Resolving the Activity-Stability Trade-Off in Methane Dry Reforming via Ru-Preferential CH₄ Activation on Isolated Ni-Ru Dual Sites.

Authors

Jingyi Wang, Ming Li, Min Liu, Xingmin Liu, Guofei Xia, Zhan Gao

Published in

Small (Weinheim an der Bergstrasse, Germany). Pages e75232. Aug 12, 2026. Epub Aug 12, 2026.

Abstract

Dry reforming of methane, the endothermic co-conversion of CH₄ and CO₂ into syngas (H₂/CO), is typically limited by low-temperature activity and carbon-induced deactivation at high temperatures. Here, a geometrically isolated dual-site architecture is established by co-anchoring Ni and Ru atomic sites on defect-rich CeO₂. The optimized 1NiRu/CeO₂ catalyst achieves CH₄/CO₂ conversions of 21.46%/24.10% and a H₂/CO ratio of 0.91 at 500°C, and approaches equilibrium (86.77%/92.78%) at 750°C. 1NiRu/CeO₂ demonstrates outstanding stability over 150 h, with negligible carbon deposition compared to 1Ru/CeO₂. Operando spectroscopy and theoretical calculations reveal preferential CH₄ activation at Ru sites in the isolated Ni-Ru dual-site structure. The Ru^δ+-O_v-Ce³⁺ interfacial sites preferentially dissociate CH₄ into CH₃ ^* species that are further oxidized to CH₃O^* via a low-barrier, lattice oxygen-mediated pathway, while Ni^δ+-O_v-Ce³⁺ sites readily activate CO₂ and replenish O_lattice. This oxidative pathway effectively suppresses CH_x deep dehydrogenation and, coupled with Ni-driven CO₂ activation, establishes a self-sustaining O_lattice/O_v redox cycle. This synergistic cycle enables a site-selective division of labour for CH₄/CO₂ activation, thereby maintaining coke-resistant activity across 400°C-750°C. This work establishes a generalizable strategy for isolated dual-site catalyst design, where Ru-preferential CH₄ activation and vacancy-governed interfacial cooperation orchestrate low-temperature activity, stability, and coke resistance, enabling efficient and durable CH₄/CO₂ valorization via dry reforming.

PMID:
42590891
Bibliographic data and abstract were imported from PubMed on 13 Aug 2026.

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