Asymmetric porous catalyst structures for low temperature photocatalytic dry reforming of methane

William Moore; Shusaku Shoji; Lieihn Tsaur; Fei Yu; R. Paxton Thedford; William R. Tait; M. Sadegh Riasi; Aniruddha Saha; Kayhun Hur; Austin Reese; Ali Y. Kozbek; Sarah Hesse; Sol M. Gruner; Lilit Yeghiazarian; Sadaf Sobhani; Jin Suntivich; Ulrich B. Wiesner

doi:10.1021/acsnano.5c04286

Journal article Asymmetric porous catalyst structures for low temperature photocatalytic dry reforming of methane

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William Moore, Shusaku Shoji, Lieihn Tsaur, Fei Yu, R. Paxton Thedford, William R. Tait, M. Sadegh Riasi, Aniruddha Saha, Kayhun Hur, Austin Reese, Ali Y. Kozbek, Sarah Hesse, Sol M. Gruner, Lilit Yeghiazarian, Sadaf Sobhani, Jin Suntivich, Ulrich B. Wiesner. Asymmetric porous catalyst structures for low temperature photocatalytic dry reforming of methane. ACS NANO. 2025, (), . https://doi.org/10.1021/acsnano.5c04286

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Recent advances in the photocatalytic activation of dry reforming of methane (DRM: CO2 + CH4 → 2CO + 2H2) 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 (Ta2O5 or TiO2) supports of Rh-decorated photocatalysts into various equilibrium and non-equilibrium derived porous morphologies and show how they modulate single-pass conversion, total production rate, and material efficiency. Supported by in-depth materials characterization and flow 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.

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This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Nano, copyright © 2025 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsnano.5c04286.

Keyword: dry reforming of methane, block copolymer, photocatalyst, self-assembly, hydrogen production, porous asymmetric membrane

Date published: 2025-07-08

Publisher: ACS Publications

Journal:

ACS NANO (ISSN: 19360851)

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Manuscript type: Author's version (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.5549

First published URL: https://doi.org/10.1021/acsnano.5c04286

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Updated at: 2025-06-26 14:18:00 +0900

Published on MDR: 2026-06-24 08:32:56 +0900

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