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PreprintCC BY-NC-NDChemRxiv

Programmable Oxidation in Flow on Interdigitated Lateral Catalytic Condensers

  • Ruixue Xiong1,2
  • Wonwoo Lee1,2
  • Chaehoon Kim1,2
  • Justin Hopkins1,2
  • Jesse Canavan1,2
  • Jaeheon Kim1,2
  • Susannah Scott1,3
  • Dan McDonald1,2
  • Matt Neurock1,2
  • Omar Abdelrahman1,4
  • C. Daniel Frisbie1,2
  • Paul Dauenhauer1,2
4 affiliations
  1. 1Center for Programmable Energy Catalysis, University of Minnesota, 421 Washington Ave. SE, Minneapolis, MN, USA, 55455
  2. 2Department of Chemical Engineering & Materials Science, University of Minnesota, 421 Washington Ave. SE, Minneapolis, MN, USA, 55455
  3. 3Department of Chemical Engineering, University of California Santa Barbara, Engineering II Building, Santa Barbara, CA, USA, 93106-5080
  4. 4Department of Chemical Engineering, University of Houston, 4726 Calhoun Road, Houston, TX, USA, 77204
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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.

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Cite

BibTeXRIS
BibTeX
@misc{xiong2026programmable,
  title = {{Programmable Oxidation in Flow on Interdigitated Lateral Catalytic Condensers}},
  author = {Ruixue Xiong and Wonwoo Lee and Chaehoon Kim and Justin Hopkins and Jesse Canavan and Jaeheon Kim and Susannah Scott and Dan McDonald and Matt Neurock and Omar Abdelrahman and C. Daniel Frisbie and Paul Dauenhauer},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv.15009022/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009022/v1},
  note = {CC BY-NC-ND},
}
RIS
TY  - UNPB
TI  - Programmable Oxidation in Flow on Interdigitated Lateral Catalytic Condensers
AU  - Ruixue Xiong
AU  - Wonwoo Lee
AU  - Chaehoon Kim
AU  - Justin Hopkins
AU  - Jesse Canavan
AU  - Jaeheon Kim
AU  - Susannah Scott
AU  - Dan McDonald
AU  - Matt Neurock
AU  - Omar Abdelrahman
AU  - C. Daniel Frisbie
AU  - Paul Dauenhauer
PY  - 2026
DA  - 2026/09/17
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15009022/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009022/v1
AB  - 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.
ER  -