AuPd Nanocatalysts Supported on Citric Acid-Modified Boron Nitride to Boost Hydrogen Generation from Formic Acid Dehydrogenation

Abstract

Formic acid (FA) dehydrogenation is a potential technology for sustainable hydrogen production, while the tardy nature of FA dehydrogenation inhibits its development. To optimize the catalytic activity of hydrogen generation from formic acid dehydrogenation, citric acid-modified boron nitride with abundant −NH2 (CA–BN-NH2) is employed as a support to control the particle distribution, particle size, and electronic structure of AuPd nanoparticles. The obtained Au0.3Pd0.7/CA–BN-NH2 exhibits extraordinary catalytic activity for hydrogen production from FA dehydrogenation, possessing 100% hydrogen selectivity and an unprecedented initial turnover frequency (TOF) of 7046 mol H2 mol catalyst–1 h–1 without any additive, outperforming most of the reported noble metal catalysts under similar conditions. Transmission electron microscopy (TEM) images, X-ray photoelectron spectroscopy (XPS) analysis, and density functional theory (DFT) calculations demonstrate that the extraordinary catalytic activities are mainly due to the geometric effect and electronic effect of AuPd nanoparticles derived from the modification of h-BN with citric acid and the accompanying −NH2. This work provides more flexibility for designing highly efficient nanocatalysts for hydrogen generation from FA dehydrogenation.