Doping carbon network with multi-heteroatom is one of the most effective ways to achieve the carbon-based metal-free electrocatalyst with a superior activity for oxygen reduction reaction (ORR). Herein, multi-heteroatom doped three-dimensional hierarchically micro/mesoporous carbon was synthesized as an efficient metal-free electrocatalyst towards ORR by pyrolyzing thiourea (THU) with nitrogen- and phosphorus-doped (N- and P-doped) hierarchically porous carbon network derived from cattle bone. The obtained sulfur, nitrogen and phosphorus ternary-doped (S, N and P ternary-doped) carbon material has both a high porosity for effective mass transport of ORR reactants and abundant surface active sites for efficient ORR. As identified by X-ray absorption near edge spectroscopy, S dopant in the reduced form (S<sub>Red</sub>) plays a major role during ORR catalytic process. When used as an ORR electrocatalyst, the S, N and P ternary-doped carbon with the highest content of S<sub>Red</sub> outperformed the commercial Pt/C electrocatalyst in alkaline electrolytes with a superior electrocatalytic activity (~40 mV higher half-wave potential), an outstanding electrochemical durability and a good anti-poisoning capability. This work presents an effective approach for the design and synthesis of efficient metal-free ORR electrocatalysts from earth-abundant cattle bone and analogues.

Enhancement mechanism of sulfur dopant on catalytic activity of N and P co-doped three-dimensional hierarchically porous carbon as metal-free oxygen reduction electrocatalyst

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.