Pub Date : 2025-04-23DOI: 10.1016/j.matt.2025.102129
Michael A. Stolberg, Jeffrey Lopez, Sawyer D. Cawthern, Abraham Herzog-Arbeitman, Ha-Kyung Kwon, Daniel Schweigert, Abraham Anapolosky, Brian D. Storey, Jeremiah A. Johnson, Yang Shao-Horn
Lithium-ion batteries aid decarbonization by enabling electric vehicles and renewable energy generation, but these applications put increasing demands on the energy density, safety, and cost of batteries. Polymer electrolytes could improve battery safety but currently do not have sufficient ionic conductivity for ambient operation. To address this challenge, we developed a high-throughput platform to increase the speed and scale of polymer electrolyte research, enabling the acquisition of data for over 60 samples per researcher hour. We utilized automated formulation and characterization operations, including electrochemical impedance spectroscopy with in situ thickness measurements, to perform a comparison of lithium and sodium salts in poly(ethylene oxide). Our study provides a high-quality, unified reference dataset for the community and greatly expands available data for sodium-based electrolytes. Secondly, our large dataset allows us to find that the local minima in glass transition temperature that corresponds to maximum ionic conductivity is a colligative property independent of either anion or cation chemistry.
{"title":"A data-driven platform for automated characterization of polymer electrolytes","authors":"Michael A. Stolberg, Jeffrey Lopez, Sawyer D. Cawthern, Abraham Herzog-Arbeitman, Ha-Kyung Kwon, Daniel Schweigert, Abraham Anapolosky, Brian D. Storey, Jeremiah A. Johnson, Yang Shao-Horn","doi":"10.1016/j.matt.2025.102129","DOIUrl":"https://doi.org/10.1016/j.matt.2025.102129","url":null,"abstract":"Lithium-ion batteries aid decarbonization by enabling electric vehicles and renewable energy generation, but these applications put increasing demands on the energy density, safety, and cost of batteries. Polymer electrolytes could improve battery safety but currently do not have sufficient ionic conductivity for ambient operation. To address this challenge, we developed a high-throughput platform to increase the speed and scale of polymer electrolyte research, enabling the acquisition of data for over 60 samples per researcher hour. We utilized automated formulation and characterization operations, including electrochemical impedance spectroscopy with <em>in situ</em> thickness measurements, to perform a comparison of lithium and sodium salts in poly(ethylene oxide). Our study provides a high-quality, unified reference dataset for the community and greatly expands available data for sodium-based electrolytes. Secondly, our large dataset allows us to find that the local minima in glass transition temperature that corresponds to maximum ionic conductivity is a colligative property independent of either anion or cation chemistry.","PeriodicalId":388,"journal":{"name":"Matter","volume":"128 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862391","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 : 2025-04-21DOI: 10.1016/j.matt.2025.102108
Yu Chen, Shai Zilberzwige-Tal, Nathan D. Rosenmann, Julia Oktawiec, Ashley K. Nensel, Qing Ma, Sasha Lichtenstein, Ehud Gazit, Nathan C. Gianneschi
Hierarchically porous materials have broad applications in biotechnology and medicine, yet current fabrication methods often lack scalability and biocompatibility. Here, we present a peptide-coordination self-assembly approach to prepare hierarchically porous microspheres composed of naturally occurring carnosine dipeptide and coordinated Zn(II) ions. Metal coordination led to microsphere formation featuring interconnected channels with a hierarchically porous structure. Characterization with scanning electron and transmission electron microscopy, as well as with extended X-ray absorption fine structure, confirmed its nanofibrous architecture and local Zn(II) coordination environment. Liquid cell transmission electron microscopy, in turn, provided real-time insight into the assembly process, revealing a stepwise process from nanoclusters to nanofibers and ultimately to porous microspheres. The carnosine-Zn(II) microspheres exhibit intrinsic blue fluorescence and high porosity, containing both micropores and mesopores, which facilitate efficient mass transport and biomolecule immobilization. We leverage these properties to generate reusable, cell-free synthesis nanoreactors, to enhance DNA transcription and translation and protect against nuclease degradation.
