Boyu Ding, Zheheng Jiang, Xinlong Guo, Shukai Wen, Kairui Wang, Shihang Li, Yongqiang Yang, Qihao Sha, Bo Li, Liang Luo, Zhaowang Dan, Yaping Li, Xiaoming Sun
The intrinsically sluggish kinetics of the oxygen evolution reaction (OER) at the anode poses a formidable challenge to the industrial application of water electrolysis, although NiFe-based oxides and hydroxides have emerged as promising anodic candidates. Within this framework, we report the synthesis of Nb-doped NiFe-layered double hydroxides (Nb/NiFe-LDH) via a straightforward one-step hydrothermal approach. Notably, Nb doping maintained the structural integrity of the NiFe-LDH framework and it enhanced the valence state of the active Ni species during the electrochemical activation process, which accelerated the concomitant reconstruction kinetics of the LDH phase. As a result, Nb/NiFe-LDH demonstrated a remarkable overpotential of 198 mV to attain a current density of 10 mA cm−2 in an alkaline electrolyte. This work proposes a novel doping strategy for enhancing the performance of OER electrocatalysts.
{"title":"Formation of electron-deficient Ni in a Nb/NiFe-layered double hydroxide nanoarray via electrochemical activation for efficient water oxidation","authors":"Boyu Ding, Zheheng Jiang, Xinlong Guo, Shukai Wen, Kairui Wang, Shihang Li, Yongqiang Yang, Qihao Sha, Bo Li, Liang Luo, Zhaowang Dan, Yaping Li, Xiaoming Sun","doi":"10.1039/d4nr05492j","DOIUrl":"https://doi.org/10.1039/d4nr05492j","url":null,"abstract":"The intrinsically sluggish kinetics of the oxygen evolution reaction (OER) at the anode poses a formidable challenge to the industrial application of water electrolysis, although NiFe-based oxides and hydroxides have emerged as promising anodic candidates. Within this framework, we report the synthesis of Nb-doped NiFe-layered double hydroxides (Nb/NiFe-LDH) <em>via</em> a straightforward one-step hydrothermal approach. Notably, Nb doping maintained the structural integrity of the NiFe-LDH framework and it enhanced the valence state of the active Ni species during the electrochemical activation process, which accelerated the concomitant reconstruction kinetics of the LDH phase. As a result, Nb/NiFe-LDH demonstrated a remarkable overpotential of 198 mV to attain a current density of 10 mA cm<small><sup>−2</sup></small> in an alkaline electrolyte. This work proposes a novel doping strategy for enhancing the performance of OER electrocatalysts.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"36 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561126","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}
Husnu Aslan, Khaled Kaja, Jose Morán-Meza, François Piquemal, Jose Alvarez, Nicolas Chauvin, José Penuelas, Steffan Moeller Soenderskov, Philippe Regreny
In this article, we present a comprehensive study utilizing Atomic Force Microscopy (AFM) as a multimetrological platform for the characterization of novel energy harvesting devices, with a particular focus on optical nanomaterials - nanowires. Despite their challenging structure, AFM offers exceptional versatility in probing dimensional and functional properties of nanowires at the nanoscale. We demonstrate the capabilities of AFM measurements to provide an extensive understanding of the structural, electrical, and spectroscopic properties of nanowires using different operational modes, including Electrostatic Force Microscopy (EFM), Kelvin Probe Force Microscopy (KPFM), and Conductive-AFM (C-AFM). Our findings establish AFM as an invaluable metrological tool for the development of cutting-edge energy harvesting technologies and optical nanomaterials.
