Pub Date : 2025-04-26DOI: 10.1016/j.jmst.2025.03.044
Zhanpeng Sun, Junjie Zou, Rui Li, Zhaofu Zhang, Junqi Mai, Zijun Qi, David Vazquez Cortes, Qijun Wang, Gai Wu, Wei Shen, Sheng Liu
Gallium oxide (Ga2O3) is an ultra-wide bandgap semiconductor with excellent potential for high-power and ultraviolet optoelectronic device applications. High-performance Ga2O3-based high-power devices rely heavily on precise processing, especially in wafer dicing. Laser stealth dicing (LSD) is an innovative laser technology that utilizes a focused laser to create subsurface modifications in the wafer without surface damage. LSD has broad application prospects in the field of semiconductor precision processing. In this work, the idea of achieving high-quality dicing of β-Ga2O3 wafers via LSD was proposed. A combination of atomistic simulations and experiments was used to understand the underlying mechanism of LSD of β-Ga2O3 wafers. On the one hand, the laser loading and fracture process of β-Ga2O3 wafers were simulated using molecular dynamics (MD) methods as well as a machine learning potential. The effects of single-pulse energy on LSD were analyzed through the lattice residual pressure, the final total energy of the system, the internal atomic strain, and the maximum stress value during uniaxial tension. On the other hand, based on the MD simulations, LSD was successfully performed on β-Ga2O3 wafers along three main crystal planes in the laboratory, resulting in good surface quality. This work not only provides profound optimization strategies for the LSD process of β-Ga2O3, establishing the foundation for high-quality dicing of β-Ga2O3 wafers, but also verifies the accuracy of MD simulations in predicting trends related to the LSD, offering a potential approach for high-quality dicing of other materials in future research.
{"title":"Laser stealth dicing of β-Ga2O3: Theoretical and experimental studies","authors":"Zhanpeng Sun, Junjie Zou, Rui Li, Zhaofu Zhang, Junqi Mai, Zijun Qi, David Vazquez Cortes, Qijun Wang, Gai Wu, Wei Shen, Sheng Liu","doi":"10.1016/j.jmst.2025.03.044","DOIUrl":"https://doi.org/10.1016/j.jmst.2025.03.044","url":null,"abstract":"Gallium oxide (Ga<sub>2</sub>O<sub>3</sub>) is an ultra-wide bandgap semiconductor with excellent potential for high-power and ultraviolet optoelectronic device applications. High-performance Ga<sub>2</sub>O<sub>3</sub>-based high-power devices rely heavily on precise processing, especially in wafer dicing. Laser stealth dicing (LSD) is an innovative laser technology that utilizes a focused laser to create subsurface modifications in the wafer without surface damage. LSD has broad application prospects in the field of semiconductor precision processing. In this work, the idea of achieving high-quality dicing of β-Ga<sub>2</sub>O<sub>3</sub> wafers via LSD was proposed. A combination of atomistic simulations and experiments was used to understand the underlying mechanism of LSD of β-Ga<sub>2</sub>O<sub>3</sub> wafers. On the one hand, the laser loading and fracture process of β-Ga<sub>2</sub>O<sub>3</sub> wafers were simulated using molecular dynamics (MD) methods as well as a machine learning potential. The effects of single-pulse energy on LSD were analyzed through the lattice residual pressure, the final total energy of the system, the internal atomic strain, and the maximum stress value during uniaxial tension. On the other hand, based on the MD simulations, LSD was successfully performed on β-Ga<sub>2</sub>O<sub>3</sub> wafers along three main crystal planes in the laboratory, resulting in good surface quality. This work not only provides profound optimization strategies for the LSD process of β-Ga<sub>2</sub>O<sub>3</sub>, establishing the foundation for high-quality dicing of β-Ga<sub>2</sub>O<sub>3</sub> wafers, but also verifies the accuracy of MD simulations in predicting trends related to the LSD, offering a potential approach for high-quality dicing of other materials in future research.","PeriodicalId":16154,"journal":{"name":"Journal of Materials Science & Technology","volume":"33 1","pages":""},"PeriodicalIF":10.9,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875816","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}
Pub Date : 2025-04-26DOI: 10.1016/j.nantod.2025.102776
Gaoxiang Xu , Mengke Wang , Qing Li , Lianghui Fan , Runpu Shen , Zhikang Xiao , Jianzhong Xu , Kun Wang , Junyang Chen
