Pub Date : 2025-01-17DOI: 10.1021/acs.nanolett.4c05644
Xinrui Zhao, Zhe Wang, Xia Deng, Hongli Li, Nan Wang, Xue Zeng, Peng Zhang, Yang Yao, Rong Peng, Shuo Jiang, Shibiao Xie, Mingsu Si, Junwei Zhang, Yong Peng
The electric dipole in materials is closely associated with their electronic transport, optical properties, and mechanical behavior. Here, we have employed the differential phase contrast (DPC) technique of the scanning transmission electron microscopy technique (STEM) to directly analyze the local electric dipole at the sub-Angstrom scale. By utilizing DPC-STEM technology, we successfully visualized the ferroelectric polarization of van der Waals material 3R α-In2Se3 and directly confirmed the dipole interlocking effect (DIE) between in-plane (IP) and out-of-plane (OOP) polarizations. Through density functional theory (DFT) calculations and structural analysis, we discovered that this DIE is caused by the central asymmetry of the middle Se atoms of each monolayer and that the reversal of polarization is accompanied by the emergence of an intermediate phase, β-In2Se3. Leveraging the DIE, we developed a multidirectional ferroelectric memristor that can effectively modulate the IP polarization by applying an OOP pulse voltage.
{"title":"Direct Observation of Dipole Interlocking Effect Occurrence in Two-Dimensional Ferroelectricity","authors":"Xinrui Zhao, Zhe Wang, Xia Deng, Hongli Li, Nan Wang, Xue Zeng, Peng Zhang, Yang Yao, Rong Peng, Shuo Jiang, Shibiao Xie, Mingsu Si, Junwei Zhang, Yong Peng","doi":"10.1021/acs.nanolett.4c05644","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c05644","url":null,"abstract":"The electric dipole in materials is closely associated with their electronic transport, optical properties, and mechanical behavior. Here, we have employed the differential phase contrast (DPC) technique of the scanning transmission electron microscopy technique (STEM) to directly analyze the local electric dipole at the sub-Angstrom scale. By utilizing DPC-STEM technology, we successfully visualized the ferroelectric polarization of van der Waals material 3R α-In<sub>2</sub>Se<sub>3</sub> and directly confirmed the dipole interlocking effect (DIE) between in-plane (IP) and out-of-plane (OOP) polarizations. Through density functional theory (DFT) calculations and structural analysis, we discovered that this DIE is caused by the central asymmetry of the middle Se atoms of each monolayer and that the reversal of polarization is accompanied by the emergence of an intermediate phase, β-In<sub>2</sub>Se<sub>3</sub>. Leveraging the DIE, we developed a multidirectional ferroelectric memristor that can effectively modulate the IP polarization by applying an OOP pulse voltage.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"45 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987572","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}
Björn Greijer, Alexandra Nefedova, Tatiana Agback, Peter Agback, Vambola Kisand, Kai Rausalu, Alexander Vanetsev, Gulaim A. Seisenbaeva, Angela Ivask, Vadim G Kessler
Recent COVID-19 pandemic has set strong quest for advanced understanding of possible tracks in abating and eliminating viral infections. In the view that several families of “pristine” small oxide nanoparticles (NPs) have demonstrated virucidal activity against SARS-CoV-2, we studied the effect of two NPs with presumably different reactivity, on two viruses aiming to evaluate two “primary suspect” routes of their antiviral activity, either specific blocking of surface proteins or causing membrane disruption. The chosen NPs were non-photoactive 3.5 nm triethanolamine terminated (surface capped) titania TiO2 NPs (TATT) and ultrasmall (1.1 nm) silicotungstate polyoxometalate (POM) NPs. The former were expected to both, interact with viral surface proteins as well as strongly complex with phosphate groups whereas the latter was not expected to form surface complexes. We demonstrated that expectedly, POM NPs up to 1.25 mM (4.5 mg/l) had no significant antiviral activity towards neither of the used viruses, an enveloped transmissible gastroenteritis virus (TGEV) belonging to coronaviruses and non-enveloped encelomyocarditis virus (EMCV). At the same time, TATT NPs exhibited statistically significant (p<0.05) antiviral activity against TGEV starting from 0.125 mM (12 µg/ml). However, no antiviral activity of TATT against non-enveloped EMCV was detected. The observation that TATT NPs showed activity only against enveloped viruses and at relatively high concentrations suggests that the effect could be related with complexation with phospholipids. Possible chemical mechanism of viral membrane disruption was investigated by a variable temperature NMR study of NP complexation with model organic phosphate molecules, proving TATT to strongly interact with them and POM remain unreacted. Viral membrane disruption by TATT NPs was additionally confirmed by demonstraing RNA leackage from TGEV upon contact with those NPs. Therefore, our study proved a new mechanism of antiviral action of titania NPs in the dark which involved membrane disruption proceeding via direct surface complexation.
