发布时间：

2026-06-15

论文名称：

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

发表刊物：

Small

关键字：

Dry reforming of methane; Interfacial vacancy engineering; Carbon-resistant; Photothermal synergistic catalysis; Interfacial sites

摘要：

High-temperature carbon deposition remains the primary challenge in the dry reforming of methane (DRM). This issue is fundamentally caused by the insufficient generation and slow migration of reactive oxygen species. Combining interfacial vacancy engineering with photothermal synergistic catalysis is a promising solution, yet their synergistic mechanism remains unclear. Here, we used a simple alkaline etching strategy to construct stable Niδ+–Ov–Al interfacial sites on a NiMgAl-A catalyst. This approach improved nickel dispersion and drove continuous electron transfer from Ni to the support. In situ characterization and theoretical calculations revealed a dual role for these interfacial sites: they act as intrinsic active centers for CH4 and CO2 activation, while also functioning as “interfacial electron traps” to boost charge separation under illumination. Consequently, photogenerated carriers accelerate the formation of reactive oxygen species. This rapid oxygen supply promotes the direct conversion of CH4 and CO2 into CHxO* intermediates, drastically reducing the coking rate. Photothermal tests at 600 °C confirmed the powerful synergy between photoelectrons and the Niδ+–Ov–Al sites. Compared to the pristine NiMgAl catalyst, NiMgAl-A achieved a 1.55-fold increase in CH4 conversion rate and a 1.61-fold increase in CO2 conversion rate. Most notably, the carbon deposition rate plunged from 0.57 g·h-1 to just 0.12 g·h-1. This work clarifies the dynamic synergy between oxygen vacancies and photoelectrons, offering a clear pathway for designing highly efficient, carbon-resistant catalysts.

合写作者：

Xu Liu,Tengfei Li,Juntao Li,Pengjie Miao

第一作者：

Yuhao Liu

通讯作者：

Yang Guo

文献类型：

J

是否译文：

否

发表时间：

2026-06-12

收录刊物：

SCI