The crystallization of ionic crystals has traditionally been explained by Gibbs's classical nucleation theory.However,recent observations of intermediate phases during nucleation suggest that the process may be mo...The crystallization of ionic crystals has traditionally been explained by Gibbs's classical nucleation theory.However,recent observations of intermediate phases during nucleation suggest that the process may be more complex,necessitating new theoretical frameworks,though key empirical evidence remains elusive.In this study,we used microdroplets to investigate the crystallization of sodium halides(NaCl,NaBr,and NaI)under homogeneous nucleation conditions across a wide range of supersaturations.In the evaporating droplet,NaCl follows the classical nucleation pathway,whereas NaBr and NaI exhibit the formation of an intermediate phase prior to the nucleation of anhydrous and hydrous single crystals,respectively.Optical and computational analyses indicate that these intermediate phases are liquid crystal phases composed of contact ion pairs.These findings establish a new theoretical framework for crystal nucleation and growth and offer methods to control nucleation pathways,enabling us to achieve desired crystals regardless of specific conditions.展开更多
Sustainable transformation and efficient utilization of biomasses and their derived materials are environ-mentally as well as economically compliant strategies.Biomass seaweed-derived nitrogen self-doped porous carbon...Sustainable transformation and efficient utilization of biomasses and their derived materials are environ-mentally as well as economically compliant strategies.Biomass seaweed-derived nitrogen self-doped porous carbon with tailored surface area and pore structures are prepared through carb on izatio n and activation.The in fluence of carb on ization temperature on morphology,surface area,and heteroatom dopants are investigated to optimize sodium-ion storage capability.Seaweed-derived nitrogen selfdoped activated carbon(SAC)as anode materials for sodium-ion batteries exhibits remarkable reversible capacity of 303/192 mAh g^(-1) after 100/500 cycles at current densities of 100/200 mA g^(-1) respectively,and a good rate capability.The interconnected and porous conducting nature along with the heteroatom dopant role in creating defective sites and charge stabilization are favorable for ion storage and diffusion and electron transport,indicating the electrodes can offer improved electrochemical performances.In addition,post-mortem analysis of the cycled carbon electrodes through ex-situ tools demonstrates the sodium-ion storage mechanism.展开更多
Conversion-reaction induced charge storage mechanisms of transition metal sulphides have received considerable interest in designing high-capacity electrodes for electrochemical energy storage devices.However,their lo...Conversion-reaction induced charge storage mechanisms of transition metal sulphides have received considerable interest in designing high-capacity electrodes for electrochemical energy storage devices.However,their low conductivity and structural degradation during cycling limit their applications as energy storage devices.A combination of different nickel sulphide phases tailored with carbon nanostructures is suggested to address these limitations.Herein,a facile,two-step approach is demonstrated for fabricating a hybrid electrode,consisting of trinickel disulphide(Ni_(3)S_(2))formed on a metallic Ni nanoparticle supported by vertical carbon nanotubes(VCN)backbone in the form Ni_(3)S_(2)/Ni@VCN.Ni_(3)S_(2)/Ni@VCN electrodes were tested as anode for lithium-ion batteries,and the electrode featured outstanding lithiumstorage capabilities with a high reversible capacity(1113 m Ah g^(-1) after 100 cycles at 100 m A g^(-1)),excellent long-term cycling stability(770 m Ah g^(-1) after 500 cycles at 200 m A g^(-1)),and good rate capability.The resulting electrode performance is one of the best Li-ion storage capabilities in the Ni_(3)S_(2)-type anode materials described.A unique “broccoli-like”structure of polycrystalline Ni_(3)S_(2)capped on conductive VCN backbone helps the interface storage process and boosts lithium storage performance.展开更多
Autonomously self-healing, reversible, and soft adhesive microarchitecturesand structured electric elements could be important features in stable and versatilebioelectronic devices adhere to complex surfaces of the hu...Autonomously self-healing, reversible, and soft adhesive microarchitecturesand structured electric elements could be important features in stable and versatilebioelectronic devices adhere to complex surfaces of the human body(rough, dry, wet, and vulnerable). In this study, we propose an autonomousself-healing multi-layered adhesive patch inspired by the octopus, which possessself-healing and robust adhesion properties in dry/underwater conditions.To implement autonomously self-healing octopus-inspired architectures, adynamic polymer reflow model based on structural and material design suggestscriteria for three-dimensional patterning self-healing elastomers. In addition,self-healing multi-layered microstructures with different moduli endowsefficient self-healing ability, human-friendly reversible bio-adhesion, and stablemechanical deformability. Through programmed molecular behavior ofmicrolevel hybrid multiscale architectures, the bioinspired adhesive patchexhibited robust adhesion against rough skin surface under both dry andunderwater conditions while enabling autonomous adhesion restoring performanceafter damaged (over 95% healing efficiency under both conditions for24 h at 30℃). Finally, we developed a self-healing skin-mountable adhesiveelectronics with repeated attachment and minimal skin irritation by laminatingthin gold electrodes on octopus-like structures. Based on the robust adhesionand intimate contact with skin, we successfully obtained reliable measurements during dynamic motion under dry, wet, and damagedconditions.展开更多
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.2021R1C1C2006535)supported by the Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Korea government(MSIT)(No.RS-2024-00403164)supported by the National Research Foundation of Korea grant funded by the Korea government,Ministry of Science and ICT(Development of Nanofiber Yarn Based Compound Sensor as a Comprehensive Wearable Healthcare Solution)(Grant No.RS-2024-00357296).
