The development of low-cost, efficient, and stable electrocatalysts for the oxygen reduction reaction (ORR) is desirable but remains a great challenge. Herein, we made a highly reactive and stable isolated single-atom Fe/N-doped porous carbon (ISA Fe/CN) catalyst with Fe loading up to 2.16 wt %. The catalyst showed excellent ORR performance with a half-wave potential (E ) of 0.900 V, which outperformed commercial Pt/C and most non-precious-metal catalysts reported to date. Besides exceptionally high kinetic current density (J ) of 37.83 mV cm at 0.85 V, it also had a good methanol tolerance and outstanding stability. Experiments demonstrated that maintaining the Fe as isolated atoms and incorporating nitrogen was essential to deliver the high performance. First principle calculations further attributed the high reactivity to the high efficiency of the single Fe atoms in transporting electrons to the adsorbed OH species.
We develop an N-coordination strategy to design a robust CO reduction reaction (CORR) electrocatalyst with atomically dispersed Co-N site anchored on polymer-derived hollow N-doped porous carbon spheres. Our catalyst exhibits high selectivity for CORR with CO Faradaic efficiency (FE) above 90% over a wide potential range from -0.57 to -0.88 V (the FE exceeded 99% at -0.73 and -0.79 V). The CO current density and FE remained nearly unchanged after electrolyzing 10 h, revealing remarkable stability. Experiments and density functional theory calculations demonstrate single-atom Co-N site is the dominating active center simultaneously for CO activation, the rapid formation of key intermediate COOH* as well as the desorption of CO.
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