Experimental and theoretical evidence of charge transfer in multi-component alloys – how chemical interactions reduce atomic size mismatch

Casillas-Trujillo, Luis; Osinger, Barbara; Lindblad, Rebecka; Karlsson, Dennis; Abrikosov, Alexei I.; Fritze, Stefan; Fieandt, Kristina von; Alling, Björn; Hotz, Ingrid; Jansson, Ulf; Abrikosov, Igor A.; Lewin, Erik

doi:10.1039/d1qm00380a

Cited by 25 publications

(12 citation statements)

References 43 publications

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“…The upshift of Co 2p and downshift of P 2p peaks compared to elemental Co (778.1 eV) and elemental P (130.2 eV) indicate that Co carries partial positive charge (Co δ+ ) and P carries partial negative charge (P δ− ) . The careful examination of the XPS profile of CoP@NC-Ru shows 0.4 eV positive shift in the B.E corresponding to Co 2p (778.8) compared to CoP@NC in accordance with the prediction of electronegativity. , This was further confirmed from the Ru 3p XPS profile (Figure c) of CoP@NC-Ru and RuNC ( vide infra ). The high-resolution Ru 3p profile corresponding to the Ru 0 shifted to lower B.E compared to that of RuNC.…”

Section: Resultssupporting

confidence: 70%

“…33 The careful examination of the XPS profile of CoP@NC-Ru shows 0.4 eV positive shift in the B.E corresponding to Co 2p (778.8) compared to CoP@NC in accordance with the prediction of electronegativity. 19,34 This was further confirmed from the Ru 3p XPS profile (Figure 1c) of CoP@NC-Ru and RuNC (vide inf ra). The high-resolution Ru 3p profile corresponding to the Ru 0 shifted to lower B.E compared to that of RuNC.…”

Section: Resultssupporting

confidence: 60%

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Surface Tailoring-Modulated Bifunctional Oxygen Electrocatalysis with CoP for Rechargeable Zn–Air Battery and Water Splitting

Kumar,

Aparna,

Nayak

et al. 2024

ACS Appl. Mater. Interfaces

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The transition metal phosphide (TMP)-based functional electrocatalysts are very promising for the development of electrochemical energy conversion and storage devices including rechargeable metal−air batteries and water electrolyzer. Tuning the electrocatalytic activity of TMPs is one of the vital steps to achieve the desired performance of these energy devices. Herein, we demonstrate the modulation of the bifunctional oxygen electrocatalytic activity of nitrogen-doped carbon-encapsulated CoP (CoP@NC) nanostructures by surface tailoring with ultralow amount (0.56 atomic %) of Ru nanoparticles (2.5 nm). The CoP at the core and the Ru nanoparticles on the shell have a facile charge transfer interaction with the encapsulating NC. The strong coupling of Ru with CoP@NC boosts the electrocatalytic performance toward oxygen reduction (ORR), oxygen evolution (OER), and hydrogen evolution (HER) reactions. The surface-tailored catalyst requires only 35 mV to deliver the benchmark current density of 10 mA•cm −2 for HER. A small potential gap of 620 mV between ORR and OER is achieved, making the catalyst highly suitable for the development of rechargeable zinc−air batteries (ZABs). The homemade ZAB delivers a specific capacity of 780 mA•hg Zn −1 and peak power density of 175 mW•cm −2 with a very small voltaic efficiency loss (1.1%) after 300 cycles. The two-electrode water splitting cell

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Section: Resultssupporting

confidence: 70%

Section: Resultssupporting

confidence: 60%

Surface Tailoring-Modulated Bifunctional Oxygen Electrocatalysis with CoP for Rechargeable Zn–Air Battery and Water Splitting

Kumar,

Aparna,

Nayak

et al. 2024

ACS Appl. Mater. Interfaces

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“…Some of the metal core level spectra in the multicomponent carbide, not shown here, exhibit a shift to lower binding energies compared with reference values for the binary carbides. This has been shown theoretically and experimentally in corresponding metal alloy and nitride films [56,57] and will be further investigated in future studies. For the film with 10 at.% especially broad metal core level spectra were observed (not shown), which is consistent with the metal-carbide composite structure already observed in XRD.…”

Section: Characterisation Of Magnetron Sputtered Multicomponent Filmsmentioning

confidence: 57%

Investigation of the phase formation in magnetron sputtered hard multicomponent (HfNbTiVZr)C coatings

et al. 2022

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“…This shift could be associated with changes in the unfilled electronic holes of the D band, resulting from the charge transfer from Cu to the adjacent Ni [ 53 ]. On the other hand, the main peak shifted up by 0.2 eV for the Sn/NiCeZr catalyst, which was likely due to the higher electronegativity of Sn (1.96) compared to that of nickel (1.91) [ 54 ].…”

Section: Resultsmentioning

confidence: 99%

Hydrogenolysis of Glycerol over NiCeZr Catalyst Modified with Mg, Cu, and Sn at the Surface Level

Vera-Hincapie,

Iriarte-Velasco,

Ayastuy

et al. 2024

IJMS

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Biomass valorization is an essential strategy for converting organic resources into valuable energy and chemicals, contributing to the circular economy, and reducing carbon footprints. Glycerol, a byproduct of biodiesel production, can be used as a feedstock for a variety of high-value products and can contribute to reducing the carbon footprint. This study examines the impact of surface-level modifications of Mg, Cu, and Sn on Ni-Ce-Zr catalysts for the hydrogenolysis of glycerol, with in situ generated hydrogen. The aim of this approach is to enhance the efficiency and sustainability of the biomass valorization process. However, the surface modification resulted in a decrease in the global conversion of glycerol due to the reduced availability of metal sites. The study found that valuable products, such as H2 and CH4 in the gas phase, and 1,2-PG in the liquid phase, were obtained. The majority of the liquid fraction was observed, particularly for Cu- and Sn-doped catalysts, which was attributed to their increased acidity. The primary selectivity was towards the cleavage of the C–O bond. Post-reaction characterizations revealed that the primary causes of deactivation was leaching, which was reduced by the inclusion of Cu and Sn. These findings demonstrate the potential of Cu- and Sn-modified Ni-Ce-Zr catalysts to provide a sustainable pathway for converting glycerol into value-added chemicals.

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Experimental and theoretical evidence of charge transfer in multi-component alloys – how chemical interactions reduce atomic size mismatch

Abstract: Ab-initio simulations of a multi-component alloy using density functional theory (DFT) were combined with experiments on thin films of the same material using X-ray photoelectron spectroscopy (XPS) to study the...

Cited by 25 publications

References 43 publications

Surface Tailoring-Modulated Bifunctional Oxygen Electrocatalysis with CoP for Rechargeable Zn–Air Battery and Water Splitting

Surface Tailoring-Modulated Bifunctional Oxygen Electrocatalysis with CoP for Rechargeable Zn–Air Battery and Water Splitting

Investigation of the phase formation in magnetron sputtered hard multicomponent (HfNbTiVZr)C coatings

Hydrogenolysis of Glycerol over NiCeZr Catalyst Modified with Mg, Cu, and Sn at the Surface Level

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