ACS Nanoscience Au最新文献

{"title":"Intermolecular Interactions and Quantum Interference Effects in Molecular Junctions.","authors":"Louise O H Hyllested, Idunn Prestholm, Gemma C Solomon","doi":"10.1021/acsnanoscienceau.4c00041","DOIUrl":"10.1021/acsnanoscienceau.4c00041","url":null,"abstract":"<p><p>Destructive quantum interference (DQI) leads to a decrease in the conductance of certain well-documented molecules. Experimental observations have revealed both direct and indirect manifestations of DQI, although a comprehensive understanding of the underlying causes of these distinct outcomes remains elusive. In both cases, DQI lowers the conductance, but only the direct case exhibits a characteristic V-shaped dip in differential conductance. Currently, the direct signature has exclusively been observed in monolayers and gated single-molecule systems. In this study, we employ density functional theory to elucidate a plausible explanation for the absence of a direct DQI signature in single molecules. Specifically, we attribute the direct DQI signature to a resonance shift induced by intermolecular interactions, which are absent in the individual molecules. By illustrating the impact of these intermolecular interactions, we emphasize the need for explicit treatment of intermolecular interactions when simulating monolayers.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"4 6","pages":"426-434"},"PeriodicalIF":4.8,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11659890/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142878075","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Intermolecular Interactions and Quantum Interference Effects in Molecular Junctions","authors":"Louise O. H. Hyllested,&nbsp;Idunn Prestholm and Gemma C. Solomon*,&nbsp;","doi":"10.1021/acsnanoscienceau.4c0004110.1021/acsnanoscienceau.4c00041","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00041https://doi.org/10.1021/acsnanoscienceau.4c00041","url":null,"abstract":"<p >Destructive quantum interference (DQI) leads to a decrease in the conductance of certain well-documented molecules. Experimental observations have revealed both direct and indirect manifestations of DQI, although a comprehensive understanding of the underlying causes of these distinct outcomes remains elusive. In both cases, DQI lowers the conductance, but only the direct case exhibits a characteristic V-shaped dip in differential conductance. Currently, the direct signature has exclusively been observed in monolayers and gated single-molecule systems. In this study, we employ density functional theory to elucidate a plausible explanation for the absence of a direct DQI signature in single molecules. Specifically, we attribute the direct DQI signature to a resonance shift induced by intermolecular interactions, which are absent in the individual molecules. By illustrating the impact of these intermolecular interactions, we emphasize the need for explicit treatment of intermolecular interactions when simulating monolayers.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"4 6","pages":"426–434 426–434"},"PeriodicalIF":4.8,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.4c00041","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142844176","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synergistic Effects of ZnO@NiM′-Layered Double Hydroxide (M′ = Mn, Co, and Fe) Composites on Supercapacitor Performance: A Comparative Evaluation","authors":"Gaurav Pandey, Surendra Serawat, Kamlendra Awasthi","doi":"10.1021/acsnanoscienceau.4c00029","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00029","url":null,"abstract":"The development of supercapacitors is pivotal for sustainable energy storage solutions, necessitating the advancement of innovative electrode materials to supplant fossil-fuel-based energy sources. Zinc oxide (ZnO) is widely studied for use in supercapacitor electrodes because of its beneficial physicochemical properties, including excellent chemical and thermal stability, semiconducting characteristics, low cost, and environmentally friendly nature. In this study, ZnO nanorods were synthesized using a simple hydrothermal method and then combined with various Ni-based layered double hydroxides (LDHs) [NiM′-LDHs (M′ = Mn, Co, and Fe)] to improve the electrochemical performance of the ZnO nanorods. These LDHs are well-known for their outstanding electrochemical and electronic properties, high specific capacitance, and efficient dispersion of cations within host nanolayers. The synthesized composites ZnO@NiMn-LDH, ZnO@NiCo-LDH, and ZnO@NiFe-LDH exhibit enhanced specific capacitances of 569.3, 284.6, and 133.0 F/g, respectively, at a current rate of 1 A/g, outperforming bare ZnO (98.4 F/g). Notably, ZnO@NiMn-LDH demonstrates superior electrochemical performance along with a capacitance retention of 76%, compared to ZnO@NiCo-LDH (58%), ZnO@NiFe-LDH (49%), and bare ZnO (23%) over 5000 cycles. Furthermore, an asymmetric supercapacitor (ASC) was developed by using ZnO@NiMn-LDH as the positive electrode and activated carbon (AC) as the negative electrode to assess its practical applicability. The fabricated ASC (ZnO@NiMn-LDH//AC) demonstrated a specific capacitance of 45.22 F/g at a current rate of 1 A/g, an energy density of 16.08 W h/kg at a power density of 798.8 W/kg, and a capacitance retention of 75% over 5000 cycles. These findings underscore the potential of the composite formation of ZnO with Ni-based LDHs in advancing the efficiency and durability of supercapacitors.