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Abstract Building upon thed-band reactivity theory in surface chemistry and catalysis, we develop a Bayesian learning approach to probing chemisorption processes at atomically tailored metal sites. With representative species, e.g., *O and *OH, Bayesian models trained with ab initio adsorption properties of transition metals predict site reactivity at a diverse range of intermetallics and near-surface alloys while naturally providing uncertainty quantification from posterior sampling. More importantly, this conceptual framework sheds light on the orbitalwise nature of chemical bonding at adsorption sites withd-states characteristics ranging from bulk-like semi-elliptic bands to free-atom-like discrete energy levels, bridging the complexity of electronic descriptors for the prediction of novel catalytic materials.
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Periodicity in the Electrochemical Dissolution of Transition Metals
Abstract Extensive research efforts are currently dedicated to the search for new electrocatalyst materials in which expensive and rare noble metals are replaced with cheaper and more abundant transition metals. Recently, numerous alloys, oxides, and composites with such metals have been identified as highly active electrocatalysts through the use of high‐throughput screening methods with the help of activity descriptors. Up to this point, stability has lacked such descriptors. Hence, we elucidate the role of intrinsic metal/oxide properties on the corrosion behavior of representative 3d, 4d, and 5d transition metals. Electrochemical dissolution of nine transition metals is quantified using online inductively coupled plasma mass spectrometry (ICP‐MS). Based on the obtained dissolution data in alkaline and acidic media, we establish clear periodic correlations between the amount of dissolved metal, the cohesive energy of the metal atoms (Ecoh), and the energy of oxygen adsorption on the metal (ΔHO,ads). Such correlations can support the knowledge‐driven search for more stable electrocatalysts.
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- Award ID(s):
- 1941204
- PAR ID:
- 10226910
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Angewandte Chemie International Edition
- Volume:
- 60
- Issue:
- 24
- ISSN:
- 1433-7851
- Page Range / eLocation ID:
- p. 13343-13349
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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