Abstract

AbstractTo achieve practical application of fuel cell, it is vital to develop highly efficient and durable Pt‐free catalysts. Herein, we prepare atomically dispersed ZnNC catalysts with Zn‐Pyrrolic‐N4 moieties and abundant mesoporous structure. The ZnNC‐based anion‐exchange membrane fuel cell (AEMFC) presents an ultrahigh peak power density of 1.63 and 0.83 W cm−2 in H2‐O2 and H2‐air (CO2‐free), and also exhibits long‐term stability with more than 120 and 100 h for H2‐air (CO2‐free) and H2‐O2, respectively. Density functional calculations further unveil that the Zn‐Pyrrolic‐N4 structure is the origin of high activity of as‐synthesized ZnNC catalyst, while the Zn‐Pyridinic‐N4 moiety is inactive for oxygen reduction reaction (ORR), which successfully explain the puzzle why most Zn‐metal‐organic framework ‐derived ZnNC catalysts in previous reports did not present good ORR activity because of their Zn‐Pyridinic‐N4 moieties. This work offers a new route for speeding up development of AEMFCs.

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