Atomistic Insights into the Stability of Pt Single-Atom Electrocatalysts
Speck F, Paul MT, Ruiz-Zepeda F, Gatalo M, Kim H, Kwon HC, Mayrhofer K, Choi M, Choi CH, Hodnik N, Cherevko S (2020)
Publication Type: Journal article
Publication year: 2020
Journal
Book Volume: 142
Pages Range: 15496-15504
Journal Issue: 36
DOI: 10.1021/jacs.0c07138
Abstract
Single-atom catalysts (SACs) have quickly emerged as a new class of catalytic materials. When confronted with classical carbon-supported nanoparticulated catalysts (Pt/C), SACs are often claimed to have superior electrocatalytic properties, e.g., stability. In this study, we critically assess this statement by investigating S-doped carbon-supported Pt SACs as a representative example of noble-metal-based SACs. We use a set of complementary techniques, which includes online inductively coupled plasma mass spectrometry (online ICP-MS), identical location transmission electron microscopy (IL-TEM), and X-ray photoelectron spectroscopy (XPS). It is shown by online ICP-MS that the dissolution behavior of as-synthesized Pt SACs is significantly different from that of metallic Pt/C. Moreover, Pt SACs are, indeed, confirmed to be more stable toward Pt dissolution. When cycled to potentials of up to 1.5 VRHE, however, the dissolution profiles of Pt SACs and Pt/C become similar. IL-TEM and XPS show that this transition is due to morphological and chemical changes caused by cycling. The latter, in turn, is a consequence of the relatively poor stability of S ligands. As monitored by online ICP-MS and XPS, significant amounts of sulfur leave the catalyst during oxidation. Hence, in case catalysts with improved stability in the anodic potential region are desired, more robust supports and ligands must be developed.
Authors with CRIS profile
Florian Speck
Lehrstuhl für Elektrokatalyse (HIERN)
Karl Mayrhofer
Lehrstuhl für Elektrokatalyse (HIERN)
Involved external institutions
Forschungszentrum Jülich / Research Centre Jülich (FZJ)
Germany (DE)
National Institute of Chemistry / Kemijski Inštitut
Slovenia (SI)
Gwangju Institute of Science and Technology (GIST) / 광주과학기술원
Korea, Republic of (KR)
Korea Advanced Institute of Science and Technology (KAIST)
Korea, Republic of (KR)
Germany (DE)
National Institute of Chemistry / Kemijski Inštitut
Slovenia (SI)
Gwangju Institute of Science and Technology (GIST) / 광주과학기술원
Korea, Republic of (KR)
Korea Advanced Institute of Science and Technology (KAIST)
Korea, Republic of (KR)
How to cite
APA:
Speck, F., Paul, M.T., Ruiz-Zepeda, F., Gatalo, M., Kim, H., Kwon, H.C.,... Cherevko, S. (2020). Atomistic Insights into the Stability of Pt Single-Atom Electrocatalysts. Journal of the American Chemical Society, 142(36), 15496-15504. https://dx.doi.org/10.1021/jacs.0c07138
MLA:
Speck, Florian, et al. "Atomistic Insights into the Stability of Pt Single-Atom Electrocatalysts." Journal of the American Chemical Society 142.36 (2020): 15496-15504.
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