{"title":"Molecular Mechanisms behind the Anti Corona Virus Activity of Small Metal Oxide Nanoparticles","authors":"Björn Greijer, Alexandra Nefedova, Tatiana Agback, Peter Agback, Vambola Kisand, Kai Rausalu, Alexander Vanetsev, Gulaim A. Seisenbaeva, Angela Ivask, Vadim G Kessler","doi":"10.1039/d4nr03730h","DOIUrl":"https://doi.org/10.1039/d4nr03730h","url":null,"abstract":"Recent COVID-19 pandemic has set strong quest for advanced understanding of possible tracks in abating and eliminating viral infections. In the view that several families of “pristine” small oxide nanoparticles (NPs) have demonstrated virucidal activity against SARS-CoV-2, we studied the effect of two NPs with presumably different reactivity, on two viruses aiming to evaluate two “primary suspect” routes of their antiviral activity, either specific blocking of surface proteins or causing membrane disruption. The chosen NPs were non-photoactive 3.5 nm triethanolamine terminated (surface capped) titania TiO2 NPs (TATT) and ultrasmall (1.1 nm) silicotungstate polyoxometalate (POM) NPs. The former were expected to both, interact with viral surface proteins as well as strongly complex with phosphate groups whereas the latter was not expected to form surface complexes. We demonstrated that expectedly, POM NPs up to 1.25 mM (4.5 mg/l) had no significant antiviral activity towards neither of the used viruses, an enveloped transmissible gastroenteritis virus (TGEV) belonging to coronaviruses and non-enveloped encelomyocarditis virus (EMCV). At the same time, TATT NPs exhibited statistically significant (p<0.05) antiviral activity against TGEV starting from 0.125 mM (12 µg/ml). However, no antiviral activity of TATT against non-enveloped EMCV was detected. The observation that TATT NPs showed activity only against enveloped viruses and at relatively high concentrations suggests that the effect could be related with complexation with phospholipids. Possible chemical mechanism of viral membrane disruption was investigated by a variable temperature NMR study of NP complexation with model organic phosphate molecules, proving TATT to strongly interact with them and POM remain unreacted. Viral membrane disruption by TATT NPs was additionally confirmed by demonstraing RNA leackage from TGEV upon contact with those NPs. Therefore, our study proved a new mechanism of antiviral action of titania NPs in the dark which involved membrane disruption proceeding via direct surface complexation.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"20 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987646","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Doaa Aasef Ahmed, Mustafa Çelik, Wernfried Mayr-Schmölzer, Abdulkadir Kızılaslan, Gregor B. Vonbun-Feldbauer
Li–O2 batteries (LOBs) are next-generation energy storage systems. However, their main challenges are the sluggish kinetics of oxygen reduction and evolution reactions (ORR/OER) and high charge overpotentials due to the formation of discharge product (Li2O2). To address this challenge, developing a catalyst with a unique structure and exceptional catalytic properties is crucial to enhancing the reversible cycling performance of LOBs, particularly under high current density conditions. Herein, the transition metal-based perovskite MnTiO3 was examined as a carbon-free cathode catalyst using density functional theory (DFT) calculations and experimental techniques. The intrinsic advantages of MnTiO3 stem from the coexistence of Mn and Ti energy levels near the Fermi level, as revealed by our density of states (DOS) analysis. This electronic structure facilitates ORR/OER, thus endowing MnTiO3 with a bifunctional role in promoting battery performance. Our DFT-based investigation elucidates the surface stability and catalytic properties of MnTiO3. Furthermore, Energy Dispersive Spectroscopy (EDS) and X-ray diffraction (XRD) confirm that the electrochemical reaction on MnTiO3 follows a two-electron pathway. Our findings reveal that a LOB with MnTiO3 exhibits a total overpotential of 1.18 V and 1.55 V using DFT and electrochemical measurements, respectively. High current densities up to 1 A g−1 also highlight its potential as a cathode catalyst for LOBs.
