Showing papers by "Sara E. Skrabalak published in 2022"
TL;DR: In this paper , core@shell nanoparticles were converted to monodisperse high entropy alloy (HEA) NPs by annealing, including quinary, senary, and septenary phases comprised of PdCuPtNi with Co, Ir, Rh, Fe, and Ru.
Abstract: Colloidally prepared core@shell nanoparticles (NPs) were converted to monodisperse high entropy alloy (HEA) NPs by annealing, including quinary, senary, and septenary phases comprised of PdCuPtNi with Co, Ir, Rh, Fe, and/or Ru. Intraparticle heterogeneity, i.e., subdomains within individual NPs with different metal distributions, was observed for NPs containing Ir and Ru, with the phase stabilities of the HEAs studied by atomistic simulations. The quinary HEA NPs were found to be durable catalysts for the oxygen reduction reaction, with all but the PdCuPtNiIr NPs presenting better activities than commercial Pt. Density functional theory (DFT) calculations for PdCuPtNiCo and PdCuPtNiIr surfaces (the two extremes in performance) found agreement with experiment by weighting the adsorption energy contributions by the probabilities of each active site based on their DFT energies. This finding highlights how intraparticle heterogeneity, which we show is likely overlooked in many systems due to analytical limitations, can be leveraged toward efficient catalysis.
10 citations
TL;DR: Chiral plasmonic nanocrystals with varied symmetries were synthesized by L-glutathione-guided overgrowth from Au tetrahedra, nanoplates, and octahedra as discussed by the authors .
5 citations
TL;DR: In this paper , poly(styrene-b-polyacrylic acid) (PSPAA) is used to asymmetrically passivate cubic Au seeds through competition with hexadecyltrimethylammonium bromide (CTAB) ligands.
Abstract: Plasmonic nanoparticles (NPs) have garnered excitement over the past several decades stemming from their unique optoelectronic properties, leading to their use in various sensing applications and theranostics. Symmetry dictates the properties of many nanomaterials, and nanostructures with low, but still defined symmetries, often display markedly different properties compared to their higher symmetry counterparts. While numerous methods are available to manipulate symmetry, surface protecting groups such as polymers are finding use due to their ability to achieve regioselective modification of NP seeds, which can be removed after overgrowth as shown here. Specifically, poly(styrene-b-polyacrylic acid) (PSPAA) is used to asymmetrically passivate cubic Au seeds through competition with hexadecyltrimethylammonium bromide (CTAB) ligands. The asymmetric passivation via collapsed PSPAA causes only select vertices and faces of the Au cubes to be available for deposition of new material (i.e., Au, Au-Ag alloy, and Au-Pd alloy) during seeded overgrowth. At low metal precursor concentrations, deposition follows observations from unpassivated seeds but with new material growing from only the exposed seed portions. At high metal precursor concentrations, nanobowl-like structures form from interaction between the depositing phase and the passivating PSPAA. Through experiment and simulation, the optoelectronic properties of these nanobowls were probed, finding that the interiors and exteriors of the nanobowls can be functionalized selectively as revealed by surface enhanced Raman spectroscopy (SERS).
4 citations
TL;DR: In this paper , the authors investigated the synthesis of volatile lanthanide coordination complexes using more environmentally sustainable mechanochemical approaches and obtained a variety of coordination compounds including the expected hydrate product, the known retro-Claisen impurity, and hydrated protonated Hhfac ligand depending on the technique employed.
Abstract: Volatile lanthanide coordination complexes are critical to the generation of new optical and magnetic materials. One of the most common precursors for preparing volatile lanthanide complexes is the hydrate with the general formula Ln(hfac)3(H2O)x (x = 3 for La-Nd, x = 2 for Sm) (hfac = 1,1,1,5,5,5-hexafluoroacetylacetonato). We have investigated the synthesis of Ln(hfac)3(H2O)x using more environmentally sustainable mechanochemical approaches. Characterization of the products using Fourier transform infrared spectroscopy, nuclear magnetic resonance spectroscopy, elemental analysis, and powder X-ray diffraction shows substantial differences in product distribution between methods. The mechanochemical synthesis of the hydrate complexes leads to a variety of coordination compounds including the expected hydrate product, the known retro-Claisen impurity, and hydrated protonated Hhfac ligand depending on the technique employed. Surprisingly, 10-coordinate complexes of the form Na2Ln(hfac)5·3H2O for Ln = La-Nd were also isolated from reactions using a mortar and pestle. The electrostatic bonding of lanthanide coordination complexes is a challenge for obtaining reproducible reactions and clean products. The reproducibility issues are most acute for the large, early lanthanides whereas for the mid to late lanthanides, reproducibility in terms of product distribution and yield is less of an issue because of their smaller size and greater charge to radius ratio. Ball milling increases reproducibility in terms of generating the desired Ln(hfac)3(H2O)x along with hydrated Hhfac (tetraol) and free Hhfac products. The results illustrate the dynamic behavior of lanthanide complexes in solution and the solid state as well as the structural diversity available to the early lanthanides.
