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Enhanced Electron Transfer and Light Absorption on an Imino Polymer Capped PdAg Nanowire Networks for Efficient Room-Temperature Dehydrogenation of Formic Acid

Abstract

The electron structure tuning of heterogeneous nanocatalysts is considered as one of most effective ways in enhancing the catalytic activity of different chemical reactions. Herein, we demonstrate an effective way for tuning the electron structure of networked PdAg nanowires (NWs) using the polyvinylpyrrolidine imine (PVPI) as a new ligand to achieve more efficient hydrogen generation from formic acid (FA) decomposition. The PVPI-capped Pd5Ag5 NWs show the highest activity for the dehydrogenation catalysis of FA with an initial turnover of turnover frequency (TOF) of 242 h-1 in all the reported catalysts, and an increased TOF of 312 h-1 under 365 nm light irradiation at room temperature. The X-ray photoelectron spectroscopy and Fourier Infrared studies reveal there is an interfacial electron transfer from PVPI to PdAg NWs surface, which is the key factor in boosting the dehydrogenation catalysis of FA herein. Density functional theory calculations suggest that the high catalytic activity primarily stems from both electronegative Pd active centers and the imino group (C=N) in PVPI for efficiently deprotonating FA to Pd-formate intermediates and subsequently for promoting the cleavage of C-H. The PVPI-capped Pd5Ag5 NWs are very stable and reusable for FA dehydrogenation catalysis.

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Publication details

The article was received on 14 Dec 2017, accepted on 09 Jan 2018 and first published on 09 Jan 2018


Article type: Communication
DOI: 10.1039/C7TA10963F
Citation: J. Mater. Chem. A, 2018, Accepted Manuscript
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    Enhanced Electron Transfer and Light Absorption on an Imino Polymer Capped PdAg Nanowire Networks for Efficient Room-Temperature Dehydrogenation of Formic Acid

    H. LIU, B. Huang, J. Zhou, K. Wang, Y. Yu, W. Yang and S. Guo, J. Mater. Chem. A, 2018, Accepted Manuscript , DOI: 10.1039/C7TA10963F

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