Li Meiping, Lv Qing, Si Wenyan, Hou Zhufeng, Huang Changshui
Science Center for Material Creation and Energy Conversion, School of Chemistry and Chemical Engineering, Institute of Frontier and Interdisciplinary Science, Shandong University, Jinan, 250100, P. R. China.
Qingdao institute of Bioenergy and Bioprocess Technology, Chinese Academy of Science, No. 189 Songling Road, Qingdao, 266101, P. R. China.
Angew Chem Int Ed Engl. 2022 Sep 19;61(38):e202208238. doi: 10.1002/anie.202208238. Epub 2022 Aug 8.
Carbon supported single-atom catalysts with metal-N configuration are considered as one of the most efficient catalysts for the oxygen reduction reaction (ORR). However, most of the metal-N active sites are composed by pyridinic N at the defect locations of graphene-like supports. Here, we employ graphdiyne (GDY) as a new carbon substrate to synthesize an iron (Fe) single atom catalyst (Fe-N-GDY), showing excellent catalytic performance. Benefitting from the abundant acetylenic bonds in GDY, sp-N anchored metal atoms are created without forming defects. The sp-N and OH ligands regulate the electronic structure of Fe atoms and optimize the adsorption energy of ORR intermediates on the active sites by reducing the electron local density of Fe atoms, which accelerates the reaction kinetics and promotes the ORR activity of Fe-N-GDY. Furthermore, the practical application of Fe-N-GDY is corroborated by its high power density and long-term performance via assembling a zinc-air battery.
具有金属 - N构型的碳载单原子催化剂被认为是氧还原反应（ORR）中最有效的催化剂之一。然而，大多数金属 - N活性位点是由类石墨烯载体缺陷位置处的吡啶氮组成。在此，我们采用石墨炔（GDY）作为新型碳基底来合成铁（Fe）单原子催化剂（Fe - N - GDY），其表现出优异的催化性能。得益于GDY中丰富的炔键，形成了sp - N锚定的金属原子而不产生缺陷。sp - N和OH配体调节Fe原子的电子结构，并通过降低Fe原子的电子局部密度来优化ORR中间体在活性位点上的吸附能，从而加速反应动力学并提升Fe - N - GDY的ORR活性。此外，通过组装锌空气电池，Fe - N - GDY的高功率密度和长期性能证实了其实际应用价值。
