Single-atom electrocatalysts based on the M−N4 coordination shells are one of the most promising non-precious metal catalysts for the oxygen reduction reaction (ORR). However, the traditional preparation methods involving high-temperature pyrolysis of carbonaceous materials often afford materials which suffer from uncontrollable site structure, a limited number of active sites, and low mass/volume specific activity. Herein, we have prepared two-dimensional conjugated aromatic networks (CAN) incorporating metal phthalocyanine (Pc(M)) materials with ultra-thin conjugated layers (ca. 3.5 nm) and a high single-metal-atom-site density (mass content of 10.7 wt.%, and 0.73 metal atoms per nm2) via a facile pyrolysis-free route involving a one-step ball milling of the solid-phase-synthesized polyphthalocyanine. These materials have electrocatalytic properties for ORR which are superior to those of both Pt and Pt/C in benchmark Pt/C; the observed mass activity of 47 mA mg-1 represents 1.3- and 6.4-fold enhancements compared with Pt and Pt/C, respectively. Density functional theory calculations revealed that the outstanding ORR properties of the CAN materials is associated with the enhanced electron delocalization on bimetallic sites within the M–N4 structure. Our strategy offers a new way to design high-performance electrocatalysts with atomic precision for use in other energy storage and conversion applications.

Two-dimensional conjugated aromatic networks as high-site-density and single-atom electrocatalysts for the oxygen reduction reaction

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.