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| Open AccessNanoscale silicate melt textures determine volcanic ash surface chemistry
Nanotexture-sensitive fracture focusing during magma fragmentation determines the surface chemistry of volcanic ash particles, thereby modifying the reactive interface and subsequent environmental impacts
- Adrian J. Hornby
- , Paul M. Ayris
- & Donald B. Dingwell
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| Open AccessElucidating the active phases of CoOx films on Au(111) in the CO oxidation reaction
Supported CoOx catalysts display higher reactivities towards CO oxidation, yet, corresponding catalytically active phases are still unclear, especially under reaction conditions. Here, by means of in-situ APXPS and ResPES, the authors demonstrate that the topographic restructuring and chemical restructuring occur on these CoOx working catalysts, and also highlight the unique catalytic properties of Co3+ sites.
- Hao Chen
- , Lorenz J. Falling
- & Miquel Salmeron
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| Open AccessComparative study of Co3O4(111), CoFe2O4(111), and Fe3O4(111) thin film electrocatalysts for the oxygen evolution reaction
Cobalt-based oxidic anodes with added iron are good electrocatalysts for alkaline oxygen evolution reaction, but the role of iron is still unclear. Here the authors investigate oxygen evolution reaction activity of three well-defined epitaxial thin-film electrodes to address this issue.
- Earl Matthew Davis
- , Arno Bergmann
- & Beatriz Roldan Cuenya
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Article
| Open AccessReal-space imaging of a phenyl group migration reaction on metal surfaces
On-surface synthesis allows fabrication of nanostructures with atomic precision and may follow different routes compared to in-solution chemistry. Here the authors, using scanning probe microscopy techniques, observe a phenyl group migration reaction on three different metal surfaces forming polycyclic aromatic hydrocarbons, which cannot be accessed by in-solution chemistry.
- Zilin Ruan
- , Baijin Li
- & Jinming Cai
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Article
| Open AccessWeak CO binding sites induced by Cu–Ag interfaces promote CO electroreduction to multi-carbon liquid products
Here, the authors demonstrate a Cu-based catalyst with Cu–Ag interfacial sites, which favor oxygenate over alcohol production in CO2 electroreduction. Near 80% selectivity for multi-carbon liquid products in a 100 cm2 membrane electrode assembly electrolyzer is exhibited over 100 h.
- Jing Li
- , Haocheng Xiong
- & Qi Lu
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Article
| Open AccessNew insights in polydopamine formation via surface adsorption
Polydopamine is a biomimetic self-adherent polymer, which can be easily deposited on a wide variety of materials but the polymerization mechanism and the key intermediate species formed during the deposition process are still controversial. Here, the authors report a systematic investigation of polydopamine formation on halloysite nanotubes.
- Hamoon Hemmatpour
- , Oreste De Luca
- & Petra Rudolf
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Article
| Open AccessStructure sensitivity in gas sorption and conversion on metal-organic frameworks
Probing gas sorption on defects and facets of porous materials at the nanoscale is challenging. Here, we visualize nano-domains of preferred formaldehyde sorption on (defective) ZIF-8 microcrystals using in situ Photo-induced Force Microscopy (PiFM).
- Guusje Delen
- , Matteo Monai
- & Bert M. Weckhuysen
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| Open AccessDirect observation of long-range chirality transfer in a self-assembled supramolecular monolayer at interface in situ
Unravelling the mechanism of chirality transfer in supramolecular assemblies is important to understand the relationship between molecular chirality and supramolecular chirality. Here, the authors use nonlinear spectroscopy and molecular dynamic simulations to study the long-range chirality transfer in a self-assembled supramolecular system.
- Yuening Zhang
- , Xujin Qin
- & Zhen Zhang
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Article
| Open AccessEffect of current density on the solid electrolyte interphase formation at the lithium∣Li6PS5Cl interface
The interface between the Li metal electrode and inorganic solid electrolyte is crucial for developing reliable all-solid-state Li batteries. Here, the authors show that the Li plating current density distinctly affects the chemistry and morphology of interphase components formed at the interface.
