1-Dimensional metal Nitride-Supported platinum nanoclusters for Low-Temperature hydrogen production from formic acid
•A 1-Dimensional metal nitride-supported platinum nanoclusters catalyst is developed for low-temperature hydrogen production from formic acid.•The Pt/GaN catalyst exhibits a high hydrogen production activity of 54.89 mmol·gcat−1· h−1 under near-ambient conditions with nearly 100% selectivity.•A high...
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Veröffentlicht in: | Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2024-11, Vol.500, p.156940, Article 156940 |
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Sprache: | eng |
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Zusammenfassung: | •A 1-Dimensional metal nitride-supported platinum nanoclusters catalyst is developed for low-temperature hydrogen production from formic acid.•The Pt/GaN catalyst exhibits a high hydrogen production activity of 54.89 mmol·gcat−1· h−1 under near-ambient conditions with nearly 100% selectivity.•A high turnover frequency (TOFPt) of 505.7 h−1 and a remarkable turnover number of 306,981 mol H2 per mole Pt over 200 h of operation are achieved.•Synergy between Pt nanoclusters and GaN nanowires reduces the energy barrier for formate intermediate formation and increases the barrier for undesired reactions.•The study presents a promising strategy for low-temperature hydrogen generation, crucial for carbon neutrality via the use of liquid hydrogen carriers.
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·gcat−1·h−1 with a nearly 100 % selectivity and a turnover frequency (TOFPt) of 505.7 h−1 under near ambient conditions, enabling 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 increases 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. |
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ISSN: | 1385-8947 |
DOI: | 10.1016/j.cej.2024.156940 |