The maintenance of an optimal inflammatory homeostasis within the body is crucial for its sustained viability within a natural environment replete with pathogenic factors. The real-time, precise detection of two antagonistic cytokines (pro- and anti-inflammatory) in an inflammatory state is fundamental to the guidance of precise clinical treatments and thus the achievement of inflammatory homeostasis. Herein, we synthesized AuAg-ZIF, which resulted in a dual enhancement of the fluorescence properties of AuNCs (35-fold increase in fluorescence intensity and 18.5-fold increase in quantum yield) by the anti-galvanic reaction between the surface Ag(I) and core Au (0), as well as by the confinement effect of ZIF-8. Furthermore, a generalized fluorescence immunoassay utilizing liposome-mediated Cu2 +-induced fluorescence quenching of AuAg-ZIF has been developed, resulting in amplification of the antigenic signal. Additionally, an interpretable machine learning prediction algorithm was constructed, comprising feature extraction, feature dimensionality reduction, model construction and validation, and model interpretation. This algorithm achieves immediate and accurate detection of factors related to anti-inflammatory, pro-inflammatory, and inflammatory levels in the human inflammatory homeostasis (R2 > 0.95), which is in line with the accuracy of the current commercial assay kits. This integration of dual-enhanced fluorescent nanoscale materials, amplification strategies, and interpretable machine learning enables the real-time, accurate observation of inflammatory homeostasis, thereby facilitating the delivery of precision clinical treatments.
{"title":"Self-assembled Gold@silver-ZIF structure-induced dual-enhancement luminescence synergized with interpretable machine learning empower precise monitoring of inflammatory homeostasis","authors":"Gaoxiang Xu , Mengke Wang , Qing Li , Lianghui Fan , Runpu Shen , Zhikang Xiao , Jianzhong Xu , Kun Wang , Junyang Chen","doi":"10.1016/j.nantod.2025.102776","DOIUrl":"10.1016/j.nantod.2025.102776","url":null,"abstract":"<div><div>The maintenance of an optimal inflammatory homeostasis within the body is crucial for its sustained viability within a natural environment replete with pathogenic factors. The real-time, precise detection of two antagonistic cytokines (pro- and anti-inflammatory) in an inflammatory state is fundamental to the guidance of precise clinical treatments and thus the achievement of inflammatory homeostasis. Herein, we synthesized AuAg-ZIF, which resulted in a dual enhancement of the fluorescence properties of AuNCs (35-fold increase in fluorescence intensity and 18.5-fold increase in quantum yield) by the anti-galvanic reaction between the surface Ag(I) and core Au (0), as well as by the confinement effect of ZIF-8. Furthermore, a generalized fluorescence immunoassay utilizing liposome-mediated Cu<sup>2 +</sup>-induced fluorescence quenching of AuAg-ZIF has been developed, resulting in amplification of the antigenic signal. Additionally, an interpretable machine learning prediction algorithm was constructed, comprising feature extraction, feature dimensionality reduction, model construction and validation, and model interpretation. This algorithm achieves immediate and accurate detection of factors related to anti-inflammatory, pro-inflammatory, and inflammatory levels in the human inflammatory homeostasis (R<sup>2</sup> > 0.95), which is in line with the accuracy of the current commercial assay kits. This integration of dual-enhanced fluorescent nanoscale materials, amplification strategies, and interpretable machine learning enables the real-time, accurate observation of inflammatory homeostasis, thereby facilitating the delivery of precision clinical treatments.</div></div>","PeriodicalId":395,"journal":{"name":"Nano Today","volume":"64 ","pages":"Article 102776"},"PeriodicalIF":13.2,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143873801","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}
Polymer electrolyte membrane fuel cells (PEMFCs) have become a promising technology due to their high efficiency and zero emission of toxic gases. The present work deals with the fabrication of a cost-efficient nanocomposite proton exchange membrane (PEM), prepared by incorporation of graphene oxide (GO) prepared in the laboratory by modified Hummer's method and thermo-mechanically modified Fly Ash (FA) within the host PVDF [poly(vinylidene fluoride)] polymer matrix. Subsequently, the nanocomposite membranes were treated with the well-known sulfonating agent chlorosulfonic acid at 60 °C for 30 min. The incorporation of GO and FA nanoparticles into the polymer matrix and the membrane sulfonation was verified using various spectroscopic methods, including XRD, FTIR, Laser Raman, FESEM-EDX, and AFM analyses. The highest ion exchange capacity (IEC) and proton conductivity (PC) are observed to be 0.88 meq g−1 and 4.08 × 10−2 S/cm respectively for the fabricated membrane SPGF-3. Further, it was interesting to note that with an increase in temperature from 25 °C to 75 °C, the fabricated membrane (SPGF-3) exhibited enhanced water uptake capacity from 25.6 % to 30.6 % respectively. The fuel cell performance test showed that the sulfonated membrane, composed of 95 wt% PVDF, 2.5 wt% GO, and 2.5 wt% FA, achieved a maximum current density of 1000 mA cm−2 and a power density of 448 mW cm−2 which quantifies its potency towards an alternative to costly Nafion membranes for PEMFCs application.