{"title":"MnTiO3 as a carbon-free cathode for rechargeable Li–O2 batteries","authors":"Doaa Aasef Ahmed, Mustafa Çelik, Wernfried Mayr-Schmölzer, Abdulkadir Kızılaslan, Gregor B. Vonbun-Feldbauer","doi":"10.1039/d4ta05571c","DOIUrl":"https://doi.org/10.1039/d4ta05571c","url":null,"abstract":"Li–O<small><sub>2</sub></small> batteries (LOBs) are next-generation energy storage systems. However, their main challenges are the sluggish kinetics of oxygen reduction and evolution reactions (ORR/OER) and high charge overpotentials due to the formation of discharge product (Li<small><sub>2</sub></small>O<small><sub>2</sub></small>). To address this challenge, developing a catalyst with a unique structure and exceptional catalytic properties is crucial to enhancing the reversible cycling performance of LOBs, particularly under high current density conditions. Herein, the transition metal-based perovskite MnTiO<small><sub>3</sub></small> was examined as a carbon-free cathode catalyst using density functional theory (DFT) calculations and experimental techniques. The intrinsic advantages of MnTiO<small><sub>3</sub></small> stem from the coexistence of Mn and Ti energy levels near the Fermi level, as revealed by our density of states (DOS) analysis. This electronic structure facilitates ORR/OER, thus endowing MnTiO<small><sub>3</sub></small> with a bifunctional role in promoting battery performance. Our DFT-based investigation elucidates the surface stability and catalytic properties of MnTiO<small><sub>3</sub></small>. Furthermore, Energy Dispersive Spectroscopy (EDS) and X-ray diffraction (XRD) confirm that the electrochemical reaction on MnTiO<small><sub>3</sub></small> follows a two-electron pathway. Our findings reveal that a LOB with MnTiO<small><sub>3</sub></small> exhibits a total overpotential of 1.18 V and 1.55 V using DFT and electrochemical measurements, respectively. High current densities up to 1 A g<small><sup>−1</sup></small> also highlight its potential as a cathode catalyst for LOBs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"55 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987860","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}
Jiangtao Chen, Yarong Zhou, Tiancheng Song, Xinyi Wang, Ting Wang, Yun Zhao, Bingjun Yang, Jianbiao Chen, Yi Zhang, Yan Li
Nowadays, smart flexible and wearable electronic devices are experiencing rapid development. As one of core components, flexible pressure sensor has attracted more attentions. High sensitivity, broad detection range and fast response of the pressure sensor with a low power consumption are urgently needed for various practical scenes but it remains a great challenge to simultaneously achieve these merits. Herein, a periodical structured MXene/PDMS composite is explored to construct high performance flexible piezoresistive sensor. The developed sensor has ultrahigh sensitivity (70.6 kPa⁻¹), fast response (18 ms), broad detection range (up to 436 kPa) as well as outstanding long-term stability (9700 cycles). More significantly, the sensor shows a low operation voltage (0.01 V) and low power consumption (Max. 120 μW), which successfully powered by a thermoelectric generator using tiny temperature difference between human skin and environment. We have also combined the sensor with an artificial neural network model and realized a high accuracy recognition (97%) to the Morse code. The results indicate that periodical structured MXene/PDMS sensors hold a great potential in practical applications such as human motion monitoring, robotic control and encrypted communication. Also, this work opens a new way toward highly sensitive, broad-range-response, and multifunctional self-powered energy-saving wearable electronics.
