Dehydrogenation of Formic Acid at Room Temperature: Boosting Palladium Nanoparticle Efficiency by Coupling with Pyridinic-Nitrogen-Doped Carbon

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• 作者：Dr. Qing-Yuan Bi ; Jian-Dong Lin ; Dr. Yong-Mei Liu ; Prof. Dr. He-Yong He ; Prof. Dr. Fu-Qiang Huang and Prof. Dr. Yong Cao
• 刊名：Angewandte Chemie International Edition
• 出版年：2016
• 出版时间：September 19, 2016
• 年：2016
• 卷：55
• 期：39
• 页码：11849-11853
• 全文大小：925K
• ISSN：1521-3773

文摘

The use of formic acid (FA) to produce molecular H₂ is a promising means of efficient energy storage in a fuel-cell-based hydrogen economy. To date, there has been a lack of heterogeneous catalyst systems that are sufficiently active, selective, and stable for clean H₂ production by FA decomposition at room temperature. For the first time, we report that flexible pyridinic-N-doped carbon hybrids as support materials can significantly boost the efficiency of palladium nanoparticle for H₂ generation; this is due to prominent surface electronic modulation. Under mild conditions, the optimized engineered Pd/CN_0.25 catalyst exhibited high performance in both FA dehydrogenation (achieving almost full conversion, and a turnover frequency of 5530 h⁻¹ at 25 °C) and the reversible process of CO₂ hydrogenation into FA. This system can lead to a full carbon-neutral energy cycle.