{"title":"Development of functionalized nanocomposite membrane composed of sulfonated PVDF/GO and thermo-mechanically modified Fly-Ash for application in PEMFCs","authors":"Ravi Bhushan Pathak , Anand Prakash Mishra , Vijay Varma , Piyush Kumar","doi":"10.1016/j.ssi.2025.116870","DOIUrl":"10.1016/j.ssi.2025.116870","url":null,"abstract":"<div><div>Polymer electrolyte membrane fuel cells (PEMFCs) have become a promising technology due to their high efficiency and zero emission of toxic gases. The present work deals with the fabrication of a cost-efficient nanocomposite proton exchange membrane (PEM), prepared by incorporation of graphene oxide (GO) prepared in the laboratory by modified Hummer's method and thermo-mechanically modified Fly Ash (FA) within the host PVDF [poly(vinylidene fluoride)] polymer matrix. Subsequently, the nanocomposite membranes were treated with the well-known sulfonating agent chlorosulfonic acid at 60 °C for 30 min. The incorporation of GO and FA nanoparticles into the polymer matrix and the membrane sulfonation was verified using various spectroscopic methods, including XRD, FTIR, Laser Raman, FESEM-EDX, and AFM analyses. The highest ion exchange capacity (IEC) and proton conductivity (PC) are observed to be 0.88 meq g<sup>−1</sup> and 4.08 × 10<sup>−2</sup> S/cm respectively for the fabricated membrane SPGF-3. Further, it was interesting to note that with an increase in temperature from 25 °C to 75 °C, the fabricated membrane (SPGF-3) exhibited enhanced water uptake capacity from 25.6 % to 30.6 % respectively. The fuel cell performance test showed that the sulfonated membrane, composed of 95 wt% PVDF, 2.5 wt% GO, and 2.5 wt% FA, achieved a maximum current density of 1000 mA cm<sup>−2</sup> and a power density of 448 mW cm<sup>−2</sup> which quantifies its potency towards an alternative to costly Nafion membranes for PEMFCs application.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"425 ","pages":"Article 116870"},"PeriodicalIF":3.0,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143874314","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-26DOI: 10.1016/j.porgcoat.2025.109335
Dashuai Yan , Zhen Chen , Wenjuan Zhang , Yanli Wang , Liman Chen
Most conventional organic anti-corrosion coatings cannot provide long-term protection for metals due to their limited functionality. Here, a smart anti-corrosion coating (ZLIP/EP) is developed by incorporating a 2D/3D structure-function integrated nanomaterial (ZLIP) into the coating matrix. ZLIP consists of polyethylene glycol (PEG)-encapsulated dodecahedral layered double hydroxide (LDH) nanocages, which contain corrosion inhibitor imidazoline (IM). Compared to ZIF-67 added to the coating, the 2D LDH layers of ZLIP can effectively extend the electrolyte solution's penetration path within the coating. When the composite coating is damaged, the LDH layers can capture chloride ions in the electrolyte solution, while IM is released to suppress corrosion. Moreover, the IM stored in the unique 3D hollow structure of ZLIP can also be released and subsequently adsorbed onto the steel substrate to further improve the active corrosion protection ability of the coating. The electrochemical test reveal that the |Z|0.01Hz of ZLIP/EP remains as high as 68.8 MΩ·cm2 after long-term immersion (40 days), demonstrating superior corrosion resistance. The ZLIP/EP system developed in this study shows significant promise for practical anti-corrosion applications.