{"title":"Ultralow voltage operation and microwatt power consumption MXene based pressure sensors with excellent sensing performance","authors":"Jiangtao Chen, Yarong Zhou, Tiancheng Song, Xinyi Wang, Ting Wang, Yun Zhao, Bingjun Yang, Jianbiao Chen, Yi Zhang, Yan Li","doi":"10.1039/d4ta08386e","DOIUrl":"https://doi.org/10.1039/d4ta08386e","url":null,"abstract":"Nowadays, smart flexible and wearable electronic devices are experiencing rapid development. As one of core components, flexible pressure sensor has attracted more attentions. High sensitivity, broad detection range and fast response of the pressure sensor with a low power consumption are urgently needed for various practical scenes but it remains a great challenge to simultaneously achieve these merits. Herein, a periodical structured MXene/PDMS composite is explored to construct high performance flexible piezoresistive sensor. The developed sensor has ultrahigh sensitivity (70.6 kPa⁻¹), fast response (18 ms), broad detection range (up to 436 kPa) as well as outstanding long-term stability (9700 cycles). More significantly, the sensor shows a low operation voltage (0.01 V) and low power consumption (Max. 120 μW), which successfully powered by a thermoelectric generator using tiny temperature difference between human skin and environment. We have also combined the sensor with an artificial neural network model and realized a high accuracy recognition (97%) to the Morse code. The results indicate that periodical structured MXene/PDMS sensors hold a great potential in practical applications such as human motion monitoring, robotic control and encrypted communication. Also, this work opens a new way toward highly sensitive, broad-range-response, and multifunctional self-powered energy-saving wearable electronics.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"15 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987867","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}
Pub Date : 2025-01-17DOI: 10.1016/j.apsusc.2025.162432
Jun-Yeong Yang, Seunghun Lee, Eun-Yeon Byeon, Joo Young Park, Do-geun Kim, Seungyeon Hong, Sung Hun Lee, Hyo Jung Kim, Sunghoon Jung
Low-loss flexible copper-clad laminates are required for next-generation ultra-high-frequency communication systems, and fluorinated polymers are one of the good dielectric candidates due to its excellent dielectric properties. However, this necessitates ensuring high adhesion between Cu and the fluorinated polymers that commonly indicate surface inertness. This study investigates the effects of Ar ion beam treatment on the interfacial adhesion between fluorinated ethylene propylene (FEP) films and Cu layers deposited via magnetron sputtering. We increased the accumulated Ar ion dose from 9.8 × 1014 to 8.6 × 1015 ions/cm2, and the maximum peel strength between FEP and Cu was recorded to be 7.4 ± 0.26 N/cm at an ion dose of 5.9 × 1015 ions/cm2 on FEP. Surface characterization revealed that in all samples, the initial delamination occurred within the FEP surface, regardless of the Ar ion dose. Interfacial adhesion of Cu/FEP was attributed to the reinforced mechanical properties of the FEP via increased surface roughness and crystallinity. These findings will contribute to ensuring the reliable interfacial adhesion of Cu/FEP systems for high-frequency communications.
