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rGO supported PdNi-CeO2 nanocomposite as an efficient catalyst for hydrogen evolution from the hydrolysis of NH3BH3
Authors:Ying-Hua Zhou  Zhiyan Zhang  Suqin Wang  Nicholas Williams  Yong Cheng  Shizhong Luo  Jing Gu
Affiliation:1. The Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Laboratory of Molecule-Based Materials (State Key Laboratory Cultivation Base), College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241000, PR China;2. Department of Chemistry and Biochemistry, San Diego State University, San Diego, CA, 92182-1030, USA
Abstract:The hydrogen economy is a proposed system that utilizes hydrogen to deliver energy. For the realization of this concept, how to safely, controllably and reversibly store and release hydrogen are critical problems which must be resolved. Metal alloys combined with suitable support materials are widely applied to various catalytic reactions. Here palladium nickel bimetallic nanoparticles doped with cerium oxide on a reduced graphene oxide (rGO) support were prepared by combining metal ion precursors and graphene oxide in a one-pot co-reduction approach. The as-received catalysts were characterized by XRD, TEM, SEM, XPS and ICP-OES, and the results revealed that PdNi-CeO2 nanoparticles were uniform dispersal on rGO. The as-synthesized PdNi-CeO2/rGO had been adopted as a heterogeneous catalyst for the hydrogen evolution from the hydrolysis of ammonia borane (NH3BH3, AB) at room temperature. Kinetically, the hydrogen-release rate was first-order with the increased concentration of catalysts. The optimized catalyst of Pd0.8Ni0.2-CeO2/rGO with the CeO2 content of 13.9 mol% exhibited an excellent activity with a turnover frequency value of 30.5 mol H2 (mol catalyst)?1 min?1 at 298 K, and a low apparent activation energy (Ea) of 37.78 kJ mol?1. The robust catalytic performance of the Pd0.8Ni0.2-CeO2/rGO is attributed to the uniform controlled nanoparticle size, the synergic effect between the nanoparticles bimetallic properties, and the effective charge transfer interactions between the metal and support.
Keywords:Hydrogen storage  Heterogeneous catalysis  Ammonia borane  Graphene  Synergistic effect
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