Carbon dioxide and formic acid—the couple for environmental-friendly hydrogen storage?

Enthaler, Stephan; Langermann, Jan von; Schmidt, Thomas E.

doi:10.1039/b907569k

Cited by 664 publications

(419 citation statements)

References 120 publications

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“…The obtained supports CNFs and N-CNFs (7 wt.% N) were mesoporous with average pore diameters of 8 and 11 nm and Brunauer-EmmettTeller (BET) surface areas of 220 and 200 m 2 g -1 , respectively. 1 wt.% Ru and Pd catalysts on the N-free and N-doped carbon (1Ru/(N-)CNFs and 1Pd/(NCNFs) were prepared via incipient wetness impregnation using an aqueous solution of Ru(NO)(NO 3 ) 3 or Pd-acetate in acetone, respectively. For the preparation of 0.3Pt/N-CNFs, 1Pt/CNFs and 1Pt/N-CNFs catalysts, 0.3 and 1 wt.% of Pt were deposited by homogeneous precipitation from H 2 PtCl 6 with NaOH.…”

Section: Methodsmentioning

confidence: 99%

“…[1][2][3][4][5] It is also important that the starting acid can be produced with high yields from renewable biomass by hydrolysis of cellulose 6 or by its oxidation. 5,7 Additionally, formic acid can be used directly for hydrogenation reactions instead of molecular hydrogen, providing the advantage of easier transportation and storage of the hydrogenating agent.…”

Section: Introductionmentioning

confidence: 99%

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Single Atoms of Pt-Group Metals Stabilized by N-Doped Carbon Nanofibers for Efficient Hydrogen Production from Formic Acid

et al. 2016

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Formic acid is a valuable chemical derived from biomass, as it has a high hydrogen-storage capacity and appears to be an attractive source of hydrogen for various applications. Hydrogen production via formic acid decomposition is often based on using supported catalysts with Pt-group metal nanoparticles. In the present paper, we show that the decomposition of the acid proceeds more rapidly on single metal atoms (by up to one order of magnitude). These atoms can be obtained by rather simple means through anchoring Pt-group metals onto mesoporous N-functionalized carbon nanofibers. A thorough evaluation of the structure of the active site by aberration-corrected scanning transmission electron microscopy (ac-STEM) in high-angle annular dark field (HAADF) mode, by CO chemisorption, X-ray photoelectron spectroscopy (XPS) and quantum-chemical calculations reveals that the metal atom is coordinated by a pair of pyridinic nitrogen atoms at the edge of graphene sheets. The chelate binding provides an ionic/electron-deficient state of these atoms prevents their aggregation and thereby leads to an excellent stability under the reaction conditions. Catalysts with single atoms have also shown very high selectivity. Evidently, the findings can be extended to hydrogen production from other chemicals and can be helpful for improving other energy-related and environmentally benign catalytic processes.

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Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Single Atoms of Pt-Group Metals Stabilized by N-Doped Carbon Nanofibers for Efficient Hydrogen Production from Formic Acid

et al. 2016

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“…[31][32][33] Among them, Pd is one of the metals with the lowest activation energy and most promising TOF values. 34,35 The incorporation of Pd NPs on different supports (carbon, zeolites, MOFs or silica) has also been studied in the literature with different results depending on the nature of the support and the active phases features. [36][37][38][39][40][41] Herein the evolution of the PVP-Pd interaction over time as well as its repercussion on the final catalytic performance in the H 2 production from the dehydrogenation of FA was assessed by synthesising a series of catalysts based on PVP-capped Pd NPs supported on a meso-and macroporous SiO 2 .…”

Section: Introductionmentioning

confidence: 99%

Evolution of the PVP–Pd Surface Interaction in Nanoparticles through the Case Study of Formic Acid Decomposition

et al. 2016

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Palladium nanoparticles (Pd NPs) were synthesised by the reduction-by-solvent method using polyvinylpirrolidone (PVP) as capping agent. The non-static interaction between PVP and the metallic surface may change the properties of the NPs due to the different possible interactions, either through the O or N atoms of the PVP. In order to analyse these effects and their repercussion in their catalytic performance, Pd NPs with various PVP/Pd molar ratios (1, 10 and 20) were prepared, deposited on silica and tested in the formic acid decomposition reaction. The catalytic tests were conducted using catalysts prepared by loading NPs with three different time lapses between their purification and their deposition on the silica support (1 day, 1 month, and 6 months). CO adsorption, FTIR spectroscopy, XPS and TEM characterisation were used to determine the accessibility of the Pd NPs surface sites, electronic state of Pd and the average NPs size, respectively. The H 2 production from the formic acid decomposition reaction has a strong dependence with the Pd surface features, which in turn are related to the NPs aging time due to the progressive removal of the PVP.

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“…(Boddien et al, 2011;Enthaler et al, 2010;Johnson et al, 2010;Scholten et al, 2010;Tedsree et al, 2011;Yasaka et al, 2010;Zhao et al, 2011) Figure 5. Reversible splitting of formic acid.…”

Section: Formic Acidmentioning

confidence: 99%

Application of Ionic Liquids in Hydrogen Storage Systems

Sahler¹,

Prechtl²

2012

Hydrogen Storage

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Carbon dioxide and formic acid—the couple for environmental-friendly hydrogen storage?

Cited by 664 publications

References 120 publications

Single Atoms of Pt-Group Metals Stabilized by N-Doped Carbon Nanofibers for Efficient Hydrogen Production from Formic Acid

Single Atoms of Pt-Group Metals Stabilized by N-Doped Carbon Nanofibers for Efficient Hydrogen Production from Formic Acid

Evolution of the PVP–Pd Surface Interaction in Nanoparticles through the Case Study of Formic Acid Decomposition

Application of Ionic Liquids in Hydrogen Storage Systems

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