Energetics and Structure of Nickel Atoms and Nanoparticles on MgO(100)

Mao, Zhongtian; Zhao, Wei; Al-Mualem, Ziareena A.; Campbell, Charles T.

doi:10.1021/acs.jpcc.0c03468

Energetics and Structure of Nickel Atoms and Nanoparticles on MgO(100)

Journal Article · Fri Jun 12 00:00:00 EDT 2020 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c03468· OSTI ID:1774928

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Univ. of Washington, Seattle, WA (United States); University of Washington
Univ. of Washington, Seattle, WA (United States); Shenzhen Univ., Guangdong (China)
Univ. of Washington, Seattle, WA (United States); Univ. of Texas, Austin, TX (United States)
Univ. of Washington, Seattle, WA (United States)

The growth morphology and interfacial energetics of vapor deposited Ni on the MgO(100) surface at 300 and 100 K have been studied using single crystal adsorption calorimetry (SCAC), He⁺ low-energy ion scattering spectroscopy (LEIS), X-ray photoelectron spectroscopy (XPS), and low-energy electron diffraction (LEED). At 300 K, the Ni atoms grow as three-dimensional nanoparticles with a saturation number density of 5 × 10¹⁶ particles/m². The differential heat of adsorption at 300 K increases rapidly with coverage, from 276 (initially) to 311 kJ/mol by 0.4 ML. Thereafter, it slowly increases asymptotically to the sublimation enthalpy of bulk Ni (430 kJ/ml) by 9 ML. The Ni 2p_3/2 XPS peak binding energy at 300 K is initially (i.e., at 0.16 ML) 1.4 eV higher than that for bulk Ni(solid), but it decreases to that value at high coverage. The Ni atoms form a metastable phase at 300 K when in nanoparticles with diameter <2.5 nm, and the adhesion energy of such Ni nanoparticles to MgO(100) was found to be 3.05 J/m². At 100 K, the Ni atoms form single adatoms and then 0.17 nm thick 2D islands at low coverage with fewer Ni-Ni bonds compared to the Ni nanoparticles formed at 300 K. Thus, the initial heat (i.e., for the first ~0.03 ML) is 148 kJ/mol at 100 K, 128 kJ/mol lower than at 300 K, and remains lower for the 2D islands. With increasing coverage at 100 K, the tiny 2D Ni islands grow in size to cover nearly the entire surface before thickening. Lastly, the XPS Ni 2p_3/2 peak binding energy for 0.21 ML Ni on MgO(100) at 100 K is 2.2 eV higher than that for bulk Ni(solid), suggesting charge transfer from Ni to MgO(100) and formation of Ni²⁺ at very low coverage.

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Research Organization:: Univ. of Washington, Seattle, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: FG02-96ER14630

OSTI ID:: 1774928

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 27 Vol. 124; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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