{"title":"Atomic Force Microscopy as a Multimetrological Platform for Energy Devices","authors":"Husnu Aslan, Khaled Kaja, Jose Morán-Meza, François Piquemal, Jose Alvarez, Nicolas Chauvin, José Penuelas, Steffan Moeller Soenderskov, Philippe Regreny","doi":"10.1039/d4nr05107f","DOIUrl":"https://doi.org/10.1039/d4nr05107f","url":null,"abstract":"In this article, we present a comprehensive study utilizing Atomic Force Microscopy (AFM) as a multimetrological platform for the characterization of novel energy harvesting devices, with a particular focus on optical nanomaterials - nanowires. Despite their challenging structure, AFM offers exceptional versatility in probing dimensional and functional properties of nanowires at the nanoscale. We demonstrate the capabilities of AFM measurements to provide an extensive understanding of the structural, electrical, and spectroscopic properties of nanowires using different operational modes, including Electrostatic Force Microscopy (EFM), Kelvin Probe Force Microscopy (KPFM), and Conductive-AFM (C-AFM). Our findings establish AFM as an invaluable metrological tool for the development of cutting-edge energy harvesting technologies and optical nanomaterials.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"8 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561128","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}
Laura Gutiérrez-Gálvez, Estefanía Enebral-Romero, Miguel Ángel Valle Amores, Clara Pina Coronado, Iñigo Torres, David López-Diego, Mónica Luna, Alberto Fraile, Félix Zamora, José Alemán, Jesús Álvarez, María José Capitán, Encarnación Lorenzo, Tania García-Mendiola
In this work, an electrochemical biosensor is prepared based on few-layer bismuthene hexagons (FLBHs) and a water-soluble BODIPY (BDP) derivative (BDP-NaSO3) for early infection diagnosis. In particular, the detection in advance of a virus sequence in nasopharyngeal swab samples was developed. The combination of the FLBHs and BDP-NaSO3 facilitates the direct, sensitive, and specific detection of gene viruses without the need for any prior amplification step. This work demonstrates that the FLBHs provide an improved electrochemical platform for immobilizing thiolated DNA capture probes that increase the sensitivity of the biosensor, while BDP-NaSO3 serves as a newly powerful electrochemical indicator of the hybridization event. As a proof of concept, SARS-CoV-2 was selected as the model virus. The developed biosensor demonstrated selective, rapid, and straightforward detection of the specific sequence RNA-dependent RNA-polymerase (RdRp) of SARS-CoV-2 with a detection limit of 4.97 fM and a linear range from 16.6 fM to 100 fM. Furthermore, this platform successfully detects the virus directly in nasopharyngeal swab samples with a viral load of at least 19 Cts without being subjected to any prior amplification stage. Finally, the high stability of the biosensor response, which has been working under ambient conditions for over one month, the selectivity and rapidity for specific virus detection, and the requirement of low-volume samples for the determination are remarkable characteristics that make it ideal for its potential application in clinical diagnosis in point-of-care settings.
{"title":"Advancing diagnostics with BODIPY-bismuthene DNA biosensors","authors":"Laura Gutiérrez-Gálvez, Estefanía Enebral-Romero, Miguel Ángel Valle Amores, Clara Pina Coronado, Iñigo Torres, David López-Diego, Mónica Luna, Alberto Fraile, Félix Zamora, José Alemán, Jesús Álvarez, María José Capitán, Encarnación Lorenzo, Tania García-Mendiola","doi":"10.1039/d4nr05258g","DOIUrl":"https://doi.org/10.1039/d4nr05258g","url":null,"abstract":"In this work, an electrochemical biosensor is prepared based on few-layer bismuthene hexagons (FLBHs) and a water-soluble BODIPY (BDP) derivative (BDP-NaSO<small><sub>3</sub></small>) for early infection diagnosis. In particular, the detection in advance of a virus sequence in nasopharyngeal swab samples was developed. The combination of the FLBHs and BDP-NaSO<small><sub>3</sub></small> facilitates the direct, sensitive, and specific detection of gene viruses without the need for any prior amplification step. This work demonstrates that the FLBHs provide an improved electrochemical platform for immobilizing thiolated DNA capture probes that increase the sensitivity of the biosensor, while BDP-NaSO<small><sub>3</sub></small> serves as a newly powerful electrochemical indicator of the hybridization event. As a proof of concept, SARS-CoV-2 was selected as the model virus. The developed biosensor demonstrated selective, rapid, and straightforward detection of the specific sequence RNA-dependent RNA-polymerase (RdRp) of SARS-CoV-2 with a detection limit of 4.97 fM and a linear range from 16.6 fM to 100 fM. Furthermore, this platform successfully detects the virus directly in nasopharyngeal swab samples with a viral load of at least 19 Cts without being subjected to any prior amplification stage. Finally, the high stability of the biosensor response, which has been working under ambient conditions for over one month, the selectivity and rapidity for specific virus detection, and the requirement of low-volume samples for the determination are remarkable characteristics that make it ideal for its potential application in clinical diagnosis in point-of-care settings.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"11 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561129","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}
Dinglong Xu, Zhaoyang Jing, Hong Wang, Weijun Yang, Pengwu Xu, Deyu Niu, Piming Ma
With the advent of the smart era, the demand for clean energy is rising, and flexible triboelectric nanogenerators (F-TENGs) based on elastomers have garnered significant attention. Based on the principles of electrostatic induction and coupling, F-TENGs can convert mechanical motion into electrical energy and are widely utilized in wearable devices and blue energy. F-TENGs offer a simple design, ease of manufacturing, and flexible usage scenarios. However, several weaknesses still limit their development. For example, F-TENG materials cannot recover from fatigue damage and are prone to output performance degradation under frequent friction or complex external conditions, leading to failure. To address these issues, researchers have explored the use of self-healable flexible polymer-based friction layers and electrodes. This review will provide a detailed summary of the key scientific and technological challenges faced by F-TENGs in complex and harsh environments, including ambient, high and low temperatures, high humidity, and strong acids and bases. Furthermore, the detailed research progress addressing these issues and the future development of F-TENGs will also be presented and explored. This paper aims to provide valuable insights and guidance for in-depth research and broad applications of flexible TENGs.