- Sudarshan Narayanan
- , Ulderico Ulissi
- & Mauro Pasta
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| Open AccessRevealing solid electrolyte interphase formation through interface-sensitive Operando X-ray absorption spectroscopy
Solid electrolyte interphase (SEI) formation on Li-ion battery anodes is critical for long-term performance. Here, the authors use operando soft X-ray absorption spectroscopy in total electron yield mode to resolve the chemical evolution of the SEI during electrochemical formation on silicon anodes.
- Jack E. N. Swallow
- , Michael W. Fraser
- & Robert S. Weatherup
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Article
| Open AccessThe Donnan potential revealed
Donnan electrical potential is widely adopted to describe ion distribution between two solutions separated by a permeable membrane with implications for many chemical and biological systems. Aydogan Gokturk et al. directly measures this potential for the first time and compare the data with theoretical models.
- Pinar Aydogan Gokturk
- , Rahul Sujanani
- & Ethan J. Crumlin
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Article
| Open AccessMagnetic molecules as local sensors of topological hysteresis of superconductors
Magnetic molecules have long been seen to hold promise in magnetic sensing applications. In this paper, Serrano et al show that a single layer of a magnetic molecule, a terbium based complex, is sensitive to the local magnetic field variation of a superconducting surface on which it is deposited.
- Giulia Serrano
- , Lorenzo Poggini
- & Roberta Sessoli
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Article
| Open AccessUnderstanding the complementarities of surface-enhanced infrared and Raman spectroscopies in CO adsorption and electrochemical reduction
Infrared and Raman spectroscopies are often assumed to provide similar insights into heterogeneous reaction mechanisms. This study shows that these techniques provide similar data when CO is strongly bound to a surface, yet distinct subpopulations of CO are probed when binding is weaker.
- Xiaoxia Chang
- , Sudarshan Vijay
- & Bingjun Xu
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| Open AccessIdentification of CO2 adsorption sites on MgO nanosheets by solid-state nuclear magnetic resonance spectroscopy
The characterization of the surface structure and binding sites of materials is crucial for designing advanced materials for adsorption processes. Here, the authors use 17O solid-state nuclear magnetic resonance spectroscopy to identify specific CO2 adsorption sites on MgO nanosheets.
- Jia-Huan Du
- , Lu Chen
- & Luming Peng
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Article
| Open AccessResolving sub-angstrom ambient motion through reconstruction from vibrational spectra
Tracking single molecule movements is a challenging task, but highly desired for applications and fundamental studies. Here the authors reconstruct the sub-angstrom relative movements of a molecule interacting with a metal adatom, by measuring its vibrational spectrum in a self-assembled monolayer, continuously modified by the adatom in a nanoparticle-on-mirror construct.
- Jack Griffiths
- , Tamás Földes
- & Jeremy J. Baumberg
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Article
| Open AccessCoexisting multi-states in catalytic hydrogen oxidation on rhodium
Catalytic reactions may exhibit oscillations in the reaction rate even at constant external parameters. Here, the authors observe and explain the coexistence of such oscillations and the steady states of catalytic activity in H2 oxidation on differently structured grains of a polycrystalline Rh foil.
- P. Winkler
- , J. Zeininger
- & G. Rupprechter
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Article
| Open AccessLiquid flow reversibly creates a macroscopic surface charge gradient
Reactions at the interface between mineral surfaces and flowing liquids are ubiquitous in nature. Here the authors explore, using surface-specific sum frequency generation spectroscopy and numeric calculations, how the liquid flow affects the charging and dissolution rates leading to flow-dependent charge gradients along the surface.
- Patrick Ober
- , Willem Q. Boon
- & Mischa Bonn
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Article
| Open AccessBulk tungsten-substituted vanadium oxide for low-temperature NOx removal in the presence of water
NH3 selective catalytic reduction is an important technique for NOx removal but water vapor critically inhibits the reaction at a low temperature. Here the authors show bulk W-substituted VOx exhibits higher NOx removal ability than the TiO2 supported vanadia catalyst in the presence of water.
