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

Qing-Yuan Bi; Jian-Dong Lin; Yong-Mei Liu; He-Yong He; Fu-Qiang Huang; Yong Cao

doi:10.1002/anie.201605961

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

Angew Chem Int Ed Engl. 2016 Sep 19;55(39):11849-53. doi: 10.1002/anie.201605961. Epub 2016 Aug 23.

Authors

Qing-Yuan Bi^{1

2}, Jian-Dong Lin¹, Yong-Mei Liu¹, He-Yong He¹, Fu-Qiang Huang², Yong Cao³

Affiliations

¹ Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, 200433, P.R. China.
² State Key Laboratory of High Performance Ceramics and Superfine Microstructures, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, P.R. China.
³ Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, 200433, P.R. China. yongcao@fudan.edu.cn.

PMID: 27552650
DOI: 10.1002/anie.201605961

Abstract

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/CN0.25 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.

Keywords: Pd nanoparticles; formic acid; heterogeneous catalysis; hydrogen storage; pyridinic-N-doped carbon.

Publication types

Research Support, Non-U.S. Gov't