Work

Programmable Oxidation in Flow on Interdigitated Lateral Catalytic Condensers

Year: 2026

Type: preprint

Abstract: Heterogeneous catalysis remains fundamentally limited by the intrinsic static electronic and physical structure of the catalyst surface during reaction that restricts catalytic rates and limits reactions to equilibrium. To circumvent these limitations, a catalytic condenser enables the non-Faradaic dynamic modulation of surface binding energies through an external potential. Here, we describe an interdigitated (IDT) internal ion gel catalytic condenser within a continuous flow reactor for the electronic control of thermochemical carbon monoxide oxidation on Pt active sites. The device utilizes a thermally stable, high-capacitance ion gel electrolyte (PA6,6/[EDMIM][TFSI]) to establish an electric double layer at the metal-electrolyte interface, enabling both charge condensation and a strong electric field at the Pt active sites. Field strength was measured by Stark tuning of 4-mercaptobenzonitrile (4-MBN) on a model Ag electrode, with field strengths on the order of ~1 V nm -1 shifting a voltage-dependent nitrile response up to ~4 cm -1 /V at negative applied potential. By applying a bias of ±1 V at 180°C, the device both increases and decreases the catalytic turnover frequency of CO oxidation. These results support surface-charge modulation as the origin of catalytic rate enhancement for the non-Faradaic dynamic tuning of thermochemical reaction rates.

Source: ChemRxiv

DOI: 10.26434/chemrxiv.15009022/v1