{"title":"Multifunctional anti-corrosion coatings based on 2D/3D structure-function integrated nanomaterials for steel protection","authors":"Dashuai Yan , Zhen Chen , Wenjuan Zhang , Yanli Wang , Liman Chen","doi":"10.1016/j.porgcoat.2025.109335","DOIUrl":"10.1016/j.porgcoat.2025.109335","url":null,"abstract":"<div><div>Most conventional organic anti-corrosion coatings cannot provide long-term protection for metals due to their limited functionality. Here, a smart anti-corrosion coating (ZLIP/EP) is developed by incorporating a 2D/3D structure-function integrated nanomaterial (ZLIP) into the coating matrix. ZLIP consists of polyethylene glycol (PEG)-encapsulated dodecahedral layered double hydroxide (LDH) nanocages, which contain corrosion inhibitor imidazoline (IM). Compared to ZIF-67 added to the coating, the 2D LDH layers of ZLIP can effectively extend the electrolyte solution's penetration path within the coating. When the composite coating is damaged, the LDH layers can capture chloride ions in the electrolyte solution, while IM is released to suppress corrosion. Moreover, the IM stored in the unique 3D hollow structure of ZLIP can also be released and subsequently adsorbed onto the steel substrate to further improve the active corrosion protection ability of the coating. The electrochemical test reveal that the |Z|<sub>0.01Hz</sub> of ZLIP/EP remains as high as 68.8 MΩ·cm<sup>2</sup> after long-term immersion (40 days), demonstrating superior corrosion resistance. The ZLIP/EP system developed in this study shows significant promise for practical anti-corrosion applications.</div></div>","PeriodicalId":20834,"journal":{"name":"Progress in Organic Coatings","volume":"206 ","pages":"Article 109335"},"PeriodicalIF":6.5,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143873319","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
As a ubiquitous substance in nature, ice has attracted substantial research interest across a variety of fields, including physics, environmental science, biology, and cryopreservation. However, the intricate structural transformations within ice remain elusive owing to the stringent experimental constraints. Herein, the detailed evolution of ice nanopores, including expansion and healing, is investigated using advanced cryo‐electron microscopy combined with low‐dose techniques, and the underlying mechanisms are revealed through surface‐free energy analysis. Three pivotal factors are identified as driving the evolution mechanism of ice nanopores: the nanopore geometry and dimensions and the thickness of the ice film. This research not only provides novel insights into the dynamic structural evolution of ice at the molecular scale but also paves the way for a deeper understanding of the fundamental properties and behaviors of ice. Moreover, the healing mechanism of the nanopores is anticipated to be utilized in ice manipulation and nanofabrication.