{"title":"Advanced flexible self-healing triboelectric nanogenerators for applications in complex environments","authors":"Dinglong Xu, Zhaoyang Jing, Hong Wang, Weijun Yang, Pengwu Xu, Deyu Niu, Piming Ma","doi":"10.1039/d4nr05170j","DOIUrl":"https://doi.org/10.1039/d4nr05170j","url":null,"abstract":"With the advent of the smart era, the demand for clean energy is rising, and flexible triboelectric nanogenerators (F-TENGs) based on elastomers have garnered significant attention. Based on the principles of electrostatic induction and coupling, F-TENGs can convert mechanical motion into electrical energy and are widely utilized in wearable devices and blue energy. F-TENGs offer a simple design, ease of manufacturing, and flexible usage scenarios. However, several weaknesses still limit their development. For example, F-TENG materials cannot recover from fatigue damage and are prone to output performance degradation under frequent friction or complex external conditions, leading to failure. To address these issues, researchers have explored the use of self-healable flexible polymer-based friction layers and electrodes. This review will provide a detailed summary of the key scientific and technological challenges faced by F-TENGs in complex and harsh environments, including ambient, high and low temperatures, high humidity, and strong acids and bases. Furthermore, the detailed research progress addressing these issues and the future development of F-TENGs will also be presented and explored. This paper aims to provide valuable insights and guidance for in-depth research and broad applications of flexible TENGs.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"2 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561131","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}
Aqueous manganese-ion batteries (MIBs) are distinguished as a possible choice for energy storage systems since the Mn anode could offer superior theoretical capacity and low redox potential. However, the capacities of cathode materials are usually limited by the large radius of solvated Mn2+. Herein, binder-free V2O5-carbon nanotube film (VO-CNT) cathodes were designed through a straightforward suction filtration method. In the films, V2O5 with open layered framework is desired to provide abundant ion transfer channels. More excited, the VO-CNT cathodes allow the co-intercalation/extraction of Mn2+ and H+ ions. Such charge storage mechanism significantly optimizes the electrochemical performance of the batteries. In addition, the carbon nanotubes form a continuous high-conductive scaffold in the film, which could contribute to good conductivity of the whole cathode. Leveraging the synergistic advantages of V2O5 and carbon nanotubes, the binder-free VO-CNT cathodes display a high capacity, exceptional rate capability, and robust cycling stability, retaining 96% capacity over 1000 cycles. This work will open new avenues to design outstanding-performance cathodes for aqueous MIBs.