3 citations
TL;DR: The crystal structures of three β-halolactic acids have been determined, namely, β-chlorolactic acid (systematic name: 3-chloro-2-hydroxypropanoic acid, C3H5ClO3) (I), β-bromolactic acyclic acid (Systematic name): 2-hydrox-3-iodopropanoic amino acid (2-H5IO3) as discussed by the authors .
Abstract: The crystal structures of three β-halolactic acids have been determined, namely, β-chlorolactic acid (systematic name: 3-chloro-2-hydroxypropanoic acid, C3H5ClO3) (I), β-bromolactic acid (systematic name: 3-bromo-2-hydroxypropanoic acid, C3H5BrO3) (II), and β-iodolactic acid (systematic name: 2-hydroxy-3-iodopropanoic acid, C3H5IO3) (III). The number of molecules in the asymmetric unit of each crystal structure (Z') was found to be two for I and II, and one for III, making I and II isostructural and III unique. The difference between the molecules in the asymmetric units of I and II is due to the direction of the hydrogen bond of the alcohol group to a neighboring molecule. Molecular packing shows that each structure has alternating layers of intermolecular hydrogen bonding and halogen-halogen interactions. Hirshfeld surfaces and two-dimensional fingerprint plots were analyzed to further explore the intermolecular interactions of these structures. In I and II, energy minimization is achieved by lowering of the symmetry to adopt two independent molecular conformations in the asymmetric unit.
2 citations
1 citations
TL;DR: The Altmetric Attention Score as discussed by the authors is a quantitative measure of the attention that a research article has received online, which is calculated using a weighted sum of full text article downloads since November 2008 (both PDF and HTML).
Abstract: ADVERTISEMENT RETURN TO ISSUEEditorialNEXTHighlighting Recent Research from Latin America in Chemistry of MaterialsCarlos Toro*Carlos ToroMore by Carlos Toro and Sara E. Skrabalak*Sara E. SkrabalakMore by Sara E. SkrabalakCite this: Chem. Mater. 2022, 34, 23, 10209–10210Publication Date (Web):November 28, 2022Publication History Received7 November 2022Published online28 November 2022Published inissue 13 December 2022https://doi.org/10.1021/acs.chemmater.2c03349Copyright © Published 2022 by American Chemical SocietyRIGHTS & PERMISSIONSArticle Views879Altmetric-Citations1LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated. Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InReddit PDF (868 KB) Get e-AlertsSUBJECTS:Adsorption,Biomaterials,Inorganic compounds,Materials,Metal organic frameworks Get e-Alerts
1 citations
TL;DR: In this article , the authors demonstrate the complete sonoelectrochemical synthesis of monodisperse metal NPs starting from bulk metal, using Cu as a model system, using ultrasound coupled with electrosynthesis to clean the electrode surface, dispersing the NPs produced at the electrode into solution.
Abstract: Traditional colloidal syntheses of metal nanoparticles (NPs) are highly sensitive to the selection of and quality of chemical reducing agents and metal precursors. To address these challenges, we demonstrate the complete sonoelectrochemical synthesis of monodisperse metal NPs starting from bulk metal, using Cu as a model system. Electrochemical syntheses of NPs are of great interest as the oxidation and reduction processes that account for product formation can occur directly at the anode and cathode, respectively. This ability has the potential to improve reproducibility by simplifying the chemical pathway to NPs, with electrosyntheses often also providing unique kinetic pathways toward green product formation. Herein, ultrasound is coupled with electrosynthesis to clean the electrode surface, dispersing the NPs produced at the electrode into solution. We were able to shift the size distribution to form monodispersed metal NPs through control of applied potential (Vapplied) and ultrasonic pulses. The synthesis begins with electrooxidation of bulk Cu metal to directly dissolve metal ions into a microemulsion system. This step is followed by sonoelectroreduction of the ions, which facilitates the formation of dispersible, monodisperse Cu NPs with diameters <10 nm. The size distribution can be controlled by adjusting the Vapplied, pulse intensity, and pulse sequence implemented during sonoelectroreduction. We view this technique as a scalable method to synthesize metal NPs from bulk metal without chemical reducing agents.