{"title":"Unveiling the Healing Mechanism of Nanopores in Ice Films","authors":"Pengfei Nan, Kang Wu, Qizhu Li, Yangrui Liu, Hongzheng Wang, Yangjian Lin, Jinlong Zhu, Jing Wu, Fang Lin, Yumei Wang, Binghui Ge","doi":"10.1002/smll.202502245","DOIUrl":"https://doi.org/10.1002/smll.202502245","url":null,"abstract":"As a ubiquitous substance in nature, ice has attracted substantial research interest across a variety of fields, including physics, environmental science, biology, and cryopreservation. However, the intricate structural transformations within ice remain elusive owing to the stringent experimental constraints. Herein, the detailed evolution of ice nanopores, including expansion and healing, is investigated using advanced cryo‐electron microscopy combined with low‐dose techniques, and the underlying mechanisms are revealed through surface‐free energy analysis. Three pivotal factors are identified as driving the evolution mechanism of ice nanopores: the nanopore geometry and dimensions and the thickness of the ice film. This research not only provides novel insights into the dynamic structural evolution of ice at the molecular scale but also paves the way for a deeper understanding of the fundamental properties and behaviors of ice. Moreover, the healing mechanism of the nanopores is anticipated to be utilized in ice manipulation and nanofabrication.","PeriodicalId":228,"journal":{"name":"Small","volume":"15 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875741","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Developing highly efficient oxygen evolution reaction (OER) electrocatalysts is critical for hydrogen production through electrocatalytic water splitting, yet it remains a significant challenge. In this study, a novel OER electrocatalyst, Fe‐doped Ni‐phytate supported on carbon nanotubes (NiFe‐phy/CNT), which simultaneously follows lattice oxygen mechanism (LOM) and exhibits a photothermal effect, is synthesized through a facile and scalable co‐precipitation method. Experimental results combined with theoretical calculations indicate that introducing Fe can facilitate the structural reconstruction of NiFe‐phy/CNT to form highly active NiFe oxyhydroxides, switch OER pathway to LOM from the adsorbate evolution mechanism, and reinforce the photothermal effect to counterbalance the enthalpy change during OER process while reducing its activation energy. Therefore, under near‐infrared light irradiation, NiFe‐phy/CNT demonstrates exceptional OER activity, featuring low overpotentials of 237, 275, and 286 mV at 100, 500, and 1000 mA cm−2, respectively. Moreover, this electrocatalyst demonstrates the capability of large‐scale synthesis and can be stored for over 120 days with a negligible decrease in activity. This work presents a novel conceptual approach to integrate lattice oxygen redox chemistry with photothermal effect for designing highly efficient OER electrocatalysts.
{"title":"Fe‐Doped Ni‐Phytate/Carbon Nanotube Hybrids Integrating Activated Lattice Oxygen Participation and Enhanced Photothermal Effect for Highly Efficient Oxygen Evolution Reaction Electrocatalyst","authors":"Peng Guan, Yuehua Zhang, Jialin Wang, Qing Ye, Yonghui Tian, Yanxia Zhao, Yongliang Cheng","doi":"10.1002/smll.202502294","DOIUrl":"https://doi.org/10.1002/smll.202502294","url":null,"abstract":"Developing highly efficient oxygen evolution reaction (OER) electrocatalysts is critical for hydrogen production through electrocatalytic water splitting, yet it remains a significant challenge. In this study, a novel OER electrocatalyst, Fe‐doped Ni‐phytate supported on carbon nanotubes (NiFe‐phy/CNT), which simultaneously follows lattice oxygen mechanism (LOM) and exhibits a photothermal effect, is synthesized through a facile and scalable co‐precipitation method. Experimental results combined with theoretical calculations indicate that introducing Fe can facilitate the structural reconstruction of NiFe‐phy/CNT to form highly active NiFe oxyhydroxides, switch OER pathway to LOM from the adsorbate evolution mechanism, and reinforce the photothermal effect to counterbalance the enthalpy change during OER process while reducing its activation energy. Therefore, under near‐infrared light irradiation, NiFe‐phy/CNT demonstrates exceptional OER activity, featuring low overpotentials of 237, 275, and 286 mV at 100, 500, and 1000 mA cm<jats:sup>−2</jats:sup>, respectively. Moreover, this electrocatalyst demonstrates the capability of large‐scale synthesis and can be stored for over 120 days with a negligible decrease in activity. This work presents a novel conceptual approach to integrate lattice oxygen redox chemistry with photothermal effect for designing highly efficient OER electrocatalysts.","PeriodicalId":228,"journal":{"name":"Small","volume":"78 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875745","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Abhishek Kumar, Charles H. Devillers, Rita Meunier‐Prest, Dimitri Sabat, Eric Lesniewska, Marcel Bouvet
Interface engineering in organic heterostructures is an important approach to tuning the characteristics of organic electronic devices and improving their performances in applications, such as gas sensing. Herein, organic heterostructures containing, a polyporphine (pZnP‐1), perfluorinated copper phthalocyanine (Cu(F16Pc)), and lutetium bis‐phthalocyanine (LuPc2) are synthesized by a combination of electrochemical and PVD methods for investigation of charge transport and ammonia (NH3) sensing application. pZnP‐1 is synthesized by controlled oxidative electropolymerization and reveals a rough surface, which influences the electrical nature of its interface with the phthalocyanine. The electrical properties of the heterojunction devices reveal distinct interfacial and bulk charge transport properties, which are modulated by the thickness of pZnP‐1 and the external electric field. Indeed, the heterojunction device containing a thin film of pZnP‐1 displays n‐type behavior at low bias and p‐type nature at higher bias; i.e., an ambipolar behavior, in which ambipolarity is triggered by the external electric field. On the other hand, the heterojunction device having a thick film of pZnP‐1 exhibits p‐type behavior at all the studied biases. Investigation of NH3 sensing properties of the heterojunction devices highlights the advantages of introducing pZnP‐1 in the heterostructures, which enhances the sensitivity, stability, repeatability, and humidity tolerance of the sensors.
