Formation of active sites on transition metals through reaction-driven migration of surface atoms

Xu, Lang; Papanikolaou, Konstantinos G.; Lechner, Barbara J.; Je, Lisa; Somorjai, Gabor A.; Salmeron, Miquel; Mavrikakis, Manos

doi:10.1126/science.add0089

Formation of active sites on transition metals through reaction-driven migration of surface atoms

Journal Article · Fri Apr 07 00:00:00 EDT 2023 · Science

DOI:https://doi.org/10.1126/science.add0089· OSTI ID:2007901

^[1]; ^[2]; ^[3]; ^[2]; Somorjai, Gabor A. ^[4]; ^[4]; ^[2]

Univ. of Wisconsin, Madison, WI (United States); University of Wisconsin–Madison Department of Chemical and Biological Engineering
Univ. of Wisconsin, Madison, WI (United States)
Technical Univ. of Munich (Germany); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)

Adopting low-index single-crystal surfaces as models for metal nanoparticle catalysts has been questioned by the experimental findings of adsorbate-induced formation of subnanometer clusters on several single-crystal surfaces. Here we used density functional theory calculations to elucidate the conditions that lead to cluster formation and show how adatom formation energies enable efficient screening of the conditions required for adsorbate-induced cluster formation. We studied a combination of eight face-centered cubic transition metals and 18 common surface intermediates and identified systems relevant to catalytic reactions, such as carbon monoxide (CO) oxidation and ammonia (NH₃) oxidation. We used kinetic Monte Carlo simulations to elucidate the CO-induced cluster formation process on a copper surface. Scanning tunneling microscopy of CO on a nickel (111) surface that contains steps and dislocations points to the structure sensitivity of this phenomenon. Metal-metal bond breaking that leads to the evolution of catalyst structures under realistic reaction conditions occurs much more broadly than previously thought.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Wisconsin, Madison, WI (United States); Univ. of California (United States)

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

Contributing Organization:: Lawrence Berkeley National Laboratory (LBNL). National Energy Research Scientific Computing Center (NERSC); Argonne National Laboratory (ANL). Center for Nanoscale Materials (CNM)

Grant/Contract Number:: FG02-05ER15731; AC02-05CH11231; AC02-06CH11357

OSTI ID:: 2007901

Journal Information:: Science, Journal Name: Science Journal Issue: 6640 Vol. 380; ISSN 0036-8075

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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