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Experimental and Theoretical Studies of Ultrafine Pd-Based Biochar Catalyst for Dehydrogenation of Formic Acid and
Liangyu Zou1, Qi Liu1, Daoyun Zhu1
1Joint International Center for Carbon-Dioxide Capture and Storage (iCCS), Advanced Catalytic Engineering Research Center of the Ministry of Education, Provincial Hunan Key Laboratory for Cost-Effective Utilization of Fossil Fuel Aimed at Reducing Carbon-Dioxide Emissions, College of Chemistry and Chemical Engineering, Hunan University, Changsha, Hunan 410082, PR China.
Abstract:
In this work, a novel "foaming" strategy uses sodium bicarbonate (NaHCO3) and ammonium oxalate ((NH4)2C2O4) as the foaming agent, turning biomass-derived carboxymethyl cellulose (CMC) into N-doped porous carbon. Highly active palladium nanoparticles (Pd NPs) immobilized on nitrogen-doped porous carbon (Pd@MC(2)-P) are produced through a phosphate-mediation approach. The phosphoric acid (H3PO4) becomes the key to the synthesis of highly dispersed ultrafine Pd NPs on active Pd-cluster-edge (the edge of the Pd-cluster-100 and Pd-cluster-111 surfaces). The Pd@MC(2)-P exhibits high activity for formic acid (FA) dehydrogenation with an initial TOFg of 971 h-1 at room temperature. The subsequent hydrogenation of phenol using FA as an in situ hydrogen source on Pd@MC(2)-P and the highly efficient hydrogenation of phenol to cyclohexanone reaches more than 90% selectivity and 80% conversion. Density functional theory (DFT) calculations reveal that the reduced H poisoning and more exposed (100) surface over Pd nanoparticles are the keys to the Pd nanoparticles' high activity.
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