{"title":"Bias Induced Ambipolar Transport in Organic Heterojunction Sensors","authors":"Abhishek Kumar, Charles H. Devillers, Rita Meunier‐Prest, Dimitri Sabat, Eric Lesniewska, Marcel Bouvet","doi":"10.1002/aelm.202400865","DOIUrl":"https://doi.org/10.1002/aelm.202400865","url":null,"abstract":"Interface engineering in organic heterostructures is an important approach to tuning the characteristics of organic electronic devices and improving their performances in applications, such as gas sensing. Herein, organic heterostructures containing, a polyporphine (pZnP‐1), perfluorinated copper phthalocyanine (Cu(F<jats:sub>16</jats:sub>Pc)), and lutetium bis‐phthalocyanine (LuPc<jats:sub>2</jats:sub>) are synthesized by a combination of electrochemical and PVD methods for investigation of charge transport and ammonia (NH<jats:sub>3</jats:sub>) sensing application. pZnP‐1 is synthesized by controlled oxidative electropolymerization and reveals a rough surface, which influences the electrical nature of its interface with the phthalocyanine. The electrical properties of the heterojunction devices reveal distinct interfacial and bulk charge transport properties, which are modulated by the thickness of pZnP‐1 and the external electric field. Indeed, the heterojunction device containing a thin film of pZnP‐1 displays n‐type behavior at low bias and p‐type nature at higher bias; i.e., an ambipolar behavior, in which ambipolarity is triggered by the external electric field. On the other hand, the heterojunction device having a thick film of pZnP‐1 exhibits p‐type behavior at all the studied biases. Investigation of NH<jats:sub>3</jats:sub> sensing properties of the heterojunction devices highlights the advantages of introducing pZnP‐1 in the heterostructures, which enhances the sensitivity, stability, repeatability, and humidity tolerance of the sensors.","PeriodicalId":110,"journal":{"name":"Advanced Electronic Materials","volume":"33 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875892","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Alexis Wolfel, Castro Johnbosco, Annalise Anspach, Marieke Meteling, Jos Olijve, Niklas Felix König, Jeroen Leijten
Light‐based volumetric bioprinting enables fabrication of cubic centimeter‐sized living materials with micrometer resolution in minutes. Xolography is a light sheet‐based volumetric printing technology that offers unprecedented volumetric generation rates and print resolutions for hard plastics. However, the limited solubility and reactivity of current dual‐color photoinitiators (DCPIs) in aqueous media have hindered their application for high‐resolution bioprinting of living matter. Here, we present a novel three‐component formulation that drastically improves photoreactivity and thereby enables high‐resolution, rapid, and cytocompatible Xolographic biofabrication of intricately architected yet mechanically robust living materials. To achieve this, various relevant additives are systematically explored, which revealed that diphenyliodonium chloride and N‐vinylpyrrolidone strongly enhance D‐mediated photoreactivity, as confirmed by dual‐color photo‐rheology. This enables Xolographic bioprinting of gelatin methacryloyl‐based bioresins, producing >1 cm3 constructs at ≈20 µm positive and 125 µm negative resolution within minutes. Multimaterial printing, molecular patterning, and grayscale‐mediated mechanical patterning are explored to programmably create intricate, biomimetic, and concentration‐controlled architectures. We demonstrate the Bioxolographic printing of various cell types, showing excellent cell viability, compatibility with long‐term culture, and ability for nascent protein deposition. These results position Bioxolography as a transformative platform for rapid, scalable, high‐resolution fabrication of functional living materials with encoded chemical and mechanical properties.
