Spray-drying as a tool to disperse conductive carbon inside Na2FePO4F particles by addition of carbon black or carbon nanotubes to the precursor solution

In this work, Na2FePO4F-carbon composite powders were prepared by spray-drying a solution of inorganic precursors with 10 and 20 wt% added carbon black (CB) or carbon nanotubes (CNTs). In order to compare the effect of CB and CNTwhen added to the precursor solutions, the structural, electrochemical, and morphological properties of the synthesized Na2FePO4F-xCB and Na2FePO4F-xCNT samples were systematically investigated. In both cases, X-ray diffraction shows that calcination at 600 °C in argon leads to the formation of Na2FePO4F as the major inorganic phase. 57Fe Mössbauer spectroscopy was used as complementary technique to probe the oxidation states, local environment, and identify the composition of the iron-containing phases. The electrochemical performance is markedly better in the case of Na2FePO4F-CNT (20 wt%), with specific capacities of about 100 mAh/g (Na2FePO4F-CNT) at C/4 rate vs. 50 mAh/g for Na2FePO4F-CB (20 wt%). SEM characterization of Na2FePO4F-CB particles revealed different particle morphologies for the Na2FePO4F-CNT and Na2FePO4F-CB powders. The carbon-poor surface observed for Na2FePO4FCB could be due to a slow diffusion of carbon in the droplets
during drying. On the contrary, Na2FePO4F-CNT shows a better CNT dispersion inside and at the surface of the NFPF particles that improves the electrochemical performance.