ACS Appl Mater Interfaces. 2018 Jun 6;10(22):18734-18745. doi: 10.1021/acsami.8b04060. Epub 2018 May 23.
Development of highly active and durable catalysts for oxygen reduction reaction (ORR) alternative to Pt-based catalyst is an essential topic of interest in the research community but a challenging task. Here, we have developed a new type of face-centered tetragonal (fct) PdFe-alloy nanoparticle-encapsulated Pd (fct-PdFe@Pd) anchored onto nitrogen-doped graphene (NG). This core-shell fct-PdFe@Pd@NG hybrid is fabricated by a facile and cost-effective technique. The effect of temperature on the transformation of face-centered cubic (fcc) to fct structure and their effect on ORR activity are systematically investigated. The core-shell fct-PdFe@Pd@NG hybrid exerts high synergistic interaction between fct-PdFe@Pd NPs and NG shell, beneficial to enhance the catalytic ORR activity and excellent durability. Impressively, core-shell fct-PdFe@Pd@NG hybrid exhibits an excellent catalytic activity for ORR with an onset potential of ∼0.97 V and a half-wave potential of ∼0.83 V versus relative hydrogen electrode, ultrahigh current density, and decent durability after 10 000 potential cycles, which is significantly higher than that of marketable Pt/C catalyst. Furthermore, the core-shell fct-PdFe@Pd@NG hybrid also shows excellent tolerance to methanol, unlike the commercial Pt/C catalyst. Thus, these findings open a new protocol for fabricating another core-shell hybrid by facile and cost-effective techniques, emphasizing great prospect in next-generation energy conversion and storage applications.
开发高效且稳定的氧还原反应(ORR)催化剂替代铂基催化剂是研究界关注的一个重要课题,但也是一项极具挑战性的任务。在这里,我们开发了一种新型面心四方(fct)钯铁合金纳米颗粒封装钯(fct-PdFe@Pd)负载在氮掺杂石墨烯(NG)上的催化剂。该核壳结构的 fct-PdFe@Pd@NG 杂化材料是通过一种简便且具有成本效益的技术制备的。我们系统地研究了温度对面心立方(fcc)到 fct 结构转变的影响及其对 ORR 活性的影响。核壳结构的 fct-PdFe@Pd@NG 杂化材料中 fct-PdFe@Pd NPs 与 NG 壳之间存在着高度协同的相互作用,有利于增强催化 ORR 活性和出色的耐久性。令人印象深刻的是,核壳结构的 fct-PdFe@Pd@NG 杂化材料在 ORR 中表现出优异的催化活性,其起始电位约为 0.97 V,半波电位约为 0.83 V 相对于相对氢电极,具有超高的电流密度和出色的耐久性,在 10000 次电势循环后仍保持稳定,明显优于市售的 Pt/C 催化剂。此外,与商业 Pt/C 催化剂相比,核壳结构的 fct-PdFe@Pd@NG 杂化材料对甲醇也具有出色的耐受性。因此,这些发现为通过简便且具有成本效益的技术制备另一种核壳杂化材料开辟了新途径,强调了其在下一代能源转换和存储应用中的广阔前景。