- Yusuke Inomata
- , Hiroe Kubota
- & Toru Murayama
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| Open AccessProbing consequences of anion-dictated electrochemistry on the electrode/monolayer/electrolyte interfacial properties
Conveying electrochemistry in terms of the electrode/electrolyte interfacial properties remains challenging. Here, the authors employ a surface-bound molecular probe and photoelectron spectroscopy to peer into the anion-dictated and potential-induced interfacial electronic and structural properties.
- Raymond A. Wong
- , Yasuyuki Yokota
- & Yousoo Kim
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| Open AccessExamining the surface evolution of LaTiOxNy an oxynitride solar water splitting photocatalyst
While solar-driven water splitting may afford a renewable means to harvest energy, it is essential to understand how photocatalysts transform during catalysis. Here, authors study LaTiOxNy films by surface-sensitive techniques before and after photoelectrochemical water splitting.
- Craig Lawley
- , Maarten Nachtegaal
- & Thomas Lippert
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| Open AccessResolving the puzzle of single-atom silver dispersion on nanosized γ-Al2O3 surface for high catalytic performance
Detailed atom-level anchoring mechanism of Ag species on γ-Al2O3 is largely unknown for the widely used Ag/γ-Al2O3 catalyst. Here, the authors demonstrate that single-Ag atom can be only anchored by the terminal hydroxyls on the (100) surfaces of γ-Al2O3 through consuming two or three terminal hydroxyls.
- Fei Wang
- , Jinzhu Ma
- & Xiao Cheng Zeng
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| Open AccessNanoscopic diffusion of water on a topological insulator
Water molecular motion on surfaces underpins a range of phenomena in nature. The authors resolve the nanoscale-nanosecond motion of water at a topological insulator’s surface by helium spin-echo spectroscopy and computations, reporting hopping among sites and repulsion between water molecules.
- Anton Tamtögl
- , Marco Sacchi
- & William Allison
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Article
| Open AccessReactivity mapping of nanoscale defect chemistry under electrochemical reaction conditions
Identifying reacting species locally with nanometer precision is a major challenge in electrochemical surface science. Using operando Raman nanoscopy, authors image the reversible, concurrent formation of nanometer-spatially separated Au2O3 and Au2O species during Au nanodefect oxidation.
- Jonas H. K. Pfisterer
- , Masoud Baghernejad
- & Katrin F. Domke
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Article
| Open AccessSolar energy storage at an atomically defined organic-oxide hybrid interface
Molecular photoswitches provide an extremely simple solution for solar energy conversion and storage. Here, the authors report on the assembly of an operational solar energy-storing organic-oxide hybrid interface, which consists of a tailor-made molecular photoswitch and an atomically-defined semiconducting oxide film.
- Christian Schuschke
- , Chantal Hohner
- & Jörg Libuda
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Article
| Open AccessDramatic differences in carbon dioxide adsorption and initial steps of reduction between silver and copper
The recycling of CO2 into storable chemicals is critical in order to mitigate climate change, although CO2’s inert nature has limited the reduction’s mechanistic considerations. Here, authors pair in-situ spectroscopy with quantum mechanics to elucidate CO2 adsorption on copper and silver surfaces.
- Yifan Ye
- , Hao Yang
- & Ethan J. Crumlin
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Article
| Open AccessUltrafast energy relaxation dynamics of amide I vibrations coupled with protein-bound water molecules
Vibrational energy relaxation of proteins helps us to understand ultrafast protein dynamics. Here, the authors determine the vibrational energy transfer time of the amide I mode in aqueous environment and find that water provides a “shortcut” through a direct resonant channel to dissipate energy into the solvent.
- Junjun Tan
- , Jiahui Zhang
- & Shuji Ye
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Article
| Open AccessUnravelling the effect of charge dynamics at the plasmonic metal/semiconductor interface for CO2 photoreduction
Light-driven CO2 reduction provides a way to limit greenhouse gas concentrations, but understanding how materials accomplish this transformation is challenging. Here, authors examine the reaction over plasmonic silver-titanium dioxide using time-resolved, in situ techniques to follow the mechanism.
