Combinatorial Search for High-Activity Hydrogen Catalysts Based on Transition-Metal-Embedded Graphitic Carbons
Abstract
Transition metal (TM) atoms in porphyrin–like complexes play important roles in many protein and enzymetic systems, where crystal–field effects are used to modify d–orbital levels. Inspired by the tunable electronic structure of these motifs, a high–throughput computational search for synthetic hydrogen catalysts is performed based on a similar motif of TM atoms embedded into the lattice of graphene. Based on an initial list of 300 possible embedding geometries, binders, and host atoms, descriptors for stability and catalytic activity are applied to extract ten promising candidates for hydrogen evolution, two of which are expected to exhibit high activity for hydrogen oxidation. In several instances, the active TM atoms are earth–abundant elements that show no activity in the bulk phase, highlighting the importance of the coordination environment in tuning the d–orbitals. In conclusion, it is found that the most active candidates involve a hitherto unreported surface reaction pathway that involves a Kubas–complex intermediate, which significantly lowers the kinetic barrier associated with hydrogen dissociation and association.
- Authors:
-
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Samsung Advanced Institute of Technology, Gyeonggi-do (South Korea)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1438765
- Report Number(s):
- LLNL-JRNL-737906
Journal ID: ISSN 1614-6832
- Grant/Contract Number:
- AC52-07NA27344
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Energy Materials
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 23; Journal ID: ISSN 1614-6832
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 08 HYDROGEN; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; computational high-throughput screening; density functional theory calculations; graphene; hydrogen catalysts; transition metals
Citation Formats
Choi, Woon Ih, Wood, Brandon C., Schwegler, Eric, and Ogitsu, Tadashi. Combinatorial Search for High-Activity Hydrogen Catalysts Based on Transition-Metal-Embedded Graphitic Carbons. United States: N. p., 2015.
Web. doi:10.1002/aenm.201501423.
Choi, Woon Ih, Wood, Brandon C., Schwegler, Eric, & Ogitsu, Tadashi. Combinatorial Search for High-Activity Hydrogen Catalysts Based on Transition-Metal-Embedded Graphitic Carbons. United States. doi:https://doi.org/10.1002/aenm.201501423
Choi, Woon Ih, Wood, Brandon C., Schwegler, Eric, and Ogitsu, Tadashi. Tue .
"Combinatorial Search for High-Activity Hydrogen Catalysts Based on Transition-Metal-Embedded Graphitic Carbons". United States. doi:https://doi.org/10.1002/aenm.201501423. https://www.osti.gov/servlets/purl/1438765.
@article{osti_1438765,
title = {Combinatorial Search for High-Activity Hydrogen Catalysts Based on Transition-Metal-Embedded Graphitic Carbons},
author = {Choi, Woon Ih and Wood, Brandon C. and Schwegler, Eric and Ogitsu, Tadashi},
abstractNote = {Transition metal (TM) atoms in porphyrin–like complexes play important roles in many protein and enzymetic systems, where crystal–field effects are used to modify d–orbital levels. Inspired by the tunable electronic structure of these motifs, a high–throughput computational search for synthetic hydrogen catalysts is performed based on a similar motif of TM atoms embedded into the lattice of graphene. Based on an initial list of 300 possible embedding geometries, binders, and host atoms, descriptors for stability and catalytic activity are applied to extract ten promising candidates for hydrogen evolution, two of which are expected to exhibit high activity for hydrogen oxidation. In several instances, the active TM atoms are earth–abundant elements that show no activity in the bulk phase, highlighting the importance of the coordination environment in tuning the d–orbitals. In conclusion, it is found that the most active candidates involve a hitherto unreported surface reaction pathway that involves a Kubas–complex intermediate, which significantly lowers the kinetic barrier associated with hydrogen dissociation and association.},
doi = {10.1002/aenm.201501423},
journal = {Advanced Energy Materials},
number = 23,
volume = 5,
place = {United States},
year = {2015},
month = {9}
}
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