{"title":"Hierarchically porous carnosine-Zn microspheres","authors":"Yu Chen, Shai Zilberzwige-Tal, Nathan D. Rosenmann, Julia Oktawiec, Ashley K. Nensel, Qing Ma, Sasha Lichtenstein, Ehud Gazit, Nathan C. Gianneschi","doi":"10.1016/j.matt.2025.102108","DOIUrl":"https://doi.org/10.1016/j.matt.2025.102108","url":null,"abstract":"Hierarchically porous materials have broad applications in biotechnology and medicine, yet current fabrication methods often lack scalability and biocompatibility. Here, we present a peptide-coordination self-assembly approach to prepare hierarchically porous microspheres composed of naturally occurring carnosine dipeptide and coordinated Zn(II) ions. Metal coordination led to microsphere formation featuring interconnected channels with a hierarchically porous structure. Characterization with scanning electron and transmission electron microscopy, as well as with extended X-ray absorption fine structure, confirmed its nanofibrous architecture and local Zn(II) coordination environment. Liquid cell transmission electron microscopy, in turn, provided real-time insight into the assembly process, revealing a stepwise process from nanoclusters to nanofibers and ultimately to porous microspheres. The carnosine-Zn(II) microspheres exhibit intrinsic blue fluorescence and high porosity, containing both micropores and mesopores, which facilitate efficient mass transport and biomolecule immobilization. We leverage these properties to generate reusable, cell-free synthesis nanoreactors, to enhance DNA transcription and translation and protect against nuclease degradation.","PeriodicalId":388,"journal":{"name":"Matter","volume":"219 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853252","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 : 2025-04-16DOI: 10.1016/j.matt.2025.102107
Yingshan Ma, Ian Kenalty, Niher R. Sarker, Yuhang Huang, Baichuan Kou, Cheng Hao, Ning Yan, Jay Werber, Eugenia Kumacheva
Water scarcity in arid regions is a challenge stimulating the need for the development of sustainable methods to harvest water vapor from the atmosphere. In this work, we developed an aerogel with a structural hierarchy for enhanced water capture and release. The aerogel was derived from nature-sourced biodegradable phytoglycogen nanoparticles (PhG NPs) that exhibit strong hydrogen bonding with water molecules. The crosslinking of acryloyl-modified PhG NPs produced microgel particles that were used as building blocks for a macroscopic hydrogel. The removal of water from this hydrogel yielded an aerogel with three characteristic pore dimensions, that is, several nanometer-, tens of nanometer-, and micrometer-size pores. The aerogel showed enhanced water-harvesting capacity and sorption kinetics. This hierarchically structured aerogel shows promise as an eco-friendly material for atmospheric water harvesting and offers a sustainable alternative to traditional sorbents.
{"title":"Hierarchically structured phytoglycogen aerogels for atmospheric water harvesting","authors":"Yingshan Ma, Ian Kenalty, Niher R. Sarker, Yuhang Huang, Baichuan Kou, Cheng Hao, Ning Yan, Jay Werber, Eugenia Kumacheva","doi":"10.1016/j.matt.2025.102107","DOIUrl":"https://doi.org/10.1016/j.matt.2025.102107","url":null,"abstract":"Water scarcity in arid regions is a challenge stimulating the need for the development of sustainable methods to harvest water vapor from the atmosphere. In this work, we developed an aerogel with a structural hierarchy for enhanced water capture and release. The aerogel was derived from nature-sourced biodegradable phytoglycogen nanoparticles (PhG NPs) that exhibit strong hydrogen bonding with water molecules. The crosslinking of acryloyl-modified PhG NPs produced microgel particles that were used as building blocks for a macroscopic hydrogel. The removal of water from this hydrogel yielded an aerogel with three characteristic pore dimensions, that is, several nanometer-, tens of nanometer-, and micrometer-size pores. The aerogel showed enhanced water-harvesting capacity and sorption kinetics. This hierarchically structured aerogel shows promise as an eco-friendly material for atmospheric water harvesting and offers a sustainable alternative to traditional sorbents.","PeriodicalId":388,"journal":{"name":"Matter","volume":"40 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836897","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 : 2025-04-11DOI: 10.1016/j.matt.2025.102106
Dimitrios Georgiou, Daniel Okegbu, Zeshi Yang, Tao Wang, Michael R. Snowdon, Amar Mohanty, Neil Gershenfeld, Wentao Yan, Christos E. Athanasiou
The housing and climate crises are intertwined: climate change increases housing costs through increased damage and insurance premiums, while resource-intensive construction boosts greenhouse gas emissions. Emerging alternative construction methods aim to reduce the environmental impact but often rely on materials with questionable sustainability benefits. In this study, we build on the concept of digital metamaterials—lightweight, reconfigurable building blocks—by introducing eco-voxels: modular, mass-producible construction units made from an in-house-developed polymer composite of partially sustainably sourced polymer and rCFs. By assessing the structural performance of an eco-voxel wall, we illustrate the suitability of this construction method for residential buildings. In parallel, by comparing the carbon footprint of a 1 m2 eco-voxel wall with traditional concrete, three-dimensional-printed concrete, and CLT, we demonstrate 20%–40% reduced greenhouse gas emissions. Our analysis demonstrates that eco-voxels meet load-bearing requirements and offer a reduced carbon footprint aligned with eco-conscious construction demands.