{"title":"Binder-Free V2O5-Carbon Nanotube Composite Films for High-Performance Aqueous Manganese-Ion Batteries","authors":"Jianan Zhao, Xinyu Wang, Xinqi Xie, Hongmei Cao","doi":"10.1039/d5nr00074b","DOIUrl":"https://doi.org/10.1039/d5nr00074b","url":null,"abstract":"Aqueous manganese-ion batteries (MIBs) are distinguished as a possible choice for energy storage systems since the Mn anode could offer superior theoretical capacity and low redox potential. However, the capacities of cathode materials are usually limited by the large radius of solvated Mn2+. Herein, binder-free V2O5-carbon nanotube film (VO-CNT) cathodes were designed through a straightforward suction filtration method. In the films, V2O5 with open layered framework is desired to provide abundant ion transfer channels. More excited, the VO-CNT cathodes allow the co-intercalation/extraction of Mn2+ and H+ ions. Such charge storage mechanism significantly optimizes the electrochemical performance of the batteries. In addition, the carbon nanotubes form a continuous high-conductive scaffold in the film, which could contribute to good conductivity of the whole cathode. Leveraging the synergistic advantages of V2O5 and carbon nanotubes, the binder-free VO-CNT cathodes display a high capacity, exceptional rate capability, and robust cycling stability, retaining 96% capacity over 1000 cycles. This work will open new avenues to design outstanding-performance cathodes for aqueous MIBs.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"33 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561150","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}
Andrey D. Trofimov, Andrey Emelyanov, Anna Matsukatova, Alexander A. Nesmelov, Sergei Zav'yalov, Timofey Patsaev, Pavel Forsh, Gang Liu, Vladimir Rylkov, Vyacheslav A. Demin
Resistive switching (RS) memory devices incorporated with the capabilities of in situ data sensing, storing and processing are promising for artificial intelligence applications. In this respect, controlling resistance not only by electrical but also optical stimulations provides attractive opportunities for the development of novel neuromorphic sensing and computing systems. Here, we demonstrate the RS of Cu/parylene-PbTe/ITO memristive devices and the dependence of RS on optical excitation for efficient neuromorphic computing with a high classification accuracy. The main memristive characteristics (multilevel resistive states, RS voltages, endurance, retention, RS time and energy, etc.) are evaluated with account of temporal and spatial variations. Additionally, the devices demonstrate a range of synaptic plasticity behaviors, such as spike-timing(amplitude,width)-dependent plasticity, long-term potentiation and depression. A qualitative model that describes photosensitive RS and takes into account the influence of photo-generated charge carriers on conductive filament growth is proposed based on the experimental results. This work presents an appealing approach towards the development of photosensitive memristive devices for upcoming neuromorphic sensing and computing systems.
{"title":"Photosensitive resistive switching in parylene-PbTe nanocomposite memristors for neuromorphic computing","authors":"Andrey D. Trofimov, Andrey Emelyanov, Anna Matsukatova, Alexander A. Nesmelov, Sergei Zav'yalov, Timofey Patsaev, Pavel Forsh, Gang Liu, Vladimir Rylkov, Vyacheslav A. Demin","doi":"10.1039/d5nr00456j","DOIUrl":"https://doi.org/10.1039/d5nr00456j","url":null,"abstract":"Resistive switching (RS) memory devices incorporated with the capabilities of in situ data sensing, storing and processing are promising for artificial intelligence applications. In this respect, controlling resistance not only by electrical but also optical stimulations provides attractive opportunities for the development of novel neuromorphic sensing and computing systems. Here, we demonstrate the RS of Cu/parylene-PbTe/ITO memristive devices and the dependence of RS on optical excitation for efficient neuromorphic computing with a high classification accuracy. The main memristive characteristics (multilevel resistive states, RS voltages, endurance, retention, RS time and energy, etc.) are evaluated with account of temporal and spatial variations. Additionally, the devices demonstrate a range of synaptic plasticity behaviors, such as spike-timing(amplitude,width)-dependent plasticity, long-term potentiation and depression. A qualitative model that describes photosensitive RS and takes into account the influence of photo-generated charge carriers on conductive filament growth is proposed based on the experimental results. This work presents an appealing approach towards the development of photosensitive memristive devices for upcoming neuromorphic sensing and computing systems.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"50 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561130","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}
Ravinder Chahal, Sirsendu Ghosal, Joydip Ghosh, P. K. Giri
Surface-enhanced Raman scattering (SERS) is a powerful spectroscopic method known for its ultrasensitive characterization capabilities. Recently, Lead-based halide perovskites incorporated with noble metals have gained much attention as a SERS substrate. However, its practical applications are often hindered by the toxicity of the lead content and low stability. Herein, for the first time, we have synthesized Lead-free halide double perovskite (DP) Cs2AgBiBr6 to overcome the toxicity, stability, and uniformity and studied the performance of lead-based perovskites SERS substrates. The self-trapped exciton (STEs) defects were controlled by post-growth annealing of the sample in an Argon (Ar) atmosphere, minimizing the AgBi and BiAg anti-site disorder. The sample with the highest STE defects demonstrates the highest SERS performance owing to the defect-assisted charge transfer process. We successfully identified methylene blue (MB) and rhodamine 6G (R6G) at concentrations as low as ~10-10 M, achieving remarkable SERS enhancement factor (EF) of 5.04×107 and 1.37×107, respectively, which is highly significant for a semiconductor-based SERS substrate. Additionally, notable amplification was observed for other cationic dyes, including Crystal Violate (CV), Rhodamine B (RhB), Malachite Green (MG). By varying the annealing temperature and the deconvolution of the photoluminescence spectra, we demonstrate a direct correlation between the defect density and the SERS signal intensity. To further understand the underlying enhancement mechanisms, we analyzed the individual contributions of chemical and electromagnetic enhancements to the overall SERS amplification. This analysis was conducted using finite element method (FEM) simulations and density functional theory (DFT) computations. These insights provide a foundational basis for designing highly efficient, metal-free SERS substrates, opening new possibilities for advanced detection technologies. Additionally, the Cs2AgBiBr6 substrate exhibited excellent stability, retaining performance after four months of storage in ambient conditions, highlighting its potential for environmental monitoring.