{"title":"Effect of Ar ion beam treatment on the interfacial adhesion between a fluorinated ethylene propylene (FEP) film and sputtered Cu","authors":"Jun-Yeong Yang, Seunghun Lee, Eun-Yeon Byeon, Joo Young Park, Do-geun Kim, Seungyeon Hong, Sung Hun Lee, Hyo Jung Kim, Sunghoon Jung","doi":"10.1016/j.apsusc.2025.162432","DOIUrl":"https://doi.org/10.1016/j.apsusc.2025.162432","url":null,"abstract":"Low-loss flexible copper-clad laminates are required for next-generation ultra-high-frequency communication systems, and fluorinated polymers are one of the good dielectric candidates due to its excellent dielectric properties. However, this necessitates ensuring high adhesion between Cu and the fluorinated polymers that commonly indicate surface inertness. This study investigates the effects of Ar ion beam treatment on the interfacial adhesion between fluorinated ethylene propylene (FEP) films and Cu layers deposited via magnetron sputtering. We increased the accumulated Ar ion dose from 9.8 × 10<sup>14</sup> to 8.6 × 10<sup>15</sup> ions/cm<sup>2</sup>, and the maximum peel strength between FEP and Cu was recorded to be 7.4 ± 0.26 N/cm at an ion dose of 5.9 × 10<sup>15</sup> ions/cm<sup>2</sup> on FEP. Surface characterization revealed that in all samples, the initial delamination occurred within the FEP surface, regardless of the Ar ion dose. Interfacial adhesion of Cu/FEP was attributed to the reinforced mechanical properties of the FEP via increased surface roughness and crystallinity. These findings will contribute to ensuring the reliable interfacial adhesion of Cu/FEP systems for high-frequency communications.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"27 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988060","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}
The MXene, which is usually transition metal carbide, nitride, and carbonitride, is one of the emerging family of 2D materials, exhibiting considerable potential across various research areas. Despite theoretical versatility, practical application of MXene is prohibited due to its spontaneous oxidative degradation. This review meticulously discusses the factors influencing the oxidation of MXenes, considering both thermodynamic and kinetic point of view. The potential mechanisms of oxidation are systematically introduced, based on experimental and theoretical models. Typically, the surfaces and edges of MXenes are susceptible to oxidation, as the surface terminal groups are easily attacked by oxygen and water molecules, ultimately leading to structural deformation. To retard oxidative degradation, ligand mediated surface/edge passivation is suggested as a promising strategy. In this regard, detailed passivation strategies for MXenes are systematically explained based on the types of chemistry at the MXene-ligand interface—covalent bonding, electrostatic interactions, and hydrogen bonding—and the type of stabilizing moieties—organic, inorganic, biomolecules, and polymers. The retardation of oxidation is discussed in relation with the interaction type and passivating moiety. This review aims to catalyze future research to identify efficient and cost-effective ligands for the surface engineering of MXenes, enhancing their oxidation stability.
{"title":"The Future of MXenes: Exploring Oxidative Degradation Pathways and Coping with Surface/Edge Passivation Approach","authors":"Zubair Khalid, Farhan Hadi, Jing Xie, Vidya Chandrabose, Jae-Min Oh","doi":"10.1002/smll.202407856","DOIUrl":"https://doi.org/10.1002/smll.202407856","url":null,"abstract":"The MXene, which is usually transition metal carbide, nitride, and carbonitride, is one of the emerging family of 2D materials, exhibiting considerable potential across various research areas. Despite theoretical versatility, practical application of MXene is prohibited due to its spontaneous oxidative degradation. This review meticulously discusses the factors influencing the oxidation of MXenes, considering both thermodynamic and kinetic point of view. The potential mechanisms of oxidation are systematically introduced, based on experimental and theoretical models. Typically, the surfaces and edges of MXenes are susceptible to oxidation, as the surface terminal groups are easily attacked by oxygen and water molecules, ultimately leading to structural deformation. To retard oxidative degradation, ligand mediated surface/edge passivation is suggested as a promising strategy. In this regard, detailed passivation strategies for MXenes are systematically explained based on the types of chemistry at the MXene-ligand interface—covalent bonding, electrostatic interactions, and hydrogen bonding—and the type of stabilizing moieties—organic, inorganic, biomolecules, and polymers. The retardation of oxidation is discussed in relation with the interaction type and passivating moiety. This review aims to catalyze future research to identify efficient and cost-effective ligands for the surface engineering of MXenes, enhancing their oxidation stability.","PeriodicalId":228,"journal":{"name":"Small","volume":"44 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988109","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}
Pub Date : 2025-01-17DOI: 10.1016/j.electacta.2025.145717
Lihong Liu, Bo Li, Ming Yang, Yannan Mu, Duo zhang, Lihua Huo
Metal oxide and graphene composite material have been a promising material for developing electrochemical sensors. In this work, we prepared graphene (rGO) doped MoO2 hollow nanosphere composite (MoO2/rGO) using a simple one-step solvothermal without any template.The hollow nanosphere was constructed by nanoparticles and uniformly anchored onto graphene sheets.The dopamine (DA) sensor was constructed by modifying the MoO2/rGO composite to the glass carbon electrode (GCE) surface with a simple drop coating (MoO2/rGO/GCE), which shows high sensitivity(101.20 μA·μM-1·cm-2), low detection limit (6.8 nM), high selectivity and good stability for DA. Meanwhile, the MoO2/rGO/GCE demonstrates very little interference with dopamine determination when both Uric acid (UA) and ascorbic acid (AA) are present. The exceptional efficacy of the sensor is attributed to the MoO₂/rGO composite's unique attributes,which include a hollow structure, low charge transfer resistance, a large electrochemical active area, and an abundance of active sites. Furthermore, the MoO₂/rGO/GCE sensor demonstrates capabilities for the detection of minute dopamine levels in human serum, utilizing the standard addition method. This suggests its applicability in the realm of biomedical diagnostics.
