Dispersions of purely semiconducting single-walled carbon nanotubes (SWCNTs) have enabled solution-processed SWCNT networks as active layers in field-effect transistors (FETs) with high carrier mobilities and excellent on/off current ratios. Although reproducibility has improved in recent years, reaching the level that is required for commercial large-scale processing remains a challenge. A key issue is the tendency of SWCNTs to aggregate over time, resulting in network inhomogeneities that cause large device performance variations. Based on the tailored formulation of colloidal inks by the choice of solvent and use of additives, we demonstrate the strong stabilization effect of phenanthroline additives on polymer-sorted (6,5) SWCNT using time-dependent near-infrared absorption spectroscopy as a fast and simple assessment tool for the aggregation rate. The addition of the N-heteropolycycle 1,10-phenanthroline significantly extends the stability of dispersions of polymer-wrapped nanotubes in toluene and hence improves the morphology of spin-coated networks even after ink storage for several days. Bottom-contact, top-gate FETs based on such networks show much higher charge carrier mobilities and drastically reduced device-to-device variations compared to devices based on SWCNT dispersions without phenanthroline. Nanotube ink formulations with small-molecule additives are an important step toward reproducible device parameters and are crucial for the translation of nanotube FETs from the laboratory to commercial applications.
Heteroatom-doped polyaromatic hydrocarbons (or nanographenes) are promising molecular electrocatalysts for the oxygen reduction reaction (ORR). Here, we use density functional theory to investigate the first step of the ORR pathway (chemisorption) for a set of molecules with experimentally determined catalytic activities. Weak chemisorption is found for only negatively charged catalysts, and a strong correlation is observed between the computed electron affinities and experimental catalytic activities for a range of B-and B,Ndoped polyaromatic hydrocarbons. The electron affinity is put forward as a simple activity descriptor of charged (activated) catalysts on an electrode.
Heteroatom-doped polyaromatic hydrocarbons (or nanographenes) are promising molecular electrocatalysts for the oxygen reduction reaction (ORR). Here, we use density functional theory to investigate the first step of the ORR pathway (chemisorption) for a set of molecules with experimentally determined catalytic activities. Weak chemisorptions are found only for negatively charged catalysts, and a strong correlation is observed between computed electron affinities and experimental catalytic activities for a range of B- and B,N-doped polyaromatic hydrocarbons. The electron affinity is put forward as a simple activity descriptor of charged (activated) catalysts on an electrode.
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