Synergy between photon-to-phonon pathway and active lattice oxygen enables efficient and stable syngas synthesis

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Guo, Chengzhi and Jain, Apoorv and Feng, Junrun and Li, Xinyu and Li, Xinru and Jia, Shuya and Wang, Juncong and Chen, Leirun and Luo, Xinjie and Zhang, Xiaolei and Li, Xiyi and Lan, Yang (2026) Synergy between photon-to-phonon pathway and active lattice oxygen enables efficient and stable syngas synthesis. Angewandte Chemie. e9236832. ISSN 1521-3757 (https://doi.org/10.1002/ange.9236832)

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Abstract

Light-driven dry reforming of methane (DRM) offers a promising route for syngas synthesis while simultaneously mitigating greenhouse gas emissions of CO2 and CH4. However, the attractive mild-temperature operating window imposes kinetic constraints on C─H/C═O activation and promotes thermodynamic tendencies for coke formation, resulting in limited efficiency and stability. Herein, manganese oxide (MnOx) is employed as a multifunctional support to integrate the classic Rh catalytic center, establishing a new benchmark photothermo catalyst for DRM. The system achieves record-high syngas production rates (H2: 948 mmol g−1 h−1; CO: 992 mmol g−1 h−1) without external heating, alongside exceptional long-term stability (∼500 h). These production rates and stability also surpass conventional thermocatalysts in similar temperature ranges, with stability exceeding most thermocatalysts by an order of magnitude. Under a separate low-conversion, high-gas hourly space velocity (GHSV) protocol, a light-to-chemical efficiency (29.5%) can also be reached. MnOx functions as a broadband light harvester, generating a localized thermal field at the micrometre-scale via an efficient photon-to-phonon pathway to facilitate C─H bond activation on Rh. Concurrently, its active lattice oxygen enables a dynamic OL-OV cycle for timely removal of C* intermediates and C═O activation. This work underscores the critical role of support engineering in advancing light-driven DRM.

ORCID iDs

Guo, Chengzhi, Jain, Apoorv ORCID logoORCID: https://orcid.org/0009-0001-7057-3264, Feng, Junrun, Li, Xinyu, Li, Xinru, Jia, Shuya ORCID logoORCID: https://orcid.org/0009-0002-7768-9099, Wang, Juncong, Chen, Leirun, Luo, Xinjie, Zhang, Xiaolei ORCID logoORCID: https://orcid.org/0000-0001-9415-3136, Li, Xiyi and Lan, Yang;
CORE (COnnecting REpositories)