{"title":"Prepared Hollow Nanosphere MoO2/rGO Composite for low concentration Dopamine Detection","authors":"Lihong Liu, Bo Li, Ming Yang, Yannan Mu, Duo zhang, Lihua Huo","doi":"10.1016/j.electacta.2025.145717","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.145717","url":null,"abstract":"Metal oxide and graphene composite material have been a promising material for developing electrochemical sensors. In this work, we prepared graphene (rGO) doped MoO<sub>2</sub> hollow nanosphere composite (MoO<sub>2</sub>/rGO) using a simple one-step solvothermal without any template.The hollow nanosphere was constructed by nanoparticles and uniformly anchored onto graphene sheets.The dopamine (DA) sensor was constructed by modifying the MoO<sub>2</sub>/rGO composite to the glass carbon electrode (GCE) surface with a simple drop coating (MoO<sub>2</sub>/rGO/GCE), which shows high sensitivity(101.20 μA·μM<sup>-1</sup>·cm<sup>-2</sup>), low detection limit (6.8 nM), high selectivity and good stability for DA. Meanwhile, the MoO<sub>2</sub>/rGO/GCE demonstrates very little interference with dopamine determination when both Uric acid (UA) and ascorbic acid (AA) are present. The exceptional efficacy of the sensor is attributed to the MoO₂/rGO composite's unique attributes,which include a hollow structure, low charge transfer resistance, a large electrochemical active area, and an abundance of active sites. Furthermore, the MoO₂/rGO/GCE sensor demonstrates capabilities for the detection of minute dopamine levels in human serum, utilizing the standard addition method. This suggests its applicability in the realm of biomedical diagnostics.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"96 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988147","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hydrogen bubble adhesion to the electrode presents a major obstacle for green hydrogen generation via the hydrogen evolution reaction (HER) as it would induce undesired overpotential and undermine the reaction efficiency by reducing reaction area, increasing transport resistance, and creating an undesired ion concentration gradient. While electrodes with aerophobic/hydrophilic surfaces have been developed to facilitate bubble detachment, they primarily rely on micro- and nanostructured catalyst surfaces to enhance buoyance-induced bubble departure. Here, we demonstrate that introducing nonreactive yet more hydrophilic surfaces can promote coalescence-induced bubble departure, thereby significantly reducing the transport overpotential and improving HER performance. Through a systematic study using patterned gold–silicon microstrip (GSM) surfaces with varied gold strip widths (50–1600 μm), we found that reducing the gold strip width results in a smaller bubble departure diameter and increased bubble departure frequencies, leading to a 400 mV reduction in transport overpotential at 400 mA/cm2 on 50 μm wide GSM surfaces. These patterned surfaces demonstrated superior HER performance compared to a plain gold surface, even with a 50% reduction in the reaction area. The optimal HER performance, characterized by the lowest total overpotential, was achieved on GSM surfaces with 200 μm wide gold strips, highlighting the intricate interplay between improved bubble dynamics and reduced reaction area.