{"title":"Bioxolography Using Diphenyliodonium Chloride and N‐Vinylpyrrolidone Enables Rapid High‐Resolution Volumetric 3D Printing of Spatially Encoded Living Matter","authors":"Alexis Wolfel, Castro Johnbosco, Annalise Anspach, Marieke Meteling, Jos Olijve, Niklas Felix König, Jeroen Leijten","doi":"10.1002/adma.202501052","DOIUrl":"https://doi.org/10.1002/adma.202501052","url":null,"abstract":"Light‐based volumetric bioprinting enables fabrication of cubic centimeter‐sized living materials with micrometer resolution in minutes. Xolography is a light sheet‐based volumetric printing technology that offers unprecedented volumetric generation rates and print resolutions for hard plastics. However, the limited solubility and reactivity of current dual‐color photoinitiators (DCPIs) in aqueous media have hindered their application for high‐resolution bioprinting of living matter. Here, we present a novel three‐component formulation that drastically improves photoreactivity and thereby enables high‐resolution, rapid, and cytocompatible Xolographic biofabrication of intricately architected yet mechanically robust living materials. To achieve this, various relevant additives are systematically explored, which revealed that diphenyliodonium chloride and <jats:italic>N</jats:italic>‐vinylpyrrolidone strongly enhance D‐mediated photoreactivity, as confirmed by dual‐color photo‐rheology. This enables Xolographic bioprinting of gelatin methacryloyl‐based bioresins, producing >1 cm<jats:sup>3</jats:sup> constructs at ≈20 µm positive and 125 µm negative resolution within minutes. Multimaterial printing, molecular patterning, and grayscale‐mediated mechanical patterning are explored to programmably create intricate, biomimetic, and concentration‐controlled architectures. We demonstrate the Bioxolographic printing of various cell types, showing excellent cell viability, compatibility with long‐term culture, and ability for nascent protein deposition. These results position Bioxolography as a transformative platform for rapid, scalable, high‐resolution fabrication of functional living materials with encoded chemical and mechanical properties.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"17 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876113","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}
Supraparticles (SPs) with unique properties are emerging as versatile platforms for applications in catalysis, photonics, and medicine. However, the synthesis of novel SPs with complex internal structures remains a challenge. Self‐Assembled Multilayered Supraparticles (SAMS) presented here are composed of concentric lamellar spherical structures made from metallic nanoparticles, formed from a synergistic three‐way interaction phenomenon between gold nanoparticles, lipidoid, and gelatin, exhibiting interlayer spacing of 3.5 ± 0.2 nm within a self‐limited 156.8 ± 56.6 nm diameter. The formation is critically influenced by both physical (including nanoparticle size, lipidoid chain length) and chemical factors (including elemental composition, nanoparticle cap, and organic material), which collectively modulate the surface chemistry and hydrophobicity, affecting interparticle interactions. SAMS can efficiently deliver labile payloads such as siRNA, achieving dose‐dependent silencing in vivo, while also showing potential for complex payloads such as mRNA. This work not only advances the field of SP design by introducing a new structure and interaction phenomenon but also demonstrates its potential in nanomedicine.