{"title":"Eco-voxels: Building blocks for sustainable, load-bearing structures","authors":"Dimitrios Georgiou, Daniel Okegbu, Zeshi Yang, Tao Wang, Michael R. Snowdon, Amar Mohanty, Neil Gershenfeld, Wentao Yan, Christos E. Athanasiou","doi":"10.1016/j.matt.2025.102106","DOIUrl":"https://doi.org/10.1016/j.matt.2025.102106","url":null,"abstract":"The housing and climate crises are intertwined: climate change increases housing costs through increased damage and insurance premiums, while resource-intensive construction boosts greenhouse gas emissions. Emerging alternative construction methods aim to reduce the environmental impact but often rely on materials with questionable sustainability benefits. In this study, we build on the concept of digital metamaterials—lightweight, reconfigurable building blocks—by introducing eco-voxels: modular, mass-producible construction units made from an in-house-developed polymer composite of partially sustainably sourced polymer and rCFs. By assessing the structural performance of an eco-voxel wall, we illustrate the suitability of this construction method for residential buildings. In parallel, by comparing the carbon footprint of a 1 m<sup>2</sup> eco-voxel wall with traditional concrete, three-dimensional-printed concrete, and CLT, we demonstrate 20%–40% reduced greenhouse gas emissions. Our analysis demonstrates that eco-voxels meet load-bearing requirements and offer a reduced carbon footprint aligned with eco-conscious construction demands.","PeriodicalId":388,"journal":{"name":"Matter","volume":"108 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143820058","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 : 2025-04-11DOI: 10.1016/j.matt.2025.102100
Danielle N. Beatty, Wil V. Srubar
This work explores the use of photosynthesized coccoliths (intricate CaCO3 particles) as a nucleation agent or cement replacement in portland cement paste. First, coccoliths were produced and harvested from the marine microalgae Emiliania huxleyi and the particle size, morphology, and mineralogy were characterized. Then, the nucleation effects of E. huxleyi coccoliths as seeding agent (0.5, 1, 3, or 5 wt % additions) and limestone filler (5 and 15 wt % cement replacements) were studied using isothermal conduction calorimetry and compressive strength testing. The results were compared with five commercially available CaCO3 sources used as nucleation agents and fillers. While the high surface area of coccoliths (12.22 m2/g) enhanced water demand, it also enhanced nucleation during cement hydration without accelerating hydration, leading to enhanced early-age strength without detriments to 28-day strength. Results highlight a potential carbon reduction strategy, namely employing photosynthesis as a method of mineral admixture production, for the cement and concrete industry.
{"title":"Nucleation effects of coccoliths in portland cement","authors":"Danielle N. Beatty, Wil V. Srubar","doi":"10.1016/j.matt.2025.102100","DOIUrl":"https://doi.org/10.1016/j.matt.2025.102100","url":null,"abstract":"This work explores the use of photosynthesized coccoliths (intricate CaCO<sub>3</sub> particles) as a nucleation agent or cement replacement in portland cement paste. First, coccoliths were produced and harvested from the marine microalgae <em>Emiliania huxleyi</em> and the particle size, morphology, and mineralogy were characterized. Then, the nucleation effects of <em>E. huxleyi</em> coccoliths as seeding agent (0.5, 1, 3, or 5 wt % additions) and limestone filler (5 and 15 wt % cement replacements) were studied using isothermal conduction calorimetry and compressive strength testing. The results were compared with five commercially available CaCO<sub>3</sub> sources used as nucleation agents and fillers. While the high surface area of coccoliths (12.22 m<sup>2</sup>/g) enhanced water demand, it also enhanced nucleation during cement hydration without accelerating hydration, leading to enhanced early-age strength without detriments to 28-day strength. Results highlight a potential carbon reduction strategy, namely employing photosynthesis as a method of mineral admixture production, for the cement and concrete industry.","PeriodicalId":388,"journal":{"name":"Matter","volume":"6 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143820015","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 : 2025-04-09DOI: 10.1016/j.matt.2025.102104
Junbing Zhu, Shuhao Zhang, Jiangfeng Ni, Liang Li
Aqueous zinc microbatteries, despite advantages like simpler assembly and lower cost, face challenges of limited areal capacity and energy, affecting long-term operation of microelectronics. In this work, we design quasi-solid-state four-electron Zn//I2 microbatteries by introducing Br− species into an imidazolium gel electrolyte with a high SO42− concentration. Incorporating Br− facilitates I2-to-I+ conversion to form interhalogen anions, which can be captured and stabilized by the imidazolium species. Meanwhile, the salting-out effect endowed by the high-concentration SO42− helps develop a dense hydration layer that reduces the interaction between the I2-based cathode and water, drastically suppressing the dissolution of the active material. This combined strategy of interhalogen and salting out enables an unprecedented areal capacity of 15.0 mAh cm−2 and energy density of 20.1 mWh cm−2 for Zn//I2 aqueous microbatteries. Moreover, Zn//I2 aqueous microbatteries have been integrated into on-ship sensor components, thus demonstrating prodigious potential for powering autonomous microelectronics.