{"title":"Lead-free Halide Double Perovskites Nanoflakes as High-Performance SERS Substrates for Detection of Trace Organic Pollutants: Chemical Enhancement versus Electromagnetic Enhancement","authors":"Ravinder Chahal, Sirsendu Ghosal, Joydip Ghosh, P. K. Giri","doi":"10.1039/d5nr00437c","DOIUrl":"https://doi.org/10.1039/d5nr00437c","url":null,"abstract":"Surface-enhanced Raman scattering (SERS) is a powerful spectroscopic method known for its ultrasensitive characterization capabilities. Recently, Lead-based halide perovskites incorporated with noble metals have gained much attention as a SERS substrate. However, its practical applications are often hindered by the toxicity of the lead content and low stability. Herein, for the first time, we have synthesized Lead-free halide double perovskite (DP) Cs2AgBiBr6 to overcome the toxicity, stability, and uniformity and studied the performance of lead-based perovskites SERS substrates. The self-trapped exciton (STEs) defects were controlled by post-growth annealing of the sample in an Argon (Ar) atmosphere, minimizing the AgBi and BiAg anti-site disorder. The sample with the highest STE defects demonstrates the highest SERS performance owing to the defect-assisted charge transfer process. We successfully identified methylene blue (MB) and rhodamine 6G (R6G) at concentrations as low as ~10-10 M, achieving remarkable SERS enhancement factor (EF) of 5.04×107 and 1.37×107, respectively, which is highly significant for a semiconductor-based SERS substrate. Additionally, notable amplification was observed for other cationic dyes, including Crystal Violate (CV), Rhodamine B (RhB), Malachite Green (MG). By varying the annealing temperature and the deconvolution of the photoluminescence spectra, we demonstrate a direct correlation between the defect density and the SERS signal intensity. To further understand the underlying enhancement mechanisms, we analyzed the individual contributions of chemical and electromagnetic enhancements to the overall SERS amplification. This analysis was conducted using finite element method (FEM) simulations and density functional theory (DFT) computations. These insights provide a foundational basis for designing highly efficient, metal-free SERS substrates, opening new possibilities for advanced detection technologies. Additionally, the Cs2AgBiBr6 substrate exhibited excellent stability, retaining performance after four months of storage in ambient conditions, highlighting its potential for environmental monitoring.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"15 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546913","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}
Electrosynthesis of hydrogen peroxide (H2O2) through the two-electron oxygen reduction reaction (2e-ORR) is environmentally friendly and sustainable. Transition-metal single-atom catalysts (SACs) have gained attention for this application due to their low cost, high atom utilization, adjustable coordination, and geometric isolation of active metal sites. Although various synthetic methods of SACs have been reported, the specific mechanism of the formation of active sites is still less studied. Herein, we presented the molecular coordination inheritance strategy for synthesizing 2e-ORR SACs with well-defined coordination environments and investigated the formation mechanism of the active sites. We select precursors including [Co(II)Salen], CoPc, Co(acac)2 to achieve specific configurations (Co-N2O2, Co-N4, Co-O4). Our results indicate that the precursors undergo decomposition and are partially embedded in the carbon substrate at lower temperatures, facilitating the inheritance of the desired configurations. As the temperature increases, the inherited configurations will rearrange, forming dual-atom structures and metal particles gradually. Among the Co-N2O2, Co-N4, and Co-O4 catalysts, the Co-N2O2 catalyst demonstrates the highest 2e-ORR selectivity. This work reveals the mechanism of regulating SAC's active site structure by the molecular coordination inheritance strategy, which may provide new insights for further research on the precise regulation and formation mechanism of SAC's active site.
