization of low permittivity and high thermal conductivity of polyimide. The obtained three‐layer porous polyimide composite film (PSLS) features an ultralow permittivity of 1.89, an in‐plane thermal conductivity as high as 13.58 W m−1 K−1, and maintains well electrical insulating property. Inspiringly, the first digital thermoacoustic generator with wide frequency response has been designed based on PSLS film. It achieves sound pressure levels up to 60.1 dB in the 20–100 kHz range and integrates the efficient sound generation of an ultrasonic generator with real‐time display. This work will provide a novel concept material for the smart electronics and electrical fields.
要解决高密度集成带来的信号传输质量差和热量积聚问题,提升现有介电材料是最有效的方法。本文提出了一种多层三维多孔复合网络的设计策略,依靠 "类晶相 "的自组装效应,实现了聚酰亚胺低介电常数和高导热系数的协同优化。所获得的三层多孔聚酰亚胺复合薄膜(PSLS)具有 1.89 的超低介电常数、高达 13.58 W m-1 K-1 的面内热导率和良好的电绝缘性能。令人鼓舞的是,基于 PSLS 薄膜设计出了第一台具有宽频率响应的数字热声发生器。它能在 20-100 kHz 范围内实现高达 60.1 dB 的声压级,并集成了超声波发生器的高效发声和实时显示功能。这项工作将为智能电子和电气领域提供一种新型概念材料。
{"title":"Coordination of Ultralow Permittivity and Higher Thermal Conductivity of Polyimide Induced by Unique Interfacial Self‐Assembly Behavior","authors":"Xiaodi Dong, Baoquan Wan, Langbiao Huang, Quanliang Zhao, Ruifeng Yao, Jinghui Gao, Can Ding, Xu Wang, Zhi‐Min Dang, George Chen, Jun‐Wei Zha","doi":"10.1002/adfm.202417843","DOIUrl":"https://doi.org/10.1002/adfm.202417843","url":null,"abstract":"Upgrading the available dielectric materials is the most effective approach to solve the poor quality of signal transmission and heat buildup caused by high density integration. In this work, a design strategy for multilayer 3D porous composite networks is proposed, relying on the self‐assembly effect of “crystal‐like phase” to achieve the synergistic optimization of low permittivity and high thermal conductivity of polyimide. The obtained three‐layer porous polyimide composite film (PSLS) features an ultralow permittivity of 1.89, an in‐plane thermal conductivity as high as 13.58 W m<jats:sup>−1</jats:sup> K<jats:sup>−1</jats:sup>, and maintains well electrical insulating property. Inspiringly, the first digital thermoacoustic generator with wide frequency response has been designed based on PSLS film. It achieves sound pressure levels up to 60.1 dB in the 20–100 kHz range and integrates the efficient sound generation of an ultrasonic generator with real‐time display. This work will provide a novel concept material for the smart electronics and electrical fields.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"94 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642967","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}