{"title":"Interhalogen and the salting-out effect enable high-capacity and long-cycle Zn//I2 aqueous microbatteries","authors":"Junbing Zhu, Shuhao Zhang, Jiangfeng Ni, Liang Li","doi":"10.1016/j.matt.2025.102104","DOIUrl":"https://doi.org/10.1016/j.matt.2025.102104","url":null,"abstract":"Aqueous zinc microbatteries, despite advantages like simpler assembly and lower cost, face challenges of limited areal capacity and energy, affecting long-term operation of microelectronics. In this work, we design quasi-solid-state four-electron Zn//I<sub>2</sub> microbatteries by introducing Br<sup>−</sup> species into an imidazolium gel electrolyte with a high SO<sub>4</sub><sup>2−</sup> concentration. Incorporating Br<sup>−</sup> facilitates I<sub>2</sub>-to-I<sup>+</sup> conversion to form interhalogen anions, which can be captured and stabilized by the imidazolium species. Meanwhile, the salting-out effect endowed by the high-concentration SO<sub>4</sub><sup>2−</sup> helps develop a dense hydration layer that reduces the interaction between the I<sub>2</sub>-based cathode and water, drastically suppressing the dissolution of the active material. This combined strategy of interhalogen and salting out enables an unprecedented areal capacity of 15.0 mAh cm<sup>−2</sup> and energy density of 20.1 mWh cm<sup>−2</sup> for Zn//I<sub>2</sub> aqueous microbatteries. Moreover, Zn//I<sub>2</sub> aqueous microbatteries have been integrated into on-ship sensor components, thus demonstrating prodigious potential for powering autonomous microelectronics.","PeriodicalId":388,"journal":{"name":"Matter","volume":"108 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806421","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 : 2025-04-09DOI: 10.1016/j.matt.2025.102105
Yejun Feng, Yishu Wang, Thomas F. Rosenbaum, Peter B. Littlewood, Hua Chen
Magnetoresistance (MR) at a fixed field can demonstrate a non-monotonic temperature dependence—an anomaly—in many systems, including low-dimensional chalcogenides, spin- and charge-density-wave metals, and topological semimetals. These systems are often low-carrier-density compensated metals, and the physics are expected to be quasi-classical. Nevertheless, the MR anomaly also exists in the highly conductive metals Cr, Mo, and W for both linear and quadratic field dependence, with their non-saturation attributed to either open orbit or electron-hole compensation. We argue that quantum transport across sharp Fermi surface arcs, but not necessarily the full cyclotron orbit, governs this MR anomaly, thereby accounting for the profound effects of disorder. In Cr, an overlay exists between three temperature dependences: MR at a constant high field, linear MR at a low field, and Shubnikov-de Haas (SdH) oscillations of the smallest orbit. In Mo, the MR anomaly extends beyond the temperature of its SdH oscillations but disappears before Kohler’s scaling reemerges.