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"41 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142266161","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synergistic Effects of ZnO@NiM′-Layered Double Hydroxide (M′ = Mn, Co, and Fe) Composites on Supercapacitor Performance: A Comparative Evaluation","authors":"Gaurav Pandey,&nbsp;Surendra Serawat and Kamlendra Awasthi*,&nbsp;","doi":"10.1021/acsnanoscienceau.4c0002910.1021/acsnanoscienceau.4c00029","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00029https://doi.org/10.1021/acsnanoscienceau.4c00029","url":null,"abstract":"<p >The development of supercapacitors is pivotal for sustainable energy storage solutions, necessitating the advancement of innovative electrode materials to supplant fossil-fuel-based energy sources. Zinc oxide (ZnO) is widely studied for use in supercapacitor electrodes because of its beneficial physicochemical properties, including excellent chemical and thermal stability, semiconducting characteristics, low cost, and environmentally friendly nature. In this study, ZnO nanorods were synthesized using a simple hydrothermal method and then combined with various Ni-based layered double hydroxides (LDHs) [NiM′-LDHs (M′ = Mn, Co, and Fe)] to improve the electrochemical performance of the ZnO nanorods. These LDHs are well-known for their outstanding electrochemical and electronic properties, high specific capacitance, and efficient dispersion of cations within host nanolayers. The synthesized composites ZnO@NiMn-LDH, ZnO@NiCo-LDH, and ZnO@NiFe-LDH exhibit enhanced specific capacitances of 569.3, 284.6, and 133.0 F/g, respectively, at a current rate of 1 A/g, outperforming bare ZnO (98.4 F/g). Notably, ZnO@NiMn-LDH demonstrates superior electrochemical performance along with a capacitance retention of 76%, compared to ZnO@NiCo-LDH (58%), ZnO@NiFe-LDH (49%), and bare ZnO (23%) over 5000 cycles. Furthermore, an asymmetric supercapacitor (ASC) was developed by using ZnO@NiMn-LDH as the positive electrode and activated carbon (AC) as the negative electrode to assess its practical applicability. The fabricated ASC (ZnO@NiMn-LDH//AC) demonstrated a specific capacitance of 45.22 F/g at a current rate of 1 A/g, an energy density of 16.08 W h/kg at a power density of 798.8 W/kg, and a capacitance retention of 75% over 5000 cycles. These findings underscore the potential of the composite formation of ZnO with Ni-based LDHs in advancing the efficiency and durability of supercapacitors.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"4 6","pages":"399–408 399–408"},"PeriodicalIF":4.8,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.4c00029","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142851209","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Crystal Facet Regulation and Ru Incorporation of Co3O4 for Acidic Oxygen Evolution Reaction Electrocatalysis","authors":"Mengting Zhao, Hanfeng Liang","doi":"10.1021/acsnanoscienceau.4c00037","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00037","url":null,"abstract":"Acidic oxygen evolution reaction (OER) has long been the bottleneck of proton exchange membrane water electrolysis. Ru- and Ir-based oxides are currently state-of-the-art electrocatalysts for acidic OER, but their high cost limits their widespread application. Co₃O₄ is a promising alternative, yet the performance requires further improvement. Crystal facet engineering can effectively regulate the kinetics of surface electrochemistry and thus enhance the OER performance. However, the facet-dependent OER activity and corrosion behavior of Co₃O₄ have not been thoroughly studied. In this study, we systematically investigated the OER performance and crystal facet dependency of Co₃O₄. The results demonstrate that Co₃O₄ with mixed {111} and {110} facets exhibits better OER activity and stability than Co₃O₄ with {111} or {100} facets. The surface Co³⁺ species are responsible for the high OER activity, but its transformation to CoO₂ is also the root cause of the dissolution, leading to an activity–stability trade-off effect. The possible approach to addressing this issue would be to increase the Co³⁺ contents by nanostructure engineering. To further improve the performance, Ru is introduced to the best-performing Co₃O₄. The resulting Co₃O₄/RuO₂ heterostructure exhibits an overpotential of 257 mV at 10 mA cm^–2 and can stably catalyze the OER for 100 h.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"189 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142266119","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Crystal Facet Regulation and Ru Incorporation of Co3O4 for Acidic Oxygen Evolution Reaction Electrocatalysis","authors":"Mengting Zhao,&nbsp; and ,&nbsp;Hanfeng Liang*,&nbsp;","doi":"10.1021/acsnanoscienceau.4c0003710.1021/acsnanoscienceau.4c00037","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00037https://doi.org/10.1021/acsnanoscienceau.4c00037","url":null,"abstract":"<p >Acidic oxygen evolution reaction (OER) has long been the bottleneck of proton exchange membrane water electrolysis. Ru- and Ir-based oxides are currently state-of-the-art electrocatalysts for acidic OER, but their high cost limits their widespread application. Co₃O₄ is a promising alternative, yet the performance requires further improvement. Crystal facet engineering can effectively regulate the kinetics of surface electrochemistry and thus enhance the OER performance. However, the facet-dependent OER activity and corrosion behavior of Co₃O₄ have not been thoroughly studied. In this study, we systematically investigated the OER performance and crystal facet dependency of Co₃O₄. The results demonstrate that Co₃O₄ with mixed {111} and {110} facets exhibits better OER activity and stability than Co₃O₄ with {111} or {100} facets. The surface Co³⁺ species are responsible for the high OER activity, but its transformation to CoO₂ is also the root cause of the dissolution, leading to an activity–stability trade-off effect. The possible approach to addressing this issue would be to increase the Co³⁺ contents by nanostructure engineering. To further improve the performance, Ru is introduced to the best-performing Co₃O₄. The resulting Co₃O₄/RuO₂ heterostructure exhibits an overpotential of 257 mV at 10 mA cm^–2 and can stably catalyze the OER for 100 h.