Tailor of high performance electrocatalyst for oxygen reduction reaction through rational structural adjustment of carbon-based architecture

Abstract The shortage of high effective and reliable cathode catalysts with desirable performance for oxygen reduction needs to be addressed to accelerate the large-scale expansion of clean and sustainable fuel cells. Herein, we report a facile hydrothermal route to tailor a new type of N, P co-doped carbon architecture with Fe2P nanoparticles embedded/encapsulated in the crumped carbon nanosheets. The rational design of carbon shell structure in strong interaction with rGO endows the catalyst with graphitic-N abundance, mesoporous structure dominance and active Fe2P isolation. We propose the pyrolyzed dicyandiamide-derived carbon fragment as not only an additional nitrogen resource but a favorable micro-structured separator and protective porous layer for metal agglomeration and demetallation, which ensures the catalyst with excellent activity and stability. The co-doped carbon shows excellent activity with positive half-wave potential of +0.823 V via complete 4 electron pathway, close to that of Pt/C material (+0.831 V). The inspiring durability is confirmed by merely 2 mV negative potential shifts after 1000 cycles of CV tests. In the end, this paper provides a promising way to develop a high effective carbon-based bifunctional catalyst for both oxygen reduction and evolution reactions through electronic design and structural engineering.