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Single Atom Catalysis Enables Preferential Middle-Ring Dehydrogenation of Perhydro-Dibenzyltoluene for
Ligang Zhang1,2, Fan Wang1, Hongchen Cao3
1State Key Laboratory of Mesoscience and Process Engineering, Beijing Key Laboratory of Ionic Liquids Clean Process, Institute of Process Engineering, Chinese Academy of Sciences, Innovation Academy for Green Manufacture, Chinese Academy of Sciences, Beijing, China.
Abstract:
Hydrogen (H2) storage/release using dibenzyltoluene/perhydro-dibenzyltoluene (DBT/H18-DBT) provides a safe route for H2 transportation but suffers from high dehydrogenation temperature due to the large C-H dissociation energy of the H18-DBT side rings. In this work, we design a single Pt atom catalyst with well controlled Pt-O coordination number (CNPt-O). The Pt single atom catalyst (SAC) with CNPt-O ≈ 4 on the step site of CeO2 results in a unique reaction mechanism of preferential dehydrogenation of the H18-DBT middle ring, enabling H2 production from H18-DBT at 200°C - a temperature far below those reported in the literature (≥ 260°C), which achieves a 7 times higher H2 evolution rate ( ) of 83430.0 molH2 molPt -1 h-1 at 300°C as compared to the published values with stable H18-DBT conversion of ∼90% during 50 repeated hydrogen storage/release cycles.
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