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"4 6","pages":"409–415 409–415"},"PeriodicalIF":4.8,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.4c00037","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142851207","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"DNA-Mediated Carbon Nanotubes Heterojunction Assembly","authors":"Zechariah Mengrani,&nbsp;Weiying Hong and Matteo Palma*,&nbsp;","doi":"10.1021/acsnanoscienceau.4c0002510.1021/acsnanoscienceau.4c00025","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00025https://doi.org/10.1021/acsnanoscienceau.4c00025","url":null,"abstract":"<p >Herein, we present a strategy for the controlled assembly of single-walled carbon nanotube (SWCNT) linear junctions mediated by DNA as a functional linker. We demonstrate this by employing SWCNTs of two different chiralities via the specific design of DNA sequences and chiral selection. Streptavidin and AuNP labeling of the SWCNT sidewalls demonstrate the presence of two different chirality within each individual CNT–DNA–CNT junction. These one-dimensional nanohybrids were further organized from solution to devices. The approach we developed is of general applicability for the assembly of functional nanohybrids based on carbon nanotubes toward functional applications.</p>","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"4 6","pages":"391–398 391–398"},"PeriodicalIF":4.8,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.4c00025","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142851253","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"DNA-Mediated Carbon Nanotubes Heterojunction Assembly","authors":"Zechariah Mengrani, Weiying Hong, Matteo Palma","doi":"10.1021/acsnanoscienceau.4c00025","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00025","url":null,"abstract":"Herein, we present a strategy for the controlled assembly of single-walled carbon nanotube (SWCNT) linear junctions mediated by DNA as a functional linker. We demonstrate this by employing SWCNTs of two different chiralities via the specific design of DNA sequences and chiral selection. Streptavidin and AuNP labeling of the SWCNT sidewalls demonstrate the presence of two different chirality within each individual CNT–DNA–CNT junction. These one-dimensional nanohybrids were further organized from solution to devices. The approach we developed is of general applicability for the assembly of functional nanohybrids based on carbon nanotubes toward functional applications.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"24 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142192266","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Exploring the Substitution of Fe(III) by Gd(III) in Nanomagnetite","authors":"Carolina Guida, Anthony Chappaz, Agnieszka Poulain, Jean-Marc Grenèche, Alexandre Gloter, Nicolas Menguy, Nathaniel Findling, Laurent Charlet","doi":"10.1021/acsnanoscienceau.4c00032","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00032","url":null,"abstract":"A promising superparamagnetic nanomagnetite dipped with Gd was synthesized for possible medical applications. Its size and morphology are independent of Gd content ranging from 1 to 5%. Gadolinium (III) replaced Fe(III) in the lattice. The sizes of Gd-doped nanoparticles ranged from 5 to 50 nm and exhibited a pure magnetite mineralogical phase.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"5 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142224799","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Interband and Intraband Hot Carrier-Driven Photocatalysis on Plasmonic Bimetallic Nanoparticles: A Case Study of Au–Cu Alloy Nanoparticles","authors":"Mengqi Sun, Ankai Wang, Min Zhang, Shengli Zou, Hui Wang","doi":"10.1021/acsnanoscienceau.4c00035","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00035","url":null,"abstract":"Photoexcited nonthermal electrons and holes in metallic nanoparticles, known as hot carriers, can be judiciously harnessed to drive interesting photocatalytic molecule-transforming processes on nanoparticle surfaces. Interband hot carriers are generated upon direct photoexcitation of electronic transitions between different electronic bands, whereas intraband hot carriers are derived from nonradiative decay of plasmonic electron oscillations. Due to their fundamentally distinct photogeneration mechanisms, these two types of hot carriers differ strikingly from each other in terms of energy distribution profiles, lifetimes, diffusion lengths, and relaxation dynamics, thereby exhibiting remarkably different photocatalytic behaviors. The spectral overlap between plasmon resonances and interband transitions has been identified as a key factor that modulates the interband damping of plasmon resonances, which regulates the relative populations, energy distributions, and photocatalytic efficacies of intraband and interband hot carriers in light-illuminated metallic nanoparticles. As exemplified by the Au–Cu alloy nanoparticles investigated in this work, both the resonant frequencies of plasmons and the energy threshold for the <i>d</i>-to-<i>sp</i> interband transitions can be systematically tuned in bimetallic alloy nanoparticles by varying the compositional stoichiometries and particle sizes. Choosing photocatalytic degradation of Rhodamine B as a model reaction, we elaborate on how the variation of the particle sizes and compositional stoichiometries profoundly influences the photocatalytic efficacies of interband and intraband hot carriers in Au–Cu alloy nanoparticles under different photoexcitation conditions.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"136 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142192242","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}