4.7 Article

Hydrogen generation rate enhancement by in situ Fe(0) and nitroarene substrates in Fe3O4@Pd catalyzed ammonia borane hydrolysis and nitroarene reduction tandem reaction

期刊

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
卷 46, 期 50, 页码 25486-25499

出版社

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2021.05.106

关键词

Hydrogen generation; Tandem reaction; Palladium catalysis; Core-shell nanoparticles; Solid-state synthesis

资金

  1. BITS-Pilani University

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The catalytic enhancement of hydrogen generation during Fe3O4@Pd core-shell nanoparticles catalyzed tandem reaction is attributed to both in situ formation of Fe(0) and the presence of nitroarenes substrates. The rate of hydrogen generation from ammonia borane depends on the nitroarene substrate, with 4-nitrophenol showing higher activity due to differences in adsorption on the catalyst surface. The electronic connection between Fe and Pd interface plays a crucial role in the enhanced catalytic performance of the tandem reaction.
We report the catalytic enhancement of hydrogen generation by 1) in situ Fe(0) formed and 2) nitroarenes substrates during Fe3O4@Pd core-shell nanoparticles catalyzed tandem reaction. The active hydrogen species are generated in Pd shell, which either combine to form H-2 gas or take part in relatively faster nitroarene reduction reaction. The rate of hydrogen generation from ammonia borane is dependent on the nitroarene substrate and is higher when 4-nitrophenol is used. This is due to the difference in ammonia borane adsorption on the surface of the catalyst. During recyclability, the H-2 generation rate of 2 wt% Pd loaded samples is higher than other compositions. Such an enhancement has been attributed to the formation of Fe(0) via gamma-FeOOH mediated by Pd species, presumably through Pd(OH)(2). The electronic connection between Fe and Pd interface is thus shown to play an important role in the catalytic enhancement of the tandem reaction. (C) 2021 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

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