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On the mechanism of visible-light accelerated methane dry reforming reaction over Ni/CeO2−x catalysts
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2021-09-22 , DOI: 10.1016/j.apcatb.2021.120745
Kristijan Lorber 1, 2 , Janez Zavašnik 3 , Jordi Sancho-Parramon 4 , Matej Bubaš 4 , Matjaž Mazaj 1 , Petar Djinović 1, 2
Affiliation  

The methane dry reforming reaction (DRM) converts methane and CO2 into syngas, a mixture of H2 and CO. When illuminated by 790 mW cm−2 of white light, the 2Ni/CeO2−x catalyst converts CH4 and CO2 beyond thermodynamic equilibrium, while the energy efficiency reaches 33%. The DRM reaction is sustained in a purely photocatalytic mode without external heating, yielding CH4 and CO2 rates of 0.21 and 0.75 mmol (gcat • min)−1, respectively. Theoretical analysis of Ni/CeO2−x optical properties agrees with in-situ UV-Vis DRS results and reveals partly reduced Ce3+ sites crucial for extending the optical absorption of Ni/CeO2−x into the visible light range. Two photocatalytic mechanisms are postulated to occur: the hot charge-carrier driven photocatalytic mechanism and the near-field induced resonant energy transfer, depending on the energy of photons used to stimulate the catalyst. This work identifies sub-stoichiometric Ni/CeO2−x as highly efficient for boosting methane activation by visible light under mild conditions.



中文翻译:

Ni/CeO2-x催化剂上可见光加速甲烷干重整反应机理

甲烷干重整反应 (DRM) 将甲烷和 CO 2转化为合成气,即 H 2和 CO的混合物。当被 790 mW cm -2白光照射时,2Ni/CeO 2-x催化剂将 CH 4和 CO 2转化超出热力学平衡,而能量效率达到33%。DRM 反应以纯光催化模式持续,无需外部加热,CH 4和CO 2 的速率分别为0.21 和0.75 mmol (g cat • min) -1。Ni/CeO 2-x光学性质的理论分析与原位一致UV-Vis DRS 结果显示部分减少的 Ce 3+位点对于将 Ni/CeO 2-x的光吸收扩展到可见光范围至关重要。假设发生两种光催化机制:热电荷载流子驱动的光催化机制和近场诱导的共振能量转移,这取决于用于刺激催化剂的光子能量。这项工作将亚化学计量的 Ni/CeO 2-x鉴定为在温和条件下通过可见光促进甲烷活化的高效方法。

更新日期:2021-10-07
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