Graphdiyne-Supported Single-Atom-Sized Fe Catalysts for the Oxygen Reduction Reaction: DFT Predictions and Experimental Validations

By Yuan Gao, Zhewei Cai, Xingchen Wu, Zhi-Suo Lv, Ping Wu, C. Cai. ACS Catalysis, 2018

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Single-atom-sized catalysts (often called single atom catalysts) are highly desired for maximizing the efficiency of metal atom use. However, their synthesis is a major challenge that largely depends on finding an appropriate supporting substrate to achieve a well-defined and highly dispersed single atom. This work demonstrates, based on density functional theory (DFT) predictions and experimental validations, that graphdiyne is a good substrate for anchoring Fe atoms through the formation of covalent Fe–C bonds to produce graphdiyne-supported single-atom-sized Fe catalysts (Fe–graphdiyne catalysts); moreover, this catalyst shows high catalytic activity to oxygen reduction reactions (ORRs) similar to or even slightly better than the precious metal benchmark (commercial 20 wt % Pt/C catalyst). DFT predicts that the O2 molecule can bind with an Fe atom, and the electron transformation process of ORRs occurs through a 4e– pathway. To validate the theoretical predictions, the Fe–graphdiyne catalyst was then s...

Subfields: Electrical and Electronic Engineering, Materials Chemistry, Renewable Energy, Sustainability and the Environment

View Paper: https://www.semanticscholar.org/paper/7605c98ca7ff75debec5cdcc7a45f2b6698e2e6f