Lanthanum-Promoted Electrocatalyst for the Oxygen Evolution Reaction: Unique Catalyst or Oxide Deconstruction?

Hartnett, Alaina C.; Evenson, Ryan J.; Thorarinsdottir, Agnes E.; Veroneau, Samuel S.; Nocera, Daniel G.

doi:10.1021/jacs.4c14696

Lanthanum-Promoted Electrocatalyst for the Oxygen Evolution Reaction: Unique Catalyst or Oxide Deconstruction?

Journal Article · Fri Dec 20 00:00:00 EST 2024 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.4c14696· OSTI ID:2868487

^[1]; Evenson, Ryan J. ^[1]; ^[2]; ^[1]; ^[1]

Harvard University, Cambridge, MA (United States)
Harvard University, Cambridge, MA (United States); University of Rochester, NY (United States)

A conventional performance metric for electrocatalysts that promote the oxygen evolution reaction (OER) is the current density at a given overpotential. However, the assumption that increased current density at lower overpotentials indicates superior catalyst design is precarious for OER catalysts in the working environment, as the crystalline lattice is prone to deconstruction and amorphization, thus greatly increasing the concentration of catalytic active sites. We show this to be the case for La³⁺ incorporation into Co₃O₄. Powder X-ray diffraction (PXRD), Raman spectroscopy and extended X-ray absorption fine structure (EXAFS) reveal smaller domain sizes with decreased long-range order and increased amorphization for La-modified Co₃O₄. This lattice deconstruction is exacerbated under the conditions of OER as indicated by operando spectroscopies. The overpotential for OER decreases with increasing La³⁺ concentration, with maximum activity achieved at 17% La incorporation. HRTEM images and electron diffraction patterns clearly show the formation of an amorphous overlayer during OER catalysis that is accelerated with La³⁺ addition. O 1s XPS spectra after OER show the loss of lattice-oxide and an increase in peak intensities associated with hydroxylated or defective O-atom environments, consistent with Co(O)_x(OH)_y species in an amorphous overlayer. Furthermore, our results suggest that improved catalytic activity of oxides incorporated with La³⁺ ions (and likely other metal ions) is due to an increase in the number of terminal octahedral Co(O)_x(OH)_y edge sites upon Co₃O₄ lattice deconstruction, rather than enhanced intrinsic catalysis.

View Accepted Manuscript (DOE)

Research Organization:: Harvard University, Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357; SC0017619

OSTI ID:: 2868487

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 1 Vol. 147; ISSN 0002-7863; ISSN 1520-5126

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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