Charge-compensated co-doping of graphdiyne with boron and nitrogen to form metal-free electrocatalysts for the oxygen reduction reaction

Literature Information

Publication Date 2019-11-29
DOI 10.1039/C9CP05344A
Impact Factor 3.676
Authors

Yaqiang Ma, Yi Li, Renyi Li, Yanan Tang, Xianqi Dai


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Abstract

The development of metal-free catalysts for the oxygen reduction reaction (ORR) is critical for rechargeable metal–air batteries and full cells. Various light non-metallic-atom-doped graphdiyne (GDY) materials have been designed based on density functional theory and evaluated as efficient ORR electrocatalysts. Volcano curve correlations between the overpotential and Gibbs adsorption free energies of oxygenated intermediates have been derived for the ORR. Optimized compensated B,N co-doped GDY monolayers exhibit the lowest ORR overpotential of 0.57 V. In compensated B,N co-doped GDY, the B atoms are positioned in the benzene rings, and the N atoms are positioned in the acetylene linkages. Moreover, some B,N co-doped GDYs have two active sites with almost the same catalytic activity: the B atom and the C atom bearing an effective positive charge nearest to the doped N atom. Based on the theoretical analysis, ideal doped GDY monolayers are expected to exhibit comparable catalytic activity to Pt-based catalysts.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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