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
Hauptverfasser: Qiu, Liang, Sheng, Bowen, Ye, Haotian, Wang, Ping, Li, Jinglin, Li, Ying, Li, Yixin, Yu, Tianqi, Salman Nasir, Muhammad, Wang, Xinqiang, Pan, Hu, Huang, Zhen, Zhou, Baowen
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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.
ISSN:1385-8947
DOI:10.1016/j.cej.2024.156940