Abstract
Safe and efficient hydrogen generation and storage has received much attention in recent years. Herein, a commercial 5 wt% Pd/C catalyst has been investigated for the catalytic, additive-free decomposition of formic acid at mild conditions, and the experimental parameters affecting the process systematically have been investigated and optimised. The 5 wt% Pd/C catalyst exhibited a remarkable 99.9% H2 selectivity and a high catalytic activity (TOF = 1136 h−1) at 30 °C toward the selective dehydrogenation of formic acid to H2 and CO2. The present commercial catalyst demonstrates to be a promising candidate for the efficient in-situ hydrogen generation at mild conditions possibiliting practical applications of formic acid systems on fuel cells. Finally DFT studies have been carried out to provide insights into the reactivity and decomposition of formic acid along with the two-reaction pathways on the Pd (111) surface.
Highlights
Energy consumption around the world is increasing every day, which requires higher energy generation capacity, better energy management, and a shift away from non-renewable fossil fuels
We report the catalytic performance of an efficient commercial 5 wt% Pd/C for the production of hydrogen from the catalytic aqueous additive-free formic acid decomposition. 5 wt% Pd/C has been selected as a commercial reference and starting point for future research and optimisation of reaction conditions
Liquid-phase formic acid decomposition was performed in a two-necked 100 ml round-bottom flask, which was placed in an oil bath with a reflux condenser and a magnetic stirrer at a pre-set temperature (30–60 °C)
Summary
Energy consumption around the world is increasing every day, which requires higher energy generation capacity, better energy management, and a shift away from non-renewable fossil fuels. Ammonia decomposition has been studied at temperatures below 500 K showing a significant reduction in activation energy when using carbon nanotubes catalysts promoted with cesium [14] Metal hydrides such those of Mg–Al–Fe has been reported to achieve a maximum rate of 499.5 ml min−1 g−1 of hydrogen at 25 °C for Mg60–Al30–Fe10 (wt%) in 0.6 mol l−1 NaCl solution [15]. Recent studies by Xing and coworkers have shown the development of Pd–Au and Pd–Ag alloys supported on carbon to overcome the poisoning and stability issued on monometallic Pd analogues These bimetallic particles generated high purity hydrogen production from the decomposition of formic acid at low temperatures. Periodic density functional theory (DFT) calculations were employed to gain insights on the energetics of formic acid decomposition on Pd (111) surface as the most represented model
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