This paper mainly uses the molecular recognition principle and synergistic effect to synthesize the functional supramolecular 2,7-bis(4-([2,2':6',2''-terpyridin]-4'-yl)phenyl)-9-(heptadecan-9-yl)-9 H -carbazole. The nitrogen active sites at both ends of terpyridine are coordinated with metal copper ions to form a metal supramolecular catalyst that contains both the metal and nitrogen active sites. The surface physical structure and elemental analysis of the synthesized complexes were analyzed using SEM and XPS. The redox properties of the catalysts were characterized using chemical characterization methods, such as cyclic voltammetry (CV), linear sweep voltammetry (LSV), and a rotating ring disk electrode (RRDE). The physical and chemical analysis showed that the catalyst was successfully synthesized and that it was subjected to a redox reaction via a four-electron process. Therefore, the prepared metal supramolecular catalyst has good catalytic performance.
Lin Gu,Yunyun Dong,Yan Zhang,Bo Wang,Qing Yuan,Hongmei Du,Jinsheng Zhao
In this study, a nitrogen-containing ligand supramolecule named PPYTZ was successfully synthesized using 2,6-pyridinedicarboxylic acid chloride and 3,5-diamino-1,2,4-triazole in order to carry out oxygen reduction reaction (ORR). Such a polymer provides abundant coordination sites for iron ions, and the PPYTZ–Fe/C composite catalyst was formed with the PPYTZ–Fe complex loading on the surface of Vulcan XC-72 carbon. The physical characteristics and ORR performance of the composite catalysts were characterized systematically via various relevant techniques, and their catalytic activity and reaction mechanism were evaluated and compared. The results showed that the catalytic activities and the reaction mechanism of ORR were highly dependent on the formation of an Fe–N unit. Accordingly, the PPYTZ–Fe/C catalyst containing Fe–N active sites exhibited high ORR catalytic activity (an onset potential of +0.86 V vs. RHE) in 0.1 M KOH. Such an Fe–N catalyst can accelerate the adsorption of O2 and increase the limiting current density (from 2.49 mA cm−2 to 4.98 mA cm−2), optimizing the ORR catalytic process from a two-electron process to a four-electron process (an n value of 3.8).