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Fe nanoparticles immobilized on polyaniline-covered carbon nanotube (CNT) surfaces (Fe NPs–PANI/CNT) are prepared by reducing FeCl 3 in the mixing solution of aniline and CNT. Significantly, the structure of such composites can be effectively optimized by pretreating FeCl 3 with sodium citrate (CA). In the absence of CNTs, we found these two routes have large differences in reduction behaviors and different PANI states with varied conductivities. Therefore, the self-assembly mechanism in the preparation is proposed and the controlled self-assembly manner in the pretreating route is disclosed. Under acid condition, both catalysts demonstrate high oxygen reduction reaction (ORR) activity with four-electron pathway, and high electrochemical durability, revealing a promising application in the proton exchange membrane fuel cells. However, the high Tafel slopes relating to the surface red-ox couple and porous conductivity are still the main obstacles to improve their ORR dynamic, and more efforts on these aspects are needed to drive non-noble catalyst application in future. [ABSTRACT FROM AUTHOR]

Abstract: This paper established an in-situ synthesis strategy that the mixing solution of aniline, CNTs and CoCl2 was directly reduced to prepare polyaniline-cobalt-carbon nanotube (PANI-Co-CNT) electrocatalyst. Furthermore, this strategy was effectively modified by pretreating CoCl2 precursor with citric acid (CA), forming 2-4nm cobalt nanoparticles uniformly distributed on PANI-CNT support with porous structure. The control experiments revealed various PANI states in the growth stage, further proposing the self-assembly mechanisms in these two routes with and without CA pretreatment. These two PANI-Co-CNT electrocatalysts were also checked by oxygen reduction reaction (ORR) in acid environment, to corroborate their basically 4-electron processes. Inspiringly, the large activity and stability for the pretreated route could be comparable with those of the advanced electrocatalysts. All these progresses lay a bottom-up approach for future electrocatalysts. [Copyright &y& Elsevier]