{"title":"Molecular Coordination Inheritance of Single Co Atom Catalysts for Two-Electron Oxygen Reduction Reaction","authors":"Qianqian Qin, Mengxue Huang, Chaoqi Han, Xue Jing, Wenwen Shi, Ruimin Ding, Xi Yin","doi":"10.1039/d5nr00337g","DOIUrl":"https://doi.org/10.1039/d5nr00337g","url":null,"abstract":"Electrosynthesis of hydrogen peroxide (H2O2) through the two-electron oxygen reduction reaction (2e-ORR) is environmentally friendly and sustainable. Transition-metal single-atom catalysts (SACs) have gained attention for this application due to their low cost, high atom utilization, adjustable coordination, and geometric isolation of active metal sites. Although various synthetic methods of SACs have been reported, the specific mechanism of the formation of active sites is still less studied. Herein, we presented the molecular coordination inheritance strategy for synthesizing 2e-ORR SACs with well-defined coordination environments and investigated the formation mechanism of the active sites. We select precursors including [Co(II)Salen], CoPc, Co(acac)2 to achieve specific configurations (Co-N2O2, Co-N4, Co-O4). Our results indicate that the precursors undergo decomposition and are partially embedded in the carbon substrate at lower temperatures, facilitating the inheritance of the desired configurations. As the temperature increases, the inherited configurations will rearrange, forming dual-atom structures and metal particles gradually. Among the Co-N2O2, Co-N4, and Co-O4 catalysts, the Co-N2O2 catalyst demonstrates the highest 2e-ORR selectivity. This work reveals the mechanism of regulating SAC's active site structure by the molecular coordination inheritance strategy, which may provide new insights for further research on the precise regulation and formation mechanism of SAC's active site.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"2 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546683","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}
Jiasheng Wang, Tianyu Zhang, Jiliang Song, Fengxin Zhang, Hong Liu, Wan-Hui Wang, Ming Bao
Unsaturated alcohols (UOLs) are important fine chemical intermediates. Thus, it is of great significance to design and prepare catalysts for highly selective hydrogenation of CO of α,β-unsaturated aldehydes (UALs). In this paper, a fluffy mesoporous Al2O3-supported Ag–In2O3 catalyst (Ag-In2O3/f-m-Al2O3) was synthesized by employing a two-solvent method, in which Ag and In2O3 form a Mott–Schottky junction and lead to electron transfer from In2O3 to Ag. Electron-rich Ag repels the CC bond owing to “four-electron repulsion”, and electron-deficient In2O3 acts as the electrophilic site to adsorb the O atom of the CO bond, thus improving the selectivity towards UOLs. In addition to a larger specific surface area and smaller mass transfer resistance, the fluffy mesopore Al2O3 exhibits a large number of Lewis acid sites, which can further improve UOL selectivity. With the help of Ag–In2O3/f-m-Al2O3, high UOL selectivity can be obtained from UALs containing aliphatic, aromatic and heterocyclic groups. This elaborate design of the catalyst could contribute to the highly selective hydrogenation of UALs to UOLs.
