Porphyrinic MOF derived Single-atom electrocatalyst enables methanol oxidation

Zhou, Zhenyu; Zhang, Jing; Mukherjee, Soumya; Hou, Shujin; Khare, Rachit; Doblinger, Markus; Tomanec, Ondrej; Otyepka, Michal; Koch, Max; Gao, Pan; Zhou, Liujiang; Li, Weijin und Rischer, Roland A. (2022): Porphyrinic MOF derived Single-atom electrocatalyst enables methanol oxidation. In: Chemical Engineering Journal, Bd. 449, 137888

Abstract

Electrochemical methanol oxidation reaction (MOR) serves as a key route for renewable energy technologies. However, unmet challenges remain in the preparation of low-cost, efficient and robust electrocatalysts for MOR. Herein, a porphyrinic metal-organic framework (MOF) with spatially isolated Ni centres is prepared. Upon pyrolysis, this affords a single-atom Ni implanted nitrogen-doped porous carbon (20% Ni-N-C). Integrating abundant and accessible single-atom Ni sites, hierarchical porosity, excellent conductivity with stable Ni-N4 moieties all in one, the derived ultra-stable 20% Ni-N-C exhibits high MOR activity, impressive durability and CO tolerance, thereby outperforming state-of-the-art nonprecious metal based electrocatalysts. Computational insights reveal a low energy barrier of 1.19 eV for the rate-determining step, in agreement with the experimental observations of superior MOR activity. As the first foray into improving MOR efficiency with nonprecious metal based single-atom electrocatalysts, the yet-unrealized potential for MOFs and related modular hybrids is demonstrated.

• Dokumententyp: Zeitschriftenartikel
• Fakultät: Chemie und Pharmazie > Department Chemie
• Themengebiete: 500 Naturwissenschaften und Mathematik > 540 Chemie
• ISSN: 1385-8947
• Sprache: Englisch
• DFG: Gefördert durch die Deutsche Forschungsgemeinschaft (DFG) - 419949637
• DFG: Gefördert durch die Deutsche Forschungsgemeinschaft (DFG) - 316376997
• DFG: Gefördert durch die Deutsche Forschungsgemeinschaft (DFG) - 390776260