Details

Autor(en) / Beteiligte

• Zhou, Wei
• Wang, Bing‐Hao
• Tang, Long
• Chen, Lang
• Guo, Jun‐Kang
• Pan, Jin‐Bo
• Lei, Ben
• Hu, Biao
• Bai, Zhang‐Jun
• Tulu, Mengistu
• Li, Zong‐Xu
• Wang, Xiong
• Au, Chak‐Tong
• Yin, Shuang‐Feng

Titel

Photocatalytic Dry Reforming of Methane Enhanced by “Dual‐Path” Strategy with Excellent Low‐Temperature Catalytic Performance

Ist Teil von

• Advanced functional materials, 2023-07, Vol.33 (27), p.n/a

Ort / Verlag

Hoboken: Wiley Subscription Services, Inc

Erscheinungsjahr

2023

Quelle

Wiley Online Library

Beschreibungen/Notizen

• Dry reforming of methane (DRM), which involves the activation of inert CH bonds and CO bonds, at mild conditions is a tremendous challenge. The sluggish mobility of oxygen during the reaction is known as a key issue causing low activity and poor stability of catalysts by the coke formation. Herein, a novel Cu‐CNN/Pd‐BDCNN photocatalyst that is made up of “Cu‐nanoparticle‐loaded g‐C3N4 nanosheets” and “Pd‐nanoparticle‐loaded boron‐doped nitrogen‐deficient g‐C3N4 nanosheets” is reported. The existing dual‐reaction‐sites benefit the reactive oxygen intermediates participate in the reaction directly without distant migration. The in situ characterizations and density functional theory calculations reveal a newly dual reaction pathway through simultaneous dehydrogenation of methoxy and methyl intermediates, and demonstrate the importance of metal loading, which promote the CO2 and CH4 activation from both aspects of thermodynamics and kinetics. The optimized Cu‐CNN/Pd‐BDCNN photocatalyst displays an excellent syngas formation rate of over 800 µmol g−1 h−1 with H2/CO = 1 and splendid stability in continuous flow reaction under 300 mW cm−2 xenon lamp irradiation at room temperature. The “dual‐site” and “dual‐path” strategy shed light on the design of effective photocatalysts for methane dry reforming. Dry reforming of methane (DRM) reaction occurs at two sites and presents two reaction pathways over the catalyst. The dual‐reaction‐site and dual‐path process not only achieves high catalytic activity, stability and syngas selectivity, but also overcomes the problems arising from poor oxygen migration on non‐oxygen‐containing catalysts. The strategy of dual reaction sites provides mechanistic insights for rational design of DRM catalysts.