Factors Influencing the Performance of Pd/C Catalysts in the Green Production of Hydrogen from Formic Acid. Issue 4 (3rd February 2017)

• Record Type: Journal Article
• Authors: Zacharska, Monika; Bulusheva, Lyubov G.; Lisitsyn, Alexander S.; Beloshapkin, Sergey; Guo, Yina; Chuvilin, Andrey L.; Shlyakhova, Elena V.; Podyacheva, Olga Y.; Leahy, James J.; Okotrub, Alexander V.; Bulushev, Dmitri A.
• Is Part Of: ChemSusChem. Volume 10:Issue 4(2017)
• Page Start: 720
• Page End: 730
• Publication Date: 2017-02-03
• Subjects: biomass -- carbon -- doping -- hydrogen -- palladium; Green chemistry -- Periodicals; Sustainable engineering -- Periodicals; Chemistry -- Periodicals; Chemical engineering -- Periodicals; 660
• DOI: 10.1002/cssc.201601637
• Languages: English
• ISSNs: 1864-5631

Abstract

Abstract: Formic acid derived from biomass is known to be used for hydrogen production over Pd catalysts. The effects of preparation variables, structure of the carbon support, surface functional composition on the state of Pd, and catalytic properties of the samples in the vapor‐phase decomposition of formic acid were studied. In all catalysts derived from Pd acetate, metal particles visible by conventional TEM had similar sizes, but the adsorption capacity towards CO responded strongly to N‐doping of the carbon surface. Moreover, a decrease in the CO/Pd values was accompanied by a significant increase in the reaction rate. Taking account of X‐ray photoelectron spectroscopy (XPS) and atomic resolution high‐angle annular dark‐field scanning transmission electron microscopy (HAADF/STEM) data, the trends observed were assigned to a larger fraction of single electron‐deficient Pd atoms in the N‐doped samples, which do not adsorb CO but interact with formic acid to produce hydrogen. This was confirmed by extended DFT studies. The obtained results are valuable for the development of Pd catalysts on carbon supports for different processes. Abstract : Hydrogen from formic acid : A significantly increased rate of hydrogen production from biomass‐derived formic acid over Pd/C catalysts is provided by N‐doping of the support. This is assigned to the formation of electron‐deficient single Pd atoms stabilized by pyridinic species of the support.