Abstract
Chemical doping through heteroatom substitution is often used to control the Fermi level of semiconductor materials. Doping also occurs when surface adsorbed molecules modify the Fermi level of low dimensional materials such as carbon nanotubes. A gradient in dopant concentration, and hence the chemical potential, across such a material generates usable electrical current. This opens up the possibility of creating asymmetric catalytic particles capable of generating voltage from a surrounding solvent that imposes such a gradient, enabling electrochemical transformations. In this work, we report that symmetry-broken carbon particles comprised of high surface area single-walled carbon nanotube networks can effectively convert exothermic solvent adsorption into usable electrical potential, turning over electrochemical redox processes in situ with no external power supply. The results from ferrocene oxidation and the selective electro-oxidation of alcohols underscore the potential of solvent powered electrocatalytic particles to extend electrochemical transformation to various environments.
Highlights
Chemical doping through heteroatom substitution is often used to control the Fermi level of semiconductor materials
As a mechanism of solvent-induced electron flow, we have recently introduced asymmetric chemical doping (ACD), a chemical potential gradient of electrical carriers in nanostructured carbon materials, established using an asymmetric adsorption of acetonitrile (CH3CN) molecular dopants, as a mechanism for adsorptioninduced electricity generation[13,14]
We fabricate symmetry-broken, carbon particles comprised of high surface area single-walled carbon nanotube (SWNT) and demonstrate their ability to convert exothermic solvent adsorption into usable electrical potential, turning over electrochemical redox processes in situ with no additional external power supplied
Summary
Chemical doping through heteroatom substitution is often used to control the Fermi level of semiconductor materials. With a tunable voltage output (up to 920 mV open-circuit potential), and a wide range of compatible solvents including the CH3CN, in this work we take advantage of this phenomenon in the design of a carbon Janus particle that generates solvent-induced electricity for electrochemical reactions (Fig. 1a).
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