{"title":"Fermi surface origin of the low-temperature magnetoresistance anomaly","authors":"Yejun Feng, Yishu Wang, Thomas F. Rosenbaum, Peter B. Littlewood, Hua Chen","doi":"10.1016/j.matt.2025.102105","DOIUrl":"https://doi.org/10.1016/j.matt.2025.102105","url":null,"abstract":"Magnetoresistance (MR) at a fixed field can demonstrate a non-monotonic temperature dependence—an anomaly—in many systems, including low-dimensional chalcogenides, spin- and charge-density-wave metals, and topological semimetals. These systems are often low-carrier-density compensated metals, and the physics are expected to be quasi-classical. Nevertheless, the MR anomaly also exists in the highly conductive metals Cr, Mo, and W for both linear and quadratic field dependence, with their non-saturation attributed to either open orbit or electron-hole compensation. We argue that quantum transport across sharp Fermi surface arcs, but not necessarily the full cyclotron orbit, governs this MR anomaly, thereby accounting for the profound effects of disorder. In Cr, an overlay exists between three temperature dependences: MR at a constant high field, linear MR at a low field, and Shubnikov-de Haas (SdH) oscillations of the smallest orbit. In Mo, the MR anomaly extends beyond the temperature of its SdH oscillations but disappears before Kohler’s scaling reemerges.","PeriodicalId":388,"journal":{"name":"Matter","volume":"39 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806424","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}
MXenes are the fastest growing family of two-dimensional (2D) materials with potential for applications from energy storage to biomedicine, sensing, and electromagnetic shielding. Despite significant progress in MXene synthesis through selective etching of layered MAX phase precursors, limited understanding of the fundamental etching mechanism and kinetics hinders rational optimization of the process. Here, we monitored the etching process using in situ and ex situ techniques at the single-particle and ensemble levels. Our work shows that etching nucleation is instantaneous and etching occurs layer by layer. Through analytical modeling, we found that etching of V2AlC is diffusion-limited. In contrast, etching of Ti2AlC and Ti3AlC2 is reaction-interface-limited, with an additional surface reaction limitation for Ti3AlC2 accounting for more than one-quarter of the total etching time. Overall, our work provides significant insights into the MAX phase etching mechanism and kinetics and an overview of the tools and techniques available to investigate etchable layered materials.
{"title":"Layer-by-layer mechanism of the MAX phase to MXene transformation","authors":"Mark Anayee, Ruocun (John) Wang, Marley Downes, Stefano Ippolito, Yury Gogotsi","doi":"10.1016/j.matt.2025.102092","DOIUrl":"https://doi.org/10.1016/j.matt.2025.102092","url":null,"abstract":"MXenes are the fastest growing family of two-dimensional (2D) materials with potential for applications from energy storage to biomedicine, sensing, and electromagnetic shielding. Despite significant progress in MXene synthesis through selective etching of layered MAX phase precursors, limited understanding of the fundamental etching mechanism and kinetics hinders rational optimization of the process. Here, we monitored the etching process using <em>in situ</em> and <em>ex situ</em> techniques at the single-particle and ensemble levels. Our work shows that etching nucleation is instantaneous and etching occurs layer by layer. Through analytical modeling, we found that etching of V<sub>2</sub>AlC is diffusion-limited. In contrast, etching of Ti<sub>2</sub>AlC and Ti<sub>3</sub>AlC<sub>2</sub> is reaction-interface-limited, with an additional surface reaction limitation for Ti<sub>3</sub>AlC<sub>2</sub> accounting for more than one-quarter of the total etching time. Overall, our work provides significant insights into the MAX phase etching mechanism and kinetics and an overview of the tools and techniques available to investigate etchable layered materials.","PeriodicalId":388,"journal":{"name":"Matter","volume":"41 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806423","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 : 2025-04-09DOI: 10.1016/j.matt.2025.102103
Pingan Zhu, Liqiu Wang
Nanoemulsions are prevalent in diverse fields, such as cosmetics, food, pharmaceuticals, oil recovery, drug delivery, and templated materials synthesis, due to their high kinetic stability and versatility in structures and compositions. However, nanoemulsions remain thermodynamically unstable and gradually undergo irreversible breakdown, posing significant constraints on their applicability. Inspired by the dynamic equilibrium of atmospheric clouds, we present thermo-induced reversible nanoemulsification of biphasic liquid systems through cyclic heating and cooling processes. With our strategy, nanodroplets dissipate through dissolution upon heating and re-emerge through nucleation upon cooling, driven by temperature-dependent solubility. Combining experimental, numerical, and theoretical studies, we identify the critical conditions for nanoemulsification, elucidate the physicochemical mechanism of nucleation, and predict the size of nanodroplets. Thermo-induced nanoemulsification (TINE) offers a reversible, facile, and scalable method for energy-efficient, surfactant-free production of nanoemulsions, characterized by good emulsion stability, diverse emulsion types, and precise control over droplet size.
