Photocatalytic Dry Reforming of Methane Enhanced by “Dual‐Path” Strategy with Excellent Low‐Temperature Catalytic Performance
Wei Zhou, Binghao Wang, Long Tang, Lang Chen, Jun‐Kang Guo, Jinbo Pan, Ben Lei, Biao Hu, Zhangjun Bai, Mengistu Tulu, Zong‐Xu Li, Xiong Wang, Chak‐Tong Au, Shuang‐Feng Yin
Abstract
Abstract Dry reforming of methane (DRM), which involves the activation of inert CH bonds and CO 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‐C 3 N 4 nanosheets” and “Pd‐nanoparticle‐loaded boron‐doped nitrogen‐deficient g‐C 3 N 4 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 CO 2 and CH 4 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 H 2 /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.