Mechanistic insights into NO‒H2 reaction over Pt/boron-doped graphene catalyst
Zhenhua Yao1, Lei Li2, Xuguang Liu3
1Hubei Key Laboratory of Industrial Fume and Dust Pollution Control, and Key Laboratory of Optoelectronic Chemical Materials and Devices of Ministry of Education, Jianghan University, Wuhan 430056, China.
Abstract:
This work presents a systematical experimental and density functional theory (DFT) studies to reveal the mechanism of NO reduction by H2 reaction over platinum nanoparticles (NPs) deposited on boron-doped graphene (denoted as Pt/BG) catalyst. Both characterizations and DFT calculations identified boron (in Pt/BG) as an additional NO adsorption site other than the widely recognized Pt NPs. Moreover, BG led to a decrease of Pt NPs size in Pt/BG, which facilitated hydrogen spillover. The mathematical and physical criteria of the Langmuir-Hinshelwood dual-site kinetic model over the Pt/BG were satisfied, indicating that adsorbed NO on boron (in Pt/BG) was further activated by H-spillover. On the other hand, Pt/graphene (Pt/Gr) demonstrated a typical Langmuir-Hinshelwood single-site mechanism where Pt NPs solely served as active sites for NO adsorption. This work helps understand NO-H2 reaction over Pt/BG and Pt/Gr catalysts in a closely mechanistic view and provides new insights into roles of active sites for improving the design of catalysts for NO abatement.
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