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Photothermal Steering of the CH4─CO2 Coupling Pathway and Coke-Suppression Mechanism by Niδ+─Ov─Al Interfacial Sites.

Created on 24 Jun 2026

Authors

Yuhao Liu, Xu Liu, Tengfei Li, Juntao Li, Pengjie Miao, Yang Guo

Published in

Small (Weinheim an der Bergstrasse, Germany). Pages e74304. Jun 24, 2026. Epub Jun 24, 2026.

Abstract

High-temperature carbon deposition is a major challenge in dry reforming of methane (DRM), mainly arising from insufficient generation and sluggish migration of reactive oxygen species. Combining interfacial vacancy engineering with photothermal synergistic catalysis is a promising solution, yet their synergistic mechanism remains unclear. Here, a simple alkaline etching strategy was employed to construct stable Niδ+-Ov-Al interfacial sites on a NiMgAl-A catalyst. These sites enhanced Ni dispersion and promoted continuous electron transfer from Ni to the support. In situ characterization and theoretical calculations revealed that Niδ+-Ov-Al sites serve as both intrinsic active centers for CH4/CO2 activation and interfacial electron traps that improve charge separation under illumination. As a result, photogenerated carriers accelerate reactive oxygen species formation, facilitating the direct conversion of CH4 and CO2 into CHxO* intermediates and effectively suppressing coke formation. Photothermal DRM tests at 600°C demonstrated strong synergy between photoelectrons and Niδ+-Ov-Al sites. Compared with pristine NiMgAl, NiMgAl-A increased CH4 and CO2 conversion rates by 1.55 and 1.61 times, respectively, while reducing the carbon deposition rate from 0.57 to 0.12 g·h-1. This work provides mechanistic insight into oxygen-vacancy/photoelectron synergy for designing efficient carbon-resistant DRM catalysts.

PMID:
42339556
Bibliographic data and abstract were imported from PubMed on 24 Jun 2026.

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