Sergey Beloshapkin

Abstract: Single-site heterogeneous catalysis with isolated Pd atoms was reported earlier, mainly for oxidation reactions and for Pd catalysts supported on oxide surfaces. In the present work, we show that single Pd atoms on nitrogen-functionalized mesoporous carbon, observed by aberration-corrected scanning transmission electron microscopy (ac STEM), contribute significantly to the catalytic activity for hydrogen production from vapor-phase formic acid decomposition, providing an increase by 2–3 times in comparison to Pd catalysts supported on nitrogen-free carbon or unsupported Pd powder. Some gain in selectivity was also achieved. According to X-ray photoelectron spectroscopy (XPS) and near-edge X-ray absorption fine structure (NEXAFS) studies after ex situ reduction in hydrogen at 573 K, these species exist in a Pd2+ state coordinated by nitrogen species of the support. Extended density functional theory (DFT) calculations confirm that an isolated Pd atom can be the active site for the reaction, giving decompos...

TL;DR: In this article, the mean metal particle size of these materials was estimated by HRTEM and turnover frequencies were calculated using these data, and the selectivity of these catalysts was found to be only weakly dependent on the reaction temperature and the formic acid conversion.

TL;DR: In this article, the authors compared the performance of N-doped and undoped Pt catalysts on carbon nanofibers with different nitrogen contents for hydrogen production by formic acid decomposition.

TL;DR: In this paper, a detailed mechanism for the oxidation of methanol on vanadia catalysts is discussed, which involves a reversible reduction of V 5+ cations, indicating that vanadia lattice oxygen participates in the oxidation via the classical Mars-van Krevelen mechanism.

TL;DR: The rate of hydrogen production from vapour-phase formic acid decomposition can be increased by 1-2 orders of magnitude by doping a Pd/C catalyst with potassium ions.