CO2 Conversion to Butene via a Tandem Photovoltaic–Electrochemical/Photothermocatalytic Process: A Co-design Approach to Coupled Microenvironments

Yap, Kyra M. K.; Aitbekova, Aisulu; Salazar, Matthew; Kistler, Tobias A.; Rodríguez Pabón, Melanie; Su, Magel P.; Watkins, Nicholas B.; Lee, Sang-Won; Agbo, Peter; Weber, Adam Z.; Peters, Jonas C.; Agapie, Theodor; Nielander, Adam C.; Atwater, Harry A.; Jaramillo, Thomas F.; Bell, Alexis T.

doi:10.1021/acsenergylett.4c01866

CO₂ Conversion to Butene via a Tandem Photovoltaic–Electrochemical/Photothermocatalytic Process: A Co-design Approach to Coupled Microenvironments

Journal Article · Thu Aug 15 00:00:00 EDT 2024 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.4c01866· OSTI ID:2441454

^[1]; ^[2]; Salazar, Matthew ^[2]; ^[3]; ^[4]; ^[2]; ^[2]; Lee, Sang-Won ^[5]; ^[3]; ^[3]; Peters, Jonas C. ^[2]; ^[2]; ^[6]; ^[2]; ^[5]; ^[7]

SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis; Stanford Univ., CA (United States); California Institute of Technology (CalTech), Pasadena, CA (United States); SLAC
California Institute of Technology (CalTech), Pasadena, CA (United States)
California Institute of Technology (CalTech), Pasadena, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Stanford Univ., CA (United States); California Institute of Technology (CalTech), Pasadena, CA (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis; Stanford Univ., CA (United States); California Institute of Technology (CalTech), Pasadena, CA (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis; California Institute of Technology (CalTech), Pasadena, CA (United States)
California Institute of Technology (CalTech), Pasadena, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)

Here, 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 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.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515; SC0021266

OSTI ID:: 2441454

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 9 Vol. 9; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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