{"title":"Fluffy mesoporous Al2O3 supported Ag–In2O3 schottky junction catalysts for selective hydrogenation of CO of α,β-unsaturated aldehydes","authors":"Jiasheng Wang, Tianyu Zhang, Jiliang Song, Fengxin Zhang, Hong Liu, Wan-Hui Wang, Ming Bao","doi":"10.1039/d4nr05518g","DOIUrl":"https://doi.org/10.1039/d4nr05518g","url":null,"abstract":"Unsaturated alcohols (UOLs) are important fine chemical intermediates. Thus, it is of great significance to design and prepare catalysts for highly selective hydrogenation of C<img alt=\"[double bond, length as m-dash]\" border=\"0\" src=\"https://www.rsc.org/images/entities/char_e001.gif\"/>O of α,β-unsaturated aldehydes (UALs). In this paper, a fluffy mesoporous Al<small><sub>2</sub></small>O<small><sub>3</sub></small>-supported Ag–In<small><sub>2</sub></small>O<small><sub>3</sub></small> catalyst (Ag-In<small><sub>2</sub></small>O<small><sub>3</sub></small>/<em>f-m</em>-Al<small><sub>2</sub></small>O<small><sub>3</sub></small>) was synthesized by employing a two-solvent method, in which Ag and In<small><sub>2</sub></small>O<small><sub>3</sub></small> form a Mott–Schottky junction and lead to electron transfer from In<small><sub>2</sub></small>O<small><sub>3</sub></small> to Ag. Electron-rich Ag repels the C<img alt=\"[double bond, length as m-dash]\" border=\"0\" src=\"https://www.rsc.org/images/entities/char_e001.gif\"/>C bond owing to “four-electron repulsion”, and electron-deficient In<small><sub>2</sub></small>O<small><sub>3</sub></small> acts as the electrophilic site to adsorb the O atom of the C<img alt=\"[double bond, length as m-dash]\" border=\"0\" src=\"https://www.rsc.org/images/entities/char_e001.gif\"/>O bond, thus improving the selectivity towards UOLs. In addition to a larger specific surface area and smaller mass transfer resistance, the fluffy mesopore Al<small><sub>2</sub></small>O<small><sub>3</sub></small> exhibits a large number of Lewis acid sites, which can further improve UOL selectivity. With the help of Ag–In<small><sub>2</sub></small>O<small><sub>3</sub></small>/<em>f-m</em>-Al<small><sub>2</sub></small>O<small><sub>3</sub></small>, high UOL selectivity can be obtained from UALs containing aliphatic, aromatic and heterocyclic groups. This elaborate design of the catalyst could contribute to the highly selective hydrogenation of UALs to UOLs.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"8 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546911","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}
We report the fabrication of pristine yttria (Y2O3) polycrystalline nanowires (NWs) by electrospinning method. An intense green photoluminescence (GPL) emission at 544 nm was observed from the Y2O3 nanograins with a statistical average crystallite size of 14.3 nm. Interestingly, the full-shell d electrons Y2O3 NWs are found weakly antiferromagnetic, and the effective magnetic moment was estimated as 1.62 10-4 B/per O at 10 K. The volume fraction of oxygen anion vacancies [VO]+ was estimated to be 1.62 % in the anion-defective electrospun Y2O3 NWs. A symmetric electron paramagnetic resonance signal at g 2.0415 revealed the presence of an unpaired electron trapped in the Y2O3 NWs. Finally, a [VO]+ electron-trapped state, i.e. F-center mechanism is proposed to explain the PL and correlating weak magnetism, which provides new insight into the origin of 4d0 diluted magnetism in nonmagnetic closed-shell Y2O3 NWs (spin from Y2O3) with GPL.
{"title":"Unexpected green-light emission and correlating room-temperature diluted magnetism in pristine non-magnetic closed-shell 4d0 yttria nanowires","authors":"Jianmin Li, Yun-Bing Hu","doi":"10.1039/d5nr00231a","DOIUrl":"https://doi.org/10.1039/d5nr00231a","url":null,"abstract":"We report the fabrication of pristine yttria (Y2O3) polycrystalline nanowires (NWs) by electrospinning method. An intense green photoluminescence (GPL) emission at 544 nm was observed from the Y2O3 nanograins with a statistical average crystallite size of 14.3 nm. Interestingly, the full-shell d electrons Y2O3 NWs are found weakly antiferromagnetic, and the effective magnetic moment was estimated as 1.62 10-4 B/per O at 10 K. The volume fraction of oxygen anion vacancies [VO]+ was estimated to be 1.62 % in the anion-defective electrospun Y2O3 NWs. A symmetric electron paramagnetic resonance signal at g 2.0415 revealed the presence of an unpaired electron trapped in the Y2O3 NWs. Finally, a [VO]+ electron-trapped state, i.e. F-center mechanism is proposed to explain the PL and correlating weak magnetism, which provides new insight into the origin of 4d0 diluted magnetism in nonmagnetic closed-shell Y2O3 NWs (spin from Y2O3) with GPL.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"67 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546682","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}
![[double bond, length as m-dash]](https://www.rsc.org/images/entities/char_e001.gif)
O of α,β-unsaturated aldehydes (UALs). In this paper, a fluffy mesoporous Al2O3-supported Ag–In2O3 catalyst (Ag-In2O3/f-m-Al2O3) was synthesized by employing a two-solvent method, in which Ag and In2O3 form a Mott–Schottky junction and lead to electron transfer from In2O3 to Ag. Electron-rich Ag repels the C
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