- Laura Collado
- , Anna Reynal
- & Víctor A. de la Peña O’Shea
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| Open AccessEvidence for auto-catalytic mineral dissolution from surface-specific vibrational spectroscopy
Although it is well known that silica can dissolve in water, the precise mechanism is unclear. Here, the authors employ sum frequency generation spectroscopy to probe the interfacial water structure reporting directly on the underlying dissolution mechanism, which appears to be auto-catalytic.
- Jan Schaefer
- , Ellen H. G. Backus
- & Mischa Bonn
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| Open AccessBoosting hot electron flux and catalytic activity at metal–oxide interfaces of PtCo bimetallic nanoparticles
The real-time quantitative detection of hot electrons provides critical clues to understand the origin of the enhanced catalytic performance of bimetallic nanoparticles (NPs). Here, the authors investigate hot electrons generated on bimetallic PtCo NPs during H2 oxidation by measuring the chemicurrent on a catalytic nanodiode.
- Hyosun Lee
- , Juhyung Lim
- & Jeong Young Park
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Article
| Open AccessOn-surface synthesis of a nitrogen-embedded buckybowl with inverse Stone–Thrower–Wales topology
Heteroatom doping of buckybowls is a viable route to tune their intrinsic physico-chemical properties, but their synthesis remains challenging. Here, the authors report on a combined in-solution and on-surface synthetic strategy towards the fabrication of a buckybowl containing two fused nitrogen-doped pentagonal rings.
- Shantanu Mishra
- , Maciej Krzeszewski
- & Daniel T. Gryko
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Article
| Open AccessSelf-cleaning and surface chemical reactions during hafnium dioxide atomic layer deposition on indium arsenide
Atomic layer deposition of high-quality thin oxide layers is crucial for many modern semiconductor electronic devices. Here, the authors explore the surface chemistry during the initial deposition and observe a previously unknown two-step process, with promise for an improved self-cleaning effect.
- Rainer Timm
- , Ashley R. Head
- & Anders Mikkelsen
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Article
| Open AccessExperimentally quantifying anion polarizability at the air/water interface
Understanding anion-specific interactions with hydrophobic interfaces is challenging due to an absence of local structural probes. Here, the authors experimentally quantify the anisotropy of perchlorate’s polarizability at the air/water interface, a window into anion and solvation shell structure.
- Yujin Tong
- , Igor Ying Zhang
- & R. Kramer Campen
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Article
| Open AccessMössbauer spectroscopy of a monolayer of single molecule magnets
Deposition of single molecule magnets onto surfaces is a key step for integration in devices exploiting their magnetic bistability and quantum properties. Here, Sessoli and colleagues exploit synchrotron Mössbauer spectroscopy to assess the effects of molecule-surface interactions on the magnetic properties of Fe(III) SMMs.
- Alberto Cini
- , Matteo Mannini
- & Roberta Sessoli
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| Open AccessScaling relationships and theory for vibrational frequencies of adsorbates on transition metal surfaces
Vibrational excitations are a fingerprint of molecule–surface interactions, but knowing how they scale across materials is tricky. Here, the authors discover correlations between the vibrational frequencies of adsorbates on transition metals, developing a predictive theory to allow interpretation of complex experimental spectra.
- Joshua L. Lansford
- , Alexander V. Mironenko
- & Dionisios G. Vlachos
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| Open AccessSecond-order spectral lineshapes from charged interfaces
Charged interfaces are important in chemical systems, but the influence of charge on vibrational sum frequency spectra has only recently been considered. Here the authors show the importance of accounting for the interfacial potential-dependent χ(3) term in interpreting spectral lineshapes from charged interfaces.
- Paul E. Ohno
- , Hong-fei Wang
- & Franz M. Geiger
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| Open AccessMapping surface-modified titania nanoparticles with implications for activity and facet control
Metal oxide nanocrystals can be grown with different facets exposed to give variations in reactivity, but the chemical state of these surfaces is not clear. Here, the authors make use of a phosphine probe molecule allowing the differences in surface chemistry to be mapped by NMR spectroscopy.
