Abstract
The electrochemical reduction of carbon dioxide to formic acid is a promising pathway to improve CO2 utilization and has potential applications as a hydrogen storage medium. In this work, a zero-gap membrane electrode assembly architecture is developed for the direct electrochemical synthesis of formic acid from carbon dioxide. The key technological advancement is a perforated cation exchange membrane, which, when utilized in a forward bias bipolar membrane configuration, allows formic acid generated at the membrane interface to exit through the anode flow field at concentrations up to 0.25 M. Having no additional interlayer components between the anode and cathode this concept is positioned to leverage currently available materials and stack designs ubiquitous in fuel cell and H2 electrolysis, enabling a more rapid transition to scale and commercialization. The perforated cation exchange membrane configuration can achieve >75% Faradaic efficiency to formic acid at <2 V and 300 mA/cm2 in a 25 cm2 cell. More critically, a 55-hour stability test at 200 mA/cm2 shows stable Faradaic efficiency and cell voltage. Technoeconomic analysis is utilized to illustrate a path towards achieving cost parity with current formic acid production methods.
| Original language | English |
|---|---|
| Article number | 7605 |
| Journal | Nature Communications |
| Volume | 14 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 2023 |
Funding
This work was funded by the Bio Energy Technology Office, authored in part by Alliance for Sustainable Energy, LLC, the manager, and operator of the National Renewable Energy Laboratory for the U.S. Department of Energy (DOE) under Contract No. DE-AC36-08GO28308. The research was supported by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office, under contract DE-AC02-06CH11357 (Argonne National Laboratory). Neither the U.S. Government nor any agency thereof, nor any of their employees or employees of contributing companies, makes any warranty, expressed or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. This work was authored in part by Argonne National Laboratory, a DOE, Office of Science Laboratory operated under Contract No. DE-AC02-06CH11357 by UChicago, Argonne, LLC. The X-ray spectroscopy experiments were performed at beamline 10-ID at the APS, which is operated by the Materials Research Collaborative Access Team (MRCAT). MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. The APS is a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The authors would like to thank Joshua Wright of 10-ID. The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for U.S. Government purposes. This work was funded by the Bio Energy Technology Office, authored in part by Alliance for Sustainable Energy, LLC, the manager, and operator of the National Renewable Energy Laboratory for the U.S. Department of Energy (DOE) under Contract No. DE-AC36-08GO28308. The research was supported by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office, under contract DE-AC02-06CH11357 (Argonne National Laboratory). Neither the U.S. Government nor any agency thereof, nor any of their employees or employees of contributing companies, makes any warranty, expressed or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. This work was authored in part by Argonne National Laboratory, a DOE, Office of Science Laboratory operated under Contract No. DE-AC02-06CH11357 by UChicago, Argonne, LLC. The X-ray spectroscopy experiments were performed at beamline 10-ID at the APS, which is operated by the Materials Research Collaborative Access Team (MRCAT). MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. The APS is a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The authors would like to thank Joshua Wright of 10-ID. The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for U.S. Government purposes.