Hierarchically structured 3D carbon nanotube electrodes for electrocatalytic applications

Abstract

Hierarchically structured 3-dimensional electrodes based on branched carbon nanotubes (CNTs) are prepared on a glassy carbon (GC) substrate in a sequence of electrodeposition and chemical vapor deposition (CVD) steps as follows: Primary CNTs are grown over electrodeposited iron by CVD followed by a second Fe deposition and finally the CVD growth of secondary CNTs. The prepared 3-dimensional CNT structures (CNT/CNT/GC) exhibit enhanced double-layer capacitance and thus larger surface area compared to CNT/GC. Pt electrodeposition onto both types of electrodes yields a uniform and homogeneous Pt nanoparticle distribution. Each preparation step is followed by scanning electron microscopy, while the CNTs were additionally characterized by Raman spectroscopy. In this way it is demonstrated that by varying the parameters during the electrodeposition and CVD steps, a tuning of the structural parameters of the hierarchical electrodes is possible. The suitability of the hierarchical electrodes for electrocatalytic applications is demonstrated using the methanol electro-oxidation as a test reaction. The Pt mass specific activity towards methanol oxidation of Pt-CNT/CNT/GC is approximately 2.5 times higher than that of Pt-CNT/GC, and the hierarchical electrode exhibits a more negative onset potential. Both structures demonstrate an exceptionally high poisoning tolerance.