文摘The crystallization of ionic crystals has traditionally been explained by Gibbs's classical nucleation theory.However,recent observations of intermediate phases during nucleation suggest that the process may be more complex,necessitating new theoretical frameworks,though key empirical evidence remains elusive.In this study,we used microdroplets to investigate the crystallization of sodium halides(NaCl,NaBr,and NaI)under homogeneous nucleation conditions across a wide range of supersaturations.In the evaporating droplet,NaCl follows the classical nucleation pathway,whereas NaBr and NaI exhibit the formation of an intermediate phase prior to the nucleation of anhydrous and hydrous single crystals,respectively.Optical and computational analyses indicate that these intermediate phases are liquid crystal phases composed of contact ion pairs.These findings establish a new theoretical framework for crystal nucleation and growth and offer methods to control nucleation pathways,enabling us to achieve desired crystals regardless of specific conditions.
基金supported by the Next Generation Engineering Researcher Program of National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(2017H1D8A2031138).
文摘Sustainable transformation and efficient utilization of biomasses and their derived materials are environ-mentally as well as economically compliant strategies.Biomass seaweed-derived nitrogen self-doped porous carbon with tailored surface area and pore structures are prepared through carb on izatio n and activation.The in fluence of carb on ization temperature on morphology,surface area,and heteroatom dopants are investigated to optimize sodium-ion storage capability.Seaweed-derived nitrogen selfdoped activated carbon(SAC)as anode materials for sodium-ion batteries exhibits remarkable reversible capacity of 303/192 mAh g^(-1) after 100/500 cycles at current densities of 100/200 mA g^(-1) respectively,and a good rate capability.The interconnected and porous conducting nature along with the heteroatom dopant role in creating defective sites and charge stabilization are favorable for ion storage and diffusion and electron transport,indicating the electrodes can offer improved electrochemical performances.In addition,post-mortem analysis of the cycled carbon electrodes through ex-situ tools demonstrates the sodium-ion storage mechanism.
基金funded by the PEGASUS(Plasma Enabled and Graphene Allowed Synthesis of Unique Nano-structures)projectfunded by the European Union’s Horizon-Future and Emerging Technologies(FET)research and innovation program under grant agreement No.766894+2 种基金the funding from the Slovenian Research Agency(ARRS)on project N2-0091the support of AD FUTURA,Public Scholarship,Development,Disability,and Maintenance Fund of the Republic of SloveniaNational Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.2017H1D8A2031138)。
文摘Conversion-reaction induced charge storage mechanisms of transition metal sulphides have received considerable interest in designing high-capacity electrodes for electrochemical energy storage devices.However,their low conductivity and structural degradation during cycling limit their applications as energy storage devices.A combination of different nickel sulphide phases tailored with carbon nanostructures is suggested to address these limitations.Herein,a facile,two-step approach is demonstrated for fabricating a hybrid electrode,consisting of trinickel disulphide(Ni_(3)S_(2))formed on a metallic Ni nanoparticle supported by vertical carbon nanotubes(VCN)backbone in the form Ni_(3)S_(2)/Ni@VCN.Ni_(3)S_(2)/Ni@VCN electrodes were tested as anode for lithium-ion batteries,and the electrode featured outstanding lithiumstorage capabilities with a high reversible capacity(1113 m Ah g^(-1) after 100 cycles at 100 m A g^(-1)),excellent long-term cycling stability(770 m Ah g^(-1) after 500 cycles at 200 m A g^(-1)),and good rate capability.The resulting electrode performance is one of the best Li-ion storage capabilities in the Ni_(3)S_(2)-type anode materials described.A unique “broccoli-like”structure of polycrystalline Ni_(3)S_(2)capped on conductive VCN backbone helps the interface storage process and boosts lithium storage performance.
基金National Research Foundation of Korea,Grant/Award Numbers: NRF-2021R1C1C1009925,2020R1A6A1A03048004, RS-2023-00214236Ministry of Trade,Industry & Energy (MOTIE, Korea),Grant/Award Number: RS-2022-00154781National Research Council of Science &Technology, Grant/Award Number:CRC230231-000。
文摘Autonomously self-healing, reversible, and soft adhesive microarchitecturesand structured electric elements could be important features in stable and versatilebioelectronic devices adhere to complex surfaces of the human body(rough, dry, wet, and vulnerable). In this study, we propose an autonomousself-healing multi-layered adhesive patch inspired by the octopus, which possessself-healing and robust adhesion properties in dry/underwater conditions.To implement autonomously self-healing octopus-inspired architectures, adynamic polymer reflow model based on structural and material design suggestscriteria for three-dimensional patterning self-healing elastomers. In addition,self-healing multi-layered microstructures with different moduli endowsefficient self-healing ability, human-friendly reversible bio-adhesion, and stablemechanical deformability. Through programmed molecular behavior ofmicrolevel hybrid multiscale architectures, the bioinspired adhesive patchexhibited robust adhesion against rough skin surface under both dry andunderwater conditions while enabling autonomous adhesion restoring performanceafter damaged (over 95% healing efficiency under both conditions for24 h at 30℃). Finally, we developed a self-healing skin-mountable adhesiveelectronics with repeated attachment and minimal skin irritation by laminatingthin gold electrodes on octopus-like structures. Based on the robust adhesionand intimate contact with skin, we successfully obtained reliable measurements during dynamic motion under dry, wet, and damagedconditions.