{"title":"Thermo-induced reversible nanoemulsification","authors":"Pingan Zhu, Liqiu Wang","doi":"10.1016/j.matt.2025.102103","DOIUrl":"https://doi.org/10.1016/j.matt.2025.102103","url":null,"abstract":"Nanoemulsions are prevalent in diverse fields, such as cosmetics, food, pharmaceuticals, oil recovery, drug delivery, and templated materials synthesis, due to their high kinetic stability and versatility in structures and compositions. However, nanoemulsions remain thermodynamically unstable and gradually undergo irreversible breakdown, posing significant constraints on their applicability. Inspired by the dynamic equilibrium of atmospheric clouds, we present thermo-induced reversible nanoemulsification of biphasic liquid systems through cyclic heating and cooling processes. With our strategy, nanodroplets dissipate through dissolution upon heating and re-emerge through nucleation upon cooling, driven by temperature-dependent solubility. Combining experimental, numerical, and theoretical studies, we identify the critical conditions for nanoemulsification, elucidate the physicochemical mechanism of nucleation, and predict the size of nanodroplets. Thermo-induced nanoemulsification (TINE) offers a reversible, facile, and scalable method for energy-efficient, surfactant-free production of nanoemulsions, characterized by good emulsion stability, diverse emulsion types, and precise control over droplet size.","PeriodicalId":388,"journal":{"name":"Matter","volume":"82 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806422","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 : 2025-04-08DOI: 10.1016/j.matt.2025.102098
Geetu Kumari, Charlie O’Mahony, Ragima V.P. Veluthaparambath, Suman Bhattacharya, Binoy K. Saha, Sarah Guerin
The confluence of crystal engineering with piezoelectric material discovery is allowing researchers to design sustainable molecular piezoelectrics at the nanoscale. Here, we use this bottom-up design approach to crystallize a series of analogous organic molecules, 2-X-pyridin-3-ol (1X; X = Cl, Br, I), with structures sustained by both halogen bonds and hydrogen bonds. Density functional theory calculations predict, quantify, and rationalize the piezoelectric response of the analogous series 1X. Our calculations reveal high shear piezoelectricity in all three crystals, with the highest predicted response of d15 = 99.19 pC/N for 1Cl. Piezoresponse force microscopy experiments confirm effective shear piezoelectric constants of 54–74 pC/N. The space groups allow for unpoled longitudinal piezoelectric responses, with experimental d33 values of 5–10 pC/N. This highlights the ability of halogen substitution to induce and modulate piezoelectricity and adds to the growing number of molecular crystals approaching triple-digit piezoelectric responses to rival conventional perovskite ceramics.
{"title":"Halogen and hydrogen bonded 2-X-pyridin-3-ol (X = Cl, Br, I) organic crystals with large shear piezoelectricity","authors":"Geetu Kumari, Charlie O’Mahony, Ragima V.P. Veluthaparambath, Suman Bhattacharya, Binoy K. Saha, Sarah Guerin","doi":"10.1016/j.matt.2025.102098","DOIUrl":"https://doi.org/10.1016/j.matt.2025.102098","url":null,"abstract":"The confluence of crystal engineering with piezoelectric material discovery is allowing researchers to design sustainable molecular piezoelectrics at the nanoscale. Here, we use this bottom-up design approach to crystallize a series of analogous organic molecules, 2-<strong>X</strong>-pyridin-3-ol (<strong>1X</strong>; <strong>X</strong> = Cl, Br, I), with structures sustained by both halogen bonds and hydrogen bonds. Density functional theory calculations predict, quantify, and rationalize the piezoelectric response of the analogous series <strong>1X</strong>. Our calculations reveal high shear piezoelectricity in all three crystals, with the highest predicted response of <em>d</em><sub><em>15</em></sub> = 99.19 pC/N for <strong>1Cl</strong>. Piezoresponse force microscopy experiments confirm effective shear piezoelectric constants of 54–74 pC/N. The space groups allow for unpoled longitudinal piezoelectric responses, with experimental <em>d</em><sub><em>33</em></sub> values of 5–10 pC/N. This highlights the ability of halogen substitution to induce and modulate piezoelectricity and adds to the growing number of molecular crystals approaching triple-digit piezoelectric responses to rival conventional perovskite ceramics.","PeriodicalId":388,"journal":{"name":"Matter","volume":"217 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798551","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}
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