Fuling Wang,Xue Liu,Binghan Jiang,Hongyan Zhuo,Wenmiao Chen,Yanli Chen,Xiyou Li
Reducing the loading of Pt precious metal is the promising pathway to positively promote the large-scale application for fuel cells and water electrolysis. In this work, a composite bifunctional electrocatalyst (named Pt@Fe SA -N-C) consisting of the atomically dispersed FeN 4 active sites and Pt nanoparticles (NPs) is successfully prepared for oxygen reduction reaction (ORR) and hydrogen evolution reactions (HER). In the process of synthesizing precursor of Pt(OH) 4 -Fe-Ppy@CNFs, the Fe-Ppy@CNFs was firstly prepared where the highly dispersed Fe 3+ ions were pre-anchored into polypyrrole (PPy) matrixes through in-situ polymerization on the surface of cellulose nanofibers (CNFs) and then Pt(OH) 4 nano-particles were deposited on Fe-Ppy@CNFs through adjusting the pH of the solution by urea hydrolysis to obtain the Pt(OH) 4 -Fe-Ppy@CNFs. Compared with the commercial 20 wt.% Pt/C, the obtained Pt@Fe SA -N-C possesses 5.5 wt.% low Pt loading. The strong synergistic effect of dual active sites between Pt NPs and FeN 4 on one-dimensional (1D) Fe SA -N-C support with a large surface area ensures effectively exposure of Fe and especial Pt active sites in the Pt@Fe SA -N-C. Both ORR and HER activities of the Pt@Fe SA -N-C were greatly improved in acid and alkaline media, even outperforming the commercial 20 wt.% Pt/C. Furthermore, the Pt@Fe SA -N-C shows an unordinary stability, with no obvious decrease in the current density after 5000 and 1000 cycles of accelerated durability tests (ADTs) for ORR and HER processes, respectively. This work highlights a preparation strategy for the synergistic effect between low-loading Pt precious metal and non-precious metals in electrocatalytic system.
Single atom catalysts with high-catalytic activity have been applied in many fields. In this work, single Fe atoms (FeSA) showed excellent catalytic performance on P-nitrophenol (PNP) degradation with high total organic carbon (TOC) removal rate and high turnover frequency (TOF). The high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) results show that Fe species in FeSA are mainly single Fe atom. X-ray absorption near-edge structure (XANES) and density functional theory (DFT) calculations show that each single Fe atom is anchored by four N atoms in the form of FeN 4 active site. This coordination environment enables FeSA possesses unique geometric configuration and highly uniform active sites, which is conducive to organic pollutant adsorption and peroxymonosulfate (PMS) activation. In addition, FeSA could maintained excellent catalytic activity in complex water bodies containing different anions and humic acids. The active species in the FeSA/PMS system were also investigated. It is found that the main oxidative active species in the system are O 2 •− and 1 O 2 . This work shows that FeSA was a highly efficient single atom catalyst for the degradation of organic pollutants and has a wide application prospect in advanced oxidation processes.