Asymmetric Porous Catalyst Structures for Low-Temperature Photocatalytic Dry Reforming of Methane
Recent advances in the photocatalytic activation of dry reforming of methane (DRM: CO<sub>2</sub> + CH<sub>4</sub> → 2CO + 2H<sub>2</sub>) at low temperature and ambient pressure have generated considerable interest as a promising route to convert greenhouse gases into valuable synthetic gas (syngas). While detailed studies have revealed the mechanisms involved in photocatalytic DRM at metal-semiconductor interfaces, less attention has been devoted to how high-surface-area semiconductor supports may enhance such conversions. Here, we structure triblock terpolymer self-assembly directed sol-gel-derived transition metal oxide (Ta<sub>2</sub>O<sub>5</sub> or TiO<sub>2</sub>) supports of Rh-loaded photocatalysts into various equilibrium and nonequilibrium derived porous morphologies and show how they modulate single-pass conversion, total production rate, and material efficiency. Supported by in-depth materials characterization, flow, and optics simulations rationalizing observed trends, results reveal record catalyst performance. Our work suggests that asymmetric pore structures simultaneously optimizing mass transport and surface area may be well-suited to maximize photocatalyst performance.
Authors
- Kahyun Hur (ORCID: https://orcid.org/0000-0002-5563-3986)
- Austin Jerad Reese (ORCID: https://orcid.org/0000-0003-1107-0349)
- Aniruddha Saha (ORCID: https://orcid.org/0000-0002-4417-1894)
- R. Paxton Thedford (ORCID: https://orcid.org/0000-0003-0811-227X)
- Sarah A. Hesse (ORCID: https://orcid.org/0000-0002-2383-4476)
- Sadaf Sobhani (ORCID: https://orcid.org/0000-0002-7088-7773)
- Shusaku Shoji (ORCID: https://orcid.org/0000-0002-8481-2633)
- Lieihn Tsaur (ORCID: https://orcid.org/0000-0002-7120-8453)
- Ali Y. Kozbek (ORCID: https://orcid.org/0000-0002-6224-7012)
- William R. T. Tait (ORCID: https://orcid.org/0000-0001-8932-9416)
- William Moore (ORCID: https://orcid.org/0000-0002-0407-5347)
- Lilit Yeghiazarian (ORCID: https://orcid.org/0000-0002-7521-1545)
- Sol M. Grüner (ORCID: https://orcid.org/0000-0002-1171-4426)
- Jin Suntivich
- Ulrich Wiesner (ORCID: https://orcid.org/0000-0001-6934-3755)
- M. Sadegh Riasi (ORCID: https://orcid.org/0000-0003-2616-8373)
- Fei Yu (ORCID: https://orcid.org/0000-0002-8191-8096)
Institutions
- National Institute for Materials Science (JP)
- Cornell University (US)
- Smith Institute (GB)
- Sibley Memorial Hospital (US)
- Korea Institute of Science and Technology (KR)
- University of Cincinnati (US)
Publication Details
- Journal
- ACS Nano
- Published
- 2025-06-24
- DOI
- https://doi.org/10.1021/acsnano.5c04286
- Citations
- 3
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 1.55
Funders
- Kavli Institute at Cornell, Cornell University
- Japan Society for the Promotion of Science
- Division of Materials Research
- Division of Chemical, Bioengineering, Environmental, and Transport Systems
- Division of Chemistry