- Yung-Kang Peng
- , Yichen Hu
- & Shik Chi Edman Tsang
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| Open AccessControlling selectivities in CO2 reduction through mechanistic understanding
Understanding the mechanism of CO2 reduction on a catalyst surface is essential for achieving the desired product selectivity. Here, the authors show an operando kinetic analysis of CO2 hydrogenation over a palladium catalyst in order to address the factors governing the selectivity of the process.
- Xiang Wang
- , Hui Shi
- & János Szanyi
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Article
| Open AccessThe most active Cu facet for low-temperature water gas shift reaction
Nanocrystals display a variety of facets with different catalytic activity. Here the authors identify the most active facet of copper nanocrystals relevant to the low-temperature water gas shift reaction and further design zinc oxide-copper nanocubes with exceptionally high catalytic activity.
- Zhenhua Zhang
- , Sha-Sha Wang
- & Weixin Huang
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Article
| Open AccessMulti-orbital charge transfer at highly oriented organic/metal interfaces
Charge transfer at molecule-metal interfaces affects the overall physical and magnetic properties of organic-based devices, and ultimately their performance. Here, the authors report evidence of a pronounced charge transfer involving nickel tetraphenyl porphyrin molecules adsorbed on copper.
- Giovanni Zamborlini
- , Daniel Lüftner
- & Claus Michael Schneider
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Article
| Open AccessA reversible dendrite-free high-areal-capacity lithium metal electrode
Despite recent technological advances, it remains challenging to realize reversible high-areal-capacity lithium metal anodes. Here, the authors demonstrate such an anode by tailoring the top solid electrolyte interphase layer.
- Hui Wang
- , Masaki Matsui
- & Nobuyuki Imanishi
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Article
| Open AccessInterfacial Ca2+ environments in nanocrystalline apatites revealed by dynamic nuclear polarization enhanced 43Ca NMR spectroscopy
Solid-state NMR can in principle be used to study calcium environments in biomaterials such as bones/teeth, but43Ca lacks receptivity. Here the authors present an approach to acquire 43Ca data for hydroxyapatite at its natural isotopic abundance, distinguishing between core and surface Ca sites.
- Daniel Lee
- , César Leroy
- & Gaël De Paëpe
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Article
| Open AccessPhase-referenced nonlinear spectroscopy of the α-quartz/water interface
Probing the polarization of water molecules at charged interfaces reveals insights into surface behaviour, but current methods are limited to isotropic materials. Here the authors exploit the nonlinear optical properties of the α-quartz/water interface to expand the scope of such methods to non-isotropic materials.
- Paul E. Ohno
- , Sarah A. Saslow
- & Kenneth B. Eisenthal
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Article
| Open AccessUnravelling the electrochemical double layer by direct probing of the solid/liquid interface
The electrochemical double layer is a key concept in chemistry, but its properties are hard to probe experimentally. Here, the authors use ambient pressure X-ray photoelectron spectroscopy to probe the electrochemical double layer potential profile at the solid/liquid interface, under polarization conditions.
- Marco Favaro
- , Beomgyun Jeong
- & Ethan J. Crumlin
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Article
| Open AccessX-ray photoemission analysis of clean and carbon monoxide-chemisorbed platinum(111) stepped surfaces using a curved crystal
Systematic variation of surface sites may allow for more efficient testing of surface chemical reactions. Here, the authors use a platinum curved crystal and, by carrying out photoemission scans, are able to systematically address the fundamental CO-chemisorption process on a ‘tunable’ vicinal surface.
- Andrew L. Walter
- , Frederik Schiller
- & J. Enrique Ortega
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Article |
Observation of strong electron pairing on bands without Fermi surfaces in LiFe1−xCoxAs
It remains to be seen if high-Tc superconductors rely on similar Fermi-surface instabilities as their BCS counterparts. Miao et al. study the high-Tc compound LiFe1−xCoxAs with high-resolution ARPES and find a robust gap with Co doping that suggests the order parameter is not tied to such instabilities.
- H. Miao
- , T. Qian
- & H. Ding