CO <sub>2</sub> Conversion to Butene via a Tandem Photovoltaic–Electrochemical/Photothermocatalytic Process: A Co-design Approach to Coupled Microenvironments
We developed a tandem, unassisted, solar-driven electrochemical and photothermocatalytic process for the single-pass conversion of CO2 to butene using only simulated solar irradiation as the energetic input. The two-step process involves electrochemical CO2 reduction (CO2R) to ethylene followed by ethylene dimerization to butene. We assessed two unassisted electrochemical setups to concentrate ethylene in the CO2R reactor, achieving concentrations up to 5.4 vol% with 1.8% average solar-to-ethylene conversion and 5.6% average CO2-to-ethylene single-pass conversion under 1-sun illumination. When the effluent electrochemical gas stream was passed through the photothermocatalytic ethylene oligomerization reactor, we generated 600 ppm of butene under 3-sun illumination. Through analysis of this process, we identified that the presence of H2, CO, and H2O leads to rapid deactivation of the Ni-based ethylene oligomerization catalyst.
Authors
- Matthew Salazar
- Theodor Agapie (ORCID: https://orcid.org/0000-0002-9692-7614)
- Aisulu Aitbekova (ORCID: https://orcid.org/0000-0003-3309-1220)
- Kyra M. K. Yap (ORCID: https://orcid.org/0000-0001-8861-993X)
- Adam C. Nielander (ORCID: https://orcid.org/0000-0002-3639-2427)
- Jonas C. Peters (ORCID: https://orcid.org/0000-0002-6610-4414)
- Tobias A. Kistler (ORCID: https://orcid.org/0000-0001-6458-8024)
- Adam Z. Weber (ORCID: https://orcid.org/0000-0002-7749-1624)
- Thomas Francisco Jaramillo (ORCID: https://orcid.org/0000-0001-9900-0622)
- Nicholas B. Watkins (ORCID: https://orcid.org/0000-0001-7251-9387)
- Peter Agbo (ORCID: https://orcid.org/0000-0003-3066-4791)
- Harry Albert Atwater (ORCID: https://orcid.org/0000-0001-9435-0201)
- Magel P. Su (ORCID: https://orcid.org/0000-0003-4898-5024)
- Alexis T. Bell (ORCID: https://orcid.org/0000-0002-5738-4645)
- Melanie Rodríguez Pabón (ORCID: https://orcid.org/0009-0007-8350-1706)
- Sang‐Won Lee (ORCID: https://orcid.org/0000-0001-6860-938X)
Institutions
- California Institute of Technology (US)
- nLIGHT (United States) (US)
- Lawrence Berkeley National Laboratory (US)
- SLAC National Accelerator Laboratory (US)
- University of California, Berkeley (US)
- Stanford University (US)
Publication Details
- Journal
- ACS Energy Letters
- Published
- 2024-08-15
- DOI
- https://doi.org/10.1021/acsenergylett.4c01866
- Citations
- 10
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 1.02
Funders
- Chevron
- Stanford University
- Kavli Nanoscience Institute, California Institute of Technology
- Division of Electrical, Communications and Cyber Systems
- Basic Energy Sciences