Multi-modal surface analysis of porous films under <i>operando</i> conditions

Eads, Calley N.; Zhong, Jiuping; Kim, Donghun; Akter, Nusnin; Chen, Zhihengyu; Norton, Angela M.; Lee, Veronica; Kelber, Jeffry A.; Tsapatsis, Michael; Boscoboinik, J. Anibal; Sadowski, Jerzy; Zahl, Percy; Tong, Xiao; Stacchiola, Darı́o; Head, Ashley R.; Tenney, Samuel A.

doi:10.1063/5.0006220

Cited by 25 publications

(34 citation statements)

References 68 publications

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“…The rigid shift is likely a consequence of new dipole interactions in the presence of CO adsorbates at the Pd surface. Our previous study showed an analogous shift of Si 2p when investigating the CO adsorption on Pd(111) under 2D silica [47] . Additionally, a report by Yao et al [19] .…”

Section: Resultssupporting

confidence: 53%

Enhanced Catalysis under 2D Silica: A CO Oxidation Study

et al. 2021

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Interfacially confined microenvironments have recently gained attention in catalysis, as they can be used to modulate reaction chemistry. The emergence of a 2D nanospace at the interface between a 2D material and its support can promote varying kinetic and energetic schemes based on molecular level confinement effects imposed in this reduced volume. We report on the use of a 2D oxide cover, bilayer silica, on catalytically active Pd(111) undergoing the CO oxidation reaction. We “uncover” mechanistic insights about the structure–activity relationship with and without a 2D silica overlayer using in situ IR and X‐ray spectroscopy and mass spectrometry methods. We find that the CO oxidation reaction on Pd(111) benefits from confinement effects imposed on surface adsorbates under 2D silica. This interaction results in a lower and more dispersed coverage of CO adsorbates with restricted CO adsorption geometries, which promote oxygen adsorption and lay the foundation for the formation of a reactive surface oxide that produces higher CO2 formation rates than Pd alone.

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Section: Resultssupporting

confidence: 53%

Enhanced Catalysis under 2D Silica: A CO Oxidation Study

et al. 2021

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“…The system was equipped with a VERTEX 80v FTIR spectrometer with an external MCT detector, and the entire IR beam path was in vacuum. Details of this instrument have been described previously . The instrument was equipped with a polarizer that allowed recording a background with s -polarized light (parallel to the surface plane), while p -polarized light (normal to the surface plane) was used to record the sample spectra.…”

Section: Methodsmentioning

confidence: 99%

“…Details of this instrument have been described previously. 33 The instrument was equipped with a polarizer that allowed recording a background with s-polarized light (parallel to the surface plane), while p-polarized light (normal to the surface plane) was used to record the sample spectra. A Pt(111) single crystal (hat-shaped, 2 mm thick, with a top diameter of 8 mm, from Princeton Scientific Corporation) was initially cleaned by Ar + sputtering and annealing cycles.…”

Section: Methodsmentioning

confidence: 99%

Experimental and Theoretical Insights into the Active Sites on WO_x/Pt(111) Surfaces for Dehydrogenation and Dehydration Reactions

et al. 2021

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The catalytic upgrading of biomass is an important step toward realizing renewable chemical production. Pt/WO x and the inverse catalyst, WO x /Pt, have been shown to be highly active and selective for the C−O bond scission of various biomassderived oxygenates. Yet, the nature of the active sites and detailed reaction mechanisms have not been well understood. In this study, carbon monoxide and isopropyl alcohol (IPA) have been used as probe molecules to study the active sites of WO x /Pt(111) model surfaces. Temperature-programmed desorption experiments identified two distinct active sites responsible for different reaction pathways: dehydrogenation over Pt sites and dehydration over WO x sites. High-resolution electron energy loss spectroscopy (HREELS) identified the surface reaction intermediates. In situ infrared reflection absorption spectroscopy and HREELS measurements confirmed the presence of hydroxyl groups on WO x , which were consumed upon the adsorption of IPA, suggesting that the hydroxyl groups were the active sites for IPA dehydration. Density functional theory (DFT) calculations further revealed the reaction mechanisms and activation barriers of the IPA dehydrogenation and dehydration reactions. The comparison of different in situ-generated hydroxyl groups on WO x by DFT calculations suggested that the most active sites for dehydration should be those with protons least strongly bound (site formation energy of −0.3 eV), with a dehydration activation barrier of 1.23 eV. The understanding from this study provides insights into the design of relevant metal/metal oxide catalysts for the upgrading of biomassderived oxygenates.

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“…XPS experiments were performed at the Center for Functional Nanomaterials at Brookhaven National Laboratory. Both sample preparation and XPS measurements were performed in a lab-based ambient pressure photoelectron spectrometer 32 by SPECS Surface Nano Analysis GmbH, with PHOIBOS 150 NAP hemispherical analyzer. The system has a sample preparation chamber and an analysis chamber separated by a gate valve; the base pressure in the analysis chamber is <10 −9 mbar.…”

Section: ■ Experimental Methodsmentioning

confidence: 99%

Reusing Face Covering Masks: Probing the Impact of Heat Treatment

Yan

Stackhouse

Waluyo

et al. 2021

ACS Sustainable Chem. Eng.

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The COVID-19 pandemic resulted in imminent shortages of personal protective equipment such as face masks. To address the shortage, new sterilization or decontamination procedures for masks are quickly being developed and employed. Dry heat and steam sterilization processes are easily scalable and allow treatment of large sample sizes, thus potentially presenting fast and efficient decontamination routes, which could significantly ease the rapidly increasing need for protective masks globally during a pandemic like COVID-19. In this study, a suite of structural and chemical characterization techniques, including scanning electron microscopy (SEM), contact angle, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Raman were utilized to probe the heat treatment impact on commercially available 3M 8210 N95 Particulate Respirator and VWR Advanced Protection surgical mask. Unique to this study is the use of the synchrotron-based In situ and Operando Soft X-ray Spectroscopy (IOS) beamline (23-ID-2) housed at the National Synchrotron Light Source II at Brookhaven National Laboratory for near-edge X-ray absorption spectroscopy (NEXAFS).

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Multi-modal surface analysis of porous films under operando conditions

Cited by 25 publications

References 68 publications

Enhanced Catalysis under 2D Silica: A CO Oxidation Study

Enhanced Catalysis under 2D Silica: A CO Oxidation Study

Experimental and Theoretical Insights into the Active Sites on WO_x/Pt(111) Surfaces for Dehydrogenation and Dehydration Reactions

Reusing Face Covering Masks: Probing the Impact of Heat Treatment

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Multi-modal surface analysis of porous films under operando conditions

Cited by 25 publications

References 68 publications

Enhanced Catalysis under 2D Silica: A CO Oxidation Study

Enhanced Catalysis under 2D Silica: A CO Oxidation Study

Experimental and Theoretical Insights into the Active Sites on WOx/Pt(111) Surfaces for Dehydrogenation and Dehydration Reactions

Reusing Face Covering Masks: Probing the Impact of Heat Treatment

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Product

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Experimental and Theoretical Insights into the Active Sites on WO_x/Pt(111) Surfaces for Dehydrogenation and Dehydration Reactions