{"title":"Enhancing Hydrogen Evolution Reaction through Coalescence-Induced Bubble Departure on Patterned Gold–Silicon Microstrip Surfaces","authors":"Chung-Te Huang, Liangwei Zheng, Yiding Zhong, Jörg G. Werner, Ming-Chang Lu, Chuanhua Duan","doi":"10.1021/acsami.4c18255","DOIUrl":"https://doi.org/10.1021/acsami.4c18255","url":null,"abstract":"Hydrogen bubble adhesion to the electrode presents a major obstacle for green hydrogen generation via the hydrogen evolution reaction (HER) as it would induce undesired overpotential and undermine the reaction efficiency by reducing reaction area, increasing transport resistance, and creating an undesired ion concentration gradient. While electrodes with aerophobic/hydrophilic surfaces have been developed to facilitate bubble detachment, they primarily rely on micro- and nanostructured catalyst surfaces to enhance buoyance-induced bubble departure. Here, we demonstrate that introducing nonreactive yet more hydrophilic surfaces can promote coalescence-induced bubble departure, thereby significantly reducing the transport overpotential and improving HER performance. Through a systematic study using patterned gold–silicon microstrip (GSM) surfaces with varied gold strip widths (50–1600 μm), we found that reducing the gold strip width results in a smaller bubble departure diameter and increased bubble departure frequencies, leading to a 400 mV reduction in transport overpotential at 400 mA/cm<sup>2</sup> on 50 μm wide GSM surfaces. These patterned surfaces demonstrated superior HER performance compared to a plain gold surface, even with a 50% reduction in the reaction area. The optimal HER performance, characterized by the lowest total overpotential, was achieved on GSM surfaces with 200 μm wide gold strips, highlighting the intricate interplay between improved bubble dynamics and reduced reaction area.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"22 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988221","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}
Hydride (H–) species on oxides have been extensively studied over the past few decades because of their critical role in various catalytic processes. Their syntheses require high temperatures and the presence of hydrogen, which involves complex equipment, high energy costs, and strict safety protocols. Hydride species tend to decompose in the presence of atmospheric oxygen and water, which reduces their catalytic activities. These challenges highlight the need for further research to improve the stability and efficiency of catalytic processes and develop safer and cost-effective synthesis methods. This paper introduces an ultrasonic fabrication method for gallium hydride species on liquid metal (LM) nanoparticles (Ga–H@LM NPs) in water and describes the evaluation of their catalytic properties. The Ga–H@LM NPs were synthesized by dispersing liquid metals of eutectic gallium–indium in water using a two-step ultrasonication process in an ice bath. The presence of Ga–H species was confirmed by Fourier-transform infrared spectroscopy. The Ga–H@LM NPs demonstrated the rapid catalytic hydrogenation of 4-nitrophenol and reductive degradation of azo dyes within minutes without the need for external reducing agents like NaBH4. The proposed mechanism involves high-energy ultrasonic cavitation at the interface between LM NPs and water, which promotes the formation of H2 from water and its activation to form Ga–H on particles surface during ultrasonication. This study has significant implications for advancing the field of catalysis because it provides a novel and efficient catalytic method for the synthesis of stable hydride species on gallium oxides.
