Preparative-scale electrolysis has been used as an industrial process to produce bulk chemicals for more than a century. Yet, examples for electrochemistry in bench-top synthesis and the fine chemicals industry remain scarce, largely due to the lack of access to a standard electrolysis instrument, and, perhaps more importantly, poor reactant-to-electrode transport that fundamentally limits the synthetic through-put. It would therefore be attractive to develop a platform with a tunable voltage supply and a facile integration into high-throughput analytical methods, all the while bypassing the traditional mass transfer limit towards the electrodes. Recent advances in understanding molecular interactions with nanostructured carbon materials have led to a myriad of exotic energy generation schemes. Along with these exciting developments, we have introduced a strategy called asymmetric chemical doping (ACD), which involves a chemical potential gradient established using acetonitrile (CH3CN) molecular dopants, as a mean of electricity generation. With a tunable voltage output in excess of 1.0 V, and a wide range of compatible solvents including the CH3CN used in abundance by chemists, we take advantage of this phenomenon, and construct a particulate platform that generates “packets” of electricity on demand, in solution, and drives electrochemical transformations in situ by virtue of interacting with the solvent. We demonstrated the potential to multiplex this form of electricity with high-throughput reaction monitoring, parameter optimization, or even continuous chemical production schemes, into what we have identified as a packed bed electrochemical reactor (PBER). We believe the idea of dividing electricity into modular and customizable units and incorporating them as synthetic building blocks, may address some of the remaining challenges in using preparative-scale electrolysis for molecular assembly.

Single-walled carbon nanotube mediated in situ electrochemistry

256th National Meeting (2018)

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