Irvine Materials Research Institute (IMRI) , University of California , Irvine , California 92697 , United States.
Department of Chemistry and Biochemistry , Northern Illinois University , DeKalb , Illinois 60115 , United States.
ACS Appl Mater Interfaces. 2019 Oct 30;11(43):39820-39826. doi: 10.1021/acsami.9b12054. Epub 2019 Oct 21.
Recently, electrocatalysts based on anchored dispersive/isolated single metal atoms on conductive carbon supports have demonstrated great promise to substitute costly Pt for the oxygen reduction reaction (ORR) in the field of fuel cells or metal-air batteries. However, developments of cost-efficient single-atom Fe catalysts with high activities are still facing various hardships. Here, we developed a facile way to synthesize isolated iron atoms anchored on the carbon nanotube (CNT) involving a one-pot pyrrole polymerization on a self-degraded organic template and a subsequent pyrolysis. The as-obtained electrocatalyst possessed unique characteristics of abundant nanopores in the wall of conductive CNTs to host the abundant atomic Fe-N active sites, showing ultrahigh ORR activity (half-wave potential: 0.93 V, kinetic current density: 59.8 mA/cm at 0.8 V), better than that of commercial Pt/C (half-wave potential: 0.91 V; kinetic current density: 38.0 mA/cm at 0.8 V) in an alkaline electrolyte. Furthermore, good ORR activity has been proven in acidic solution with a half-wave-potential of 0.73 V.
最近,基于负载在导电碳载体上的锚定分散/孤立单金属原子的电催化剂在燃料电池或金属空气电池领域中,为替代昂贵的 Pt 用于氧还原反应(ORR)展示出巨大的应用前景。然而,开发具有高活性的成本效益高的单原子 Fe 催化剂仍然面临着各种困难。在这里,我们开发了一种简便的方法来合成锚定在碳纳米管(CNT)上的孤立铁原子,涉及在自降解有机模板上的一锅吡咯聚合和随后的热解。所获得的电催化剂具有独特的特性,即导电 CNT 壁中丰富的纳米孔可以容纳丰富的原子 Fe-N 活性位,在碱性电解质中表现出超高的 ORR 活性(半波电位:0.93 V,在 0.8 V 时的动力学电流密度:59.8 mA/cm),优于商业 Pt/C(半波电位:0.91 V;在 0.8 V 时的动力学电流密度:38.0 mA/cm)。此外,在酸性溶液中也表现出良好的 ORR 活性,半波电位为 0.73 V。