1-Dimensional metal Nitride-Supported platinum nanoclusters for Low-Temperature hydrogen production from formic acid

Abstract

Formic acid is widely recognized as a suitable liquid hydrogen carrier for linking renewable energies toward various economic sectors. Designing efficient and stable heterogeneous catalysts for low-temperature hydrogen generation from formic acid is vital for this topic. In this study, a rational hierarchical architecture is explored by assembling Pt nanoclusters with 1-dimensional (1D) GaN nanowires. The catalytic architecture describes a considerable hydrogen production activity of 54.89 mmol·g_cat⁻¹·h⁻¹ with a nearly 100 % selectivity and a turnover frequency (TOF_Pt) of 505.7 h⁻¹ under near ambient condition, enables the achievement of a high turnover number of 306,981 mol H₂ per mole Pt over 200 h of long-term operation. Through comprehensive mechanistic studies, it is unraveled that the synergistic effect between Pt nanoclusters and GaN significantly reduces the energy barrier for the formation of the key HCOO* intermediate from formic acid dehydrogenation whereas significantly increase the energy barrier of HCOOH → HCO* + *OH. It thus simultaneously contributes to improving the activity and selectivity of formic acid decomposition toward H₂. This study proposes a promising strategy for hydrogen generation from formic acid at low temperatures, which is critical for achieving carbon neutrality by coordinating industrial waste heat with renewable energies via liquid hydrogen carriers.