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Bimetallic M/N/C catalysts prepared from π-expanded metal salen precursors toward an efficient oxygen reduction reaction

机译:由π膨胀的金属Salen前体制备的双金属M / N / C催化剂,可实现有效的氧还原反应

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Nonprecious metal electrocatalysts are being explored as alternatives to platinum-group metal electrocatalysts for the oxygen reduction reaction (ORR) which is required for cathode materials in fuel cells. Herein, we describe a new method for preparing bimetallic nitrogen-containing carbon catalysts with high ORR activity using π-expanded M(salen) precursors. The M/N/C and bimetallic FeM/N/C ORR catalysts were obtained by pyrolysis of a mixture of a carbon support (Vulcan XC-72R) and the metal complex as a precursor. The bimetallic FeCu catalyst prepared from Fe and Cu complexes with the N,N′-bis(2-hydroxy-1-naphthylidene)-1,2-phenylenediamine ligand (2NAPD) is found to have an onset potential of 0.87 V, which is positively shifted by 50 mV from that of the catalyst prepared from the monometallic Fe(2NAPD) complex. The FeCu/N/C catalyst promotes efficient four-electron reduction in the ORR. High-resolution transmission electron microscopy studies reveal that both Fe and Cu metals together with pyridinic nitrogen species are highly dispersed within the carbonaceous structure in FeCu/2NAPD@VC, suggesting that the N-coordinated Fe and Cu sites promote efficient four-electron reduction of O2. This new methodology facilitates design of nonprecious bimetallic carbon catalysts with excellent ORR activity.
机译:人们正在探索非贵金属电催化剂,以替代用于氧还原反应(ORR)的铂族金属电催化剂,这是燃料电池中阴极材料所必需的。在这里,我们描述了一种使用π膨胀的M(salen)前驱体制备具有高ORR活性的双金属含氮碳催化剂的新方法。 M / N / C和双金属FeM / N / C ORR催化剂是通过碳载体(Vulcan XC-72R)和作为前体的金属配合物的混合物热解而获得的。由Fe和Cu与 N N '-双(2-羟基-1-萘)-1,2-苯二胺配体(2NAPD)形成的双金属FeCu催化剂)被发现具有0.87 V的起始电势,与由单金属Fe(2NAPD)络合物制备的催化剂的起始电势正移50 mV。 FeCu / N / C催化剂可促进ORR的有效四电子还原。高分辨率透射电子显微镜研究表明,FeCu / 2NAPD @ VC的碳质结构中Fe和Cu金属以及吡啶氮元素都高度分散,这表明N配位的Fe和Cu位点促进了高效的四电子还原。 O 2 。这种新方法简化了具有出色ORR活性的非贵金属双金属碳催化剂的设计。

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