{"title":"Self‐Assembled Multilayered Concentric Supraparticle Architecture","authors":"Agasthya Suresh, Dhananjay Suresh, Zhaohui Li, John Sansalone, Narayana Aluru, Anandhi Upendran, Raghuraman Kannan","doi":"10.1002/adma.202502055","DOIUrl":"https://doi.org/10.1002/adma.202502055","url":null,"abstract":"Supraparticles (SPs) with unique properties are emerging as versatile platforms for applications in catalysis, photonics, and medicine. However, the synthesis of novel SPs with complex internal structures remains a challenge. Self‐Assembled Multilayered Supraparticles (SAMS) presented here are composed of concentric lamellar spherical structures made from metallic nanoparticles, formed from a synergistic three‐way interaction phenomenon between gold nanoparticles, lipidoid, and gelatin, exhibiting interlayer spacing of 3.5 ± 0.2 nm within a self‐limited 156.8 ± 56.6 nm diameter. The formation is critically influenced by both physical (including nanoparticle size, lipidoid chain length) and chemical factors (including elemental composition, nanoparticle cap, and organic material), which collectively modulate the surface chemistry and hydrophobicity, affecting interparticle interactions. SAMS can efficiently deliver labile payloads such as siRNA, achieving dose‐dependent silencing in vivo, while also showing potential for complex payloads such as mRNA. This work not only advances the field of SP design by introducing a new structure and interaction phenomenon but also demonstrates its potential in nanomedicine.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"33 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876118","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}
The thickness and composition of the solid electrolyte interphase (SEI) on lithium (Li) metal are critical factors influencing dendrite growth. This study introduces a novel electrolyte selection strategy based on electrochemical corrosion principles. By employing LiCl and LiNO3 simultaneously, the electrolyte itself has a high donor number, low desolvation energy, high Li⁺ transference number and conductivity, and a moderate electrochemical stability window. In addition, it dynamically reduces the SEI thickness and reactivates dead Li, forming a ≈100 nm SEI enriched with LiF and Li2O on Li metal anode, which ensures the stable cycling of Li symmetric cells for 2000 h at a current density of 5 mA cm⁻2. Consequently, Li metal cells using LiFePO4 (LFP) as the cathode with the LiNO3‐LiCl‐added electrolyte exhibit excellent cycling performance for 1600 cycles at 680 mA g⁻1. Even with a thin Li metal anode, the Li (5 µm)|LFP cell retains 95% capacity after 70 cycles at 170 mA g⁻1. The universality and feasibility of this electrolyte design are also validated in diverse battery chemistries such as anode‐free Cu|LFP, Li|LiNi0.8Mn0.1Co0.1O2 (NMC811), and Li|S cells, as well as in pouch cells with high‐loading LFP and NMC811 cathodes, showcasing the promising electrolyte design strategy for Li metal batteries.
{"title":"Achieving Ultra‐Thin Solid Electrolyte Interphase for High‐Performance Lithium Metal Anodes via Chloride‐Assisted Electrochemical Corrosion","authors":"Xue Wang, Qiao Zhang, Zengwu Wei, Kaiwei Zhou, Xianhui Chen, Zhao Qian, Jun Wang, Xing Xin","doi":"10.1002/smll.202502682","DOIUrl":"https://doi.org/10.1002/smll.202502682","url":null,"abstract":"The thickness and composition of the solid electrolyte interphase (SEI) on lithium (Li) metal are critical factors influencing dendrite growth. This study introduces a novel electrolyte selection strategy based on electrochemical corrosion principles. By employing LiCl and LiNO<jats:sub>3</jats:sub> simultaneously, the electrolyte itself has a high donor number, low desolvation energy, high Li⁺ transference number and conductivity, and a moderate electrochemical stability window. In addition, it dynamically reduces the SEI thickness and reactivates dead Li, forming a ≈100 nm SEI enriched with LiF and Li<jats:sub>2</jats:sub>O on Li metal anode, which ensures the stable cycling of Li symmetric cells for 2000 h at a current density of 5 mA cm⁻<jats:sup>2</jats:sup>. Consequently, Li metal cells using LiFePO<jats:sub>4</jats:sub> (LFP) as the cathode with the LiNO<jats:sub>3</jats:sub>‐LiCl‐added electrolyte exhibit excellent cycling performance for 1600 cycles at 680 mA g⁻<jats:sup>1</jats:sup>. Even with a thin Li metal anode, the Li (5 µm)|LFP cell retains 95% capacity after 70 cycles at 170 mA g⁻<jats:sup>1</jats:sup>. The universality and feasibility of this electrolyte design are also validated in diverse battery chemistries such as anode‐free Cu|LFP, Li|LiNi<jats:sub>0.8</jats:sub>Mn<jats:sub>0.1</jats:sub>Co<jats:sub>0.1</jats:sub>O<jats:sub>2</jats:sub> (NMC811), and Li|S cells, as well as in pouch cells with high‐loading LFP and NMC811 cathodes, showcasing the promising electrolyte design strategy for Li metal batteries.","PeriodicalId":228,"journal":{"name":"Small","volume":"78 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876123","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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