Chinese Journal of Catalysis ›› 2019, Vol. 40 ›› Issue (11): 1704-1712.DOI: 10.1016/S1872-2067(19)63303-6

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Catalytic dehydrogenation of formic acid over palladium nanoparticles immobilized on fibrous mesoporous silica KCC-1

Siqian Zhang, Yingjie Qian, Wha-Seung Ahn   

  1. Department of Chemistry and Chemical Engineering, Inha University, Incheon 402-751, Republic of Korea
  • Received:2018-12-09 Revised:2019-01-14 Online:2019-11-18 Published:2019-09-06
  • Contact: Wha-Seung Ahn
  • Supported by:
    This work was supported by C1 Gas Refinery Program (2015M3D3A1A01064899) by the Ministry of Science, ICT & Future Planning, and also by Basic Science Research Program through the National Research Foundation of Korea funded by the Ministry of Education (Grant No.:NRF-2015R1A4A1042434).

Abstract: Uniform Pd nanoparticles immobilized on N-(3-trimethoxysilylpropyl)diethylenetriamine (PDETA)-functionalized fibrous silica KCC-1 (Pd/KCC-1-PDETA) were prepared with a mean Pd particle size of 2.8 nm. After characterization using powder X-ray diffraction, X-ray photoelectron spectroscopy, and N2 adsorption-desorption isotherms, Pd/KCC-1-PDETA was used as catalyst for additive-free dehydrogenation of formic acid to produce H2. Pd nanoparticle catalysts supported on two other mesoporous silica materials (MSF and KIT-6) were also synthesized to examine how the support affects the reaction. Among the three catalysts, Pd/KCC-1-PDETA exhibited significant catalytic activity (a turnover frequency of 332 h-1 at 323 K and 100% selectivity towards hydrogen), owing to the unique fibrous morphology of KCC-1 and the presence of amine groups that reduced the Pd particle size and improved the access of reactant to the catalytically active Pd sites. The influence of Pd loading (2-10 wt.%), reaction temperature, and reaction time was also examined for the dehydrogenation reaction. Pd/KCC-1-PDETA was recovered easily after the reaction and showed good reusability up to five times without any significant loss in catalytic performance.

Key words: Fibrous nanosilica, KCC-1, Palladium nanoparticles, Hydrogen storage, Formic acid dehydrogenation