TL;DR: In this article , local structures of synthesized, durable and high-activity Bi4TaO8Cl and Bi2GdO4Cl intergrowth photocatalysts are investigated by pair distribution function, structure mining and strain analysis and correlated to their optoelectronic properties.
Abstract: Local structures of synthesized, durable and high-activity Bi4TaO8Cl–Bi2GdO4Cl intergrowth photocatalysts are investigated by pair distribution function, structure mining and strain analysis and correlated to their optoelectronic properties.
TL;DR: The Altmetric Attention Score as discussed by the authors is a quantitative measure of the attention that a research article has received online, and it is calculated using a weighted sum of full text article downloads since November 2008.
Abstract: ADVERTISEMENT RETURN TO ISSUEEditorialNEXTUnraveling the Complex Structure of Graphite Oxide: An Interview with Tamás Szabó for Chemistry of Materials’ 1k ClubCarlos ToroCarlos ToroMore by Carlos Torohttps://orcid.org/0000-0002-8359-462X and Sara E. SkrabalakSara E. SkrabalakMore by Sara E. Skrabalakhttps://orcid.org/0000-0002-1873-100XCite this: Chem. Mater. 2022, 34, 19, 8469–8470Publication Date (Web):October 11, 2022Publication History Received15 September 2022Published online11 October 2022Published inissue 11 October 2022https://doi.org/10.1021/acs.chemmater.2c02840Copyright © Published 2022 by American Chemical SocietyRIGHTS & PERMISSIONSArticle Views294Altmetric-Citations-LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated. Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InReddit PDF (3 MB) Get e-AlertsSUBJECTS:Chemical structure,Electron paramagnetic resonance spectroscopy,Materials,Oxides,Two dimensional materials Get e-Alerts
TL;DR: The Altmetric Attention Score as discussed by the authors is a quantitative measure of the attention that a research article has received online, and it is calculated using a weighted sum of full text article downloads since November 2008 across all institutions and individuals.
Abstract: ADVERTISEMENT RETURN TO ISSUEEditorialNEXTRevisiting the Early Literature on Nanocomposites and the Path to Transformative Technologies: An Interview with Rupali Gangopadhyay for Chemistry of Materials’ 1k ClubCarlos ToroCarlos ToroMore by Carlos Torohttps://orcid.org/0000-0002-8359-462X and Sara E. SkrabalakSara E. SkrabalakMore by Sara E. Skrabalakhttps://orcid.org/0000-0002-1873-100XCite this: Chem. Mater. 2022, 34, 21, 9305–9306Publication Date (Web):November 8, 2022Publication History Received25 September 2022Published online8 November 2022Published inissue 8 November 2022https://doi.org/10.1021/acs.chemmater.2c02936Copyright © Published 2022 by American Chemical SocietyRIGHTS & PERMISSIONSArticle Views403Altmetric-Citations-LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated. Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InReddit PDF (3 MB) Get e-AlertsSUBJECTS:Materials,Nanocomposites,Nanoparticles,Plastics,Polymers Get e-Alerts
TL;DR: Toro et al. as discussed by the authors proposed the Altmetric Attention Score, a quantitative measure of the attention that a research article has received online, which is calculated using a weighted sum of full text article downloads since November 2008 (both PDF and HTML).
Abstract: ADVERTISEMENT RETURN TO ISSUEEditorialNEXTRinging in the New Year with Gratitude and Editorial Team UpdatesCarlos Toro*Carlos ToroMore by Carlos Torohttps://orcid.org/0000-0002-8359-462X and Sara E. Skrabalak*Sara E. SkrabalakMore by Sara E. Skrabalakhttps://orcid.org/0000-0002-1873-100XCite this: Chem. Mater. 2022, 34, 1, 1–4Publication Date (Web):January 11, 2022Publication History Published online11 January 2022Published inissue 11 January 2022https://doi.org/10.1021/acs.chemmater.1c04326Copyright © Published 2022 by American Chemical SocietyRIGHTS & PERMISSIONSArticle Views905Altmetric-Citations-LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated. Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InReddit PDF (562 KB) Get e-AlertsSUBJECTS:Covalent organic frameworks,Interfaces,Material properties,Materials,Metal organic frameworks Get e-Alerts