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Hydrogen Assisted Synthesis of Branched Nickel Nanostructures: A Combined Theoretical and Experimental Study

Abstract

The selective adsorption of small molecules over specific facets plays an important role in morphology controlled synthesis of metal nanocrystals. In the present work, hydrogen is found to be a good capping agent for direct synthesis of branched nickel nanocrystals, i.e., secondary branching (Ni-SB) nanoparticles and multipods (Ni-MP). Using ab initio thermodynamics and Wulff construction principle, it had been found that: (i) in the presence of hydrogen (PH2=6 bar), the facet structure stability follows the order of Ni(100) > Ni(111) > Ni(110), resulting in competitive over-growth along <111> and <110> directions; (ii) with increasing hydrogen pressure, the Ni deposition rate over the crystal surface increases as the result of more Ni2+ reduction; the competition between deposition and surface diffusion, therefore, becomes the vital factor for the nanocrystal growth process; (iii) the diffusion energy barrier of a surface Ni atom on Ni(111) is lower than it on Ni(110), especially on hydrogen covered surfaces, indicating that the kinetic over-growth only along <111> direction producing Ni-MP will be dominant under PH2=14 bar; (iv) ab initio based Wulff construction principle predicts the shapes and morphologies at different hydrogen pressures are further confirmed with HRTEM results. Finally, compared with synthesized nickel nanoparticles (Ni-NP) in the absence of hydrogen, the hydrogen assisted branched Ni nanomaterials, especially the Ni-MP, shows higher catalytic activities for hydrogenation reactions of acetophenone and nitrobenzene.

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Publication details

The article was received on 11 Jul 2017, accepted on 07 Sep 2017 and first published on 08 Sep 2017


Article type: Paper
DOI: 10.1039/C7CP04673A
Citation: Phys. Chem. Chem. Phys., 2017, Accepted Manuscript
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    Hydrogen Assisted Synthesis of Branched Nickel Nanostructures: A Combined Theoretical and Experimental Study

    X. Liang, N. Liu, H. Qiu, C. Zhang, D. Mei and B. Chen, Phys. Chem. Chem. Phys., 2017, Accepted Manuscript , DOI: 10.1039/C7CP04673A

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