{"title":"Ultrasonically Activated Liquid Metal Catalysts in Water for Enhanced Hydrogenation Efficiency","authors":"Nichayanan Manyuan, Naoya Tanimoto, Kousuke Ueda, Ken Yamamoto, Tomoharu Tokunaga, Masaki Nishio, Tetsu Yonezawa, Hideya Kawasaki","doi":"10.1021/acsami.4c19936","DOIUrl":"https://doi.org/10.1021/acsami.4c19936","url":null,"abstract":"Hydride (H<sup>–</sup>) species on oxides have been extensively studied over the past few decades because of their critical role in various catalytic processes. Their syntheses require high temperatures and the presence of hydrogen, which involves complex equipment, high energy costs, and strict safety protocols. Hydride species tend to decompose in the presence of atmospheric oxygen and water, which reduces their catalytic activities. These challenges highlight the need for further research to improve the stability and efficiency of catalytic processes and develop safer and cost-effective synthesis methods. This paper introduces an ultrasonic fabrication method for gallium hydride species on liquid metal (LM) nanoparticles (Ga–H@LM NPs) in water and describes the evaluation of their catalytic properties. The Ga–H@LM NPs were synthesized by dispersing liquid metals of eutectic gallium–indium in water using a two-step ultrasonication process in an ice bath. The presence of Ga–H species was confirmed by Fourier-transform infrared spectroscopy. The Ga–H@LM NPs demonstrated the rapid catalytic hydrogenation of 4-nitrophenol and reductive degradation of azo dyes within minutes without the need for external reducing agents like NaBH<sub>4</sub>. The proposed mechanism involves high-energy ultrasonic cavitation at the interface between LM NPs and water, which promotes the formation of H<sub>2</sub> from water and its activation to form Ga–H on particles surface during ultrasonication. This study has significant implications for advancing the field of catalysis because it provides a novel and efficient catalytic method for the synthesis of stable hydride species on gallium oxides.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"25 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988223","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}
Printing of large-area solar panels necessitates advanced organic solar cells with thick active layers. However, increasing the active layer thickness typically leads to a marked drop in the power conversion efficiency. Here we developed an organic semiconductor regulator, called AT-β2O, to tune the crystallization sequence of the components in active layers. When adding AT-β2O in the donor (D18-Cl) and acceptor (N3) blend, N3 crystallizes behind D18-Cl, and this phenomenon is different from the co-crystallization observed in binary D18-Cl:N3 blends. This manipulation of crystallization dynamics is favourable to form bulk-heterojunction-gradient vertical phase separation in the active layer accompanied by the high crystallinity of the acceptor and balanced charge carrier mobilities in thick films. The resultant single-junction organic solar cells exhibited a certified power conversion efficiency of over 20%, as well as demonstrated exceptional adaptability across the active layer thicknesses (100–400 nm) and remarkable universality. Such breakthroughs enable large-area modules with a certified power conversion efficiency of 18.04%.
{"title":"Organic solar cells with 20.82% efficiency and high tolerance of active layer thickness through crystallization sequence manipulation","authors":"Haiyang Chen, Yuting Huang, Rui Zhang, Hongyu Mou, Junyuan Ding, Jiadong Zhou, Zukun Wang, Hongxiang Li, Weijie Chen, Juan Zhu, Qinrong Cheng, Hao Gu, Xiaoxiao Wu, Tianjiao Zhang, Yingyi Wang, Haiming Zhu, Zengqi Xie, Feng Gao, Yaowen Li, Yongfang Li","doi":"10.1038/s41563-024-02062-0","DOIUrl":"https://doi.org/10.1038/s41563-024-02062-0","url":null,"abstract":"<p>Printing of large-area solar panels necessitates advanced organic solar cells with thick active layers. However, increasing the active layer thickness typically leads to a marked drop in the power conversion efficiency. Here we developed an organic semiconductor regulator, called AT-β2O, to tune the crystallization sequence of the components in active layers. When adding AT-β2O in the donor (D18-Cl) and acceptor (N3) blend, N3 crystallizes behind D18-Cl, and this phenomenon is different from the co-crystallization observed in binary D18-Cl:N3 blends. This manipulation of crystallization dynamics is favourable to form bulk-heterojunction-gradient vertical phase separation in the active layer accompanied by the high crystallinity of the acceptor and balanced charge carrier mobilities in thick films. The resultant single-junction organic solar cells exhibited a certified power conversion efficiency of over 20%, as well as demonstrated exceptional adaptability across the active layer thicknesses (100–400 nm) and remarkable universality. Such breakthroughs enable large-area modules with a certified power conversion efficiency of 18.04%.</p>","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"95 1","pages":""},"PeriodicalIF":41.2,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987281","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}