Dörthe Mellmann

Leibniz Institute for Catalysis

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Matthias Beller

Leibniz Institute for Catalysis

Henrik Junge

RWTH Aachen University

Peter Sponholz

University of Rostock

Albert Boddien

Sasol (Germany)

Ralf Jackstell

Leibniz Institute for Catalysis

Gábor Laurenczy

École Polytechnique Fédérale de Lausanne

Felix Gärtner

GSI Helmholtz Centre for Heavy Ion Research

Ralf Ludwig

University of Rostock

Christopher Federsel

Leibniz Institute for Catalysis

Matthias Bauer

Paderborn University

Cooperative Institutions

Leibniz Institute for Catalysis

University of Rostock

Institute for the Chemistry of OrganoMetallic Compounds

Leibniz Institute for Neurobiology

National Research Council

École Polytechnique Fédérale de Lausanne

Rostocker Zentrum zur Erforschung des Demografischen Wandels

Consorzio Roma Ricerche

Aarhus University

Centre National de la Recherche Scientifique

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Towards a Practical Setup for Hydrogen Production from Formic Acid

ChemSusChem (2013)

Peter Sponholz Dörthe Mellmann Henrik Junge Matthias Beller

Formic acid cracker: A mini plant that allows for continuous formic acid decomposition to hydrogen and carbon dioxide under ambient conditions is presented. By using an in situ-formed ruthenium catalyst, unprecedented turnover numbers over 1 000 000 are achieved. The active catalyst is formed in situ from commercially available [RuCl2(benzene)]2 and 1,2-bisdiphenylphosphinoethane.

10.1002/cssc.201300186

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Citations (126)

Efficient Dehydrogenation of Formic Acid Using an Iron Catalyst

Science (2011)

Albert Boddien Dörthe Mellmann Felix Gärtner Ralf Jackstell Henrik Junge

Iron-catalyzed hydrogen generation raises prospects for a cheap hydrogen storage medium.

10.1126/science.1206613

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Citations (776)

Formic acid as a hydrogen storage material – development of homogeneous catalysts for selective hydrogen release

Chemical Society Reviews (2016)

Dörthe Mellmann Peter Sponholz Henrik Junge Matthias Beller

Liquid energy: formic acid is an ideal candidate for catalytic release and storage of hydrogen.

10.1039/c5cs00618j

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Citations (752)

Inner- versus Outer-Sphere Ru-Catalyzed Formic Acid Dehydrogenation: A Computational Study

Organometallics (2013)

Gabriele Manca Irene Mellone F. Bertini Maurizio Peruzzini Luca Rosi

A detailed hybrid density functional theory study was carried out to clarify the mechanism of Ru-catalyzed dehydrogenation of formic acid in the presence of the octahedral complexes [Ru(κ4-NP3)Cl2] (1) and [Ru(κ3-triphos)(MeCN)3](PF6)2 (2·PF6) [NP3 = N(CH2CH2PPh2)3, triphos = MeC(CH2PPh2)3]. It was shown that Ru-hydrido vs Ru-formato species are pivotal to bringing about the efficient release of H2 and CO2 following either a metal-centered (inner-sphere) or a ligand-centered (outer-sphere) pathway, respectively.

Triphos

Coordination sphere

10.1021/om400761t

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Kohlenstoffdioxid‐neutrale Wasserstoffspeicherung basierend auf Bicarbonaten und Formiaten

Angewandte Chemie (2011)

Albert Boddien Felix Gärtner Christopher Federsel Peter Sponholz Dörthe Mellmann

Die selektiven Hydrierungen von Bicarbonaten und Carbonaten sowie von CO2 und Base zu Formiaten und die selektive Dehydrierung von Formiaten zu Bicarbonaten gelingen mit ein und demselben In-situ-Rutheniumkatalysator. Beide Reaktionen können zu einem reversiblen Wasserstoffspeichersystem gekoppelt werden. dppm=1,2-Bis(diphenylphosphanyl)methan.

10.1002/ange.201101995

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Citations (73)

Base‐Free Non‐Noble‐Metal‐Catalyzed Hydrogen Generation from Formic Acid: Scope and Mechanistic Insights

Chemistry - A European Journal (2014)

Dörthe Mellmann Enrico Barsch Matthias Bauer Kathleen Grabow Albert Boddien

Abstract The iron‐catalyzed dehydrogenation of formic acid has been studied both experimentally and mechanistically. The most active catalysts were generated in situ from cationic Fe II /Fe III precursors and tris[2‐(diphenylphosphino)ethyl]phosphine ( 1 , PP 3 ). In contrast to most known noble‐metal catalysts used for this transformation, no additional base was necessary. The activity of the iron catalyst depended highly on the solvent used, the presence of halide ions, the water content, and the ligand‐to‐metal ratio. The optimal catalytic performance was achieved by using [FeH(PP 3 )]BF 4 /PP 3 in propylene carbonate in the presence of traces of water. With the exception of fluoride, the presence of halide ions in solution inhibited the catalytic activity. IR, Raman, UV/Vis, and EXAFS/XANES analyses gave detailed insights into the mechanism of hydrogen generation from formic acid at low temperature, supported by DFT calculations. In situ transmission FTIR measurements revealed the formation of an active iron formate species by the band observed at 1543 cm −1 , which could be correlated with the evolution of gas. This active species was deactivated in the presence of chloride ions due to the formation of a chloro species (UV/Vis, Raman, IR, and XAS). In addition, XAS measurements demonstrated the importance of the solvent for the coordination of the PP 3 ligand.

X-ray absorption spectroscopy

Noble metal

10.1002/chem.201403602

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Citations (53)

CO₂‐“Neutral” Hydrogen Storage Based on Bicarbonates and Formates

Angewandte Chemie International Edition (2011)

Albert Boddien Felix Gärtner Christopher Federsel Peter Sponholz Dörthe Mellmann

Let the circle be unbroken! One ruthenium catalyst generated in situ facilitates the selective hydrogenation of bicarbonates and carbonates, as well as CO2 and base, to give formates and also the selective dehydrogenation of formates back to bicarbonates. The two reactions can be coupled, leading to a reversible hydrogen-storage system. dppm=1,2-bis(diphenylphosphino)methane.

Base (topology)

10.1002/anie.201101995

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Citations (289)

Formic acid dehydrogenation catalysed by ruthenium complexes bearing the tripodal ligands triphos and NP₃

Dalton Transactions (2012)

Irene Mellone Maurizio Peruzzini Luca Rosi Dörthe Mellmann Henrik Junge

The selective formic acid dehydrogenation to a mixture of CO2 and H2 was achieved with moderate to good productivities in the presence of homogeneous Ru catalysts bearing the polydentate tripodal ligands 1,1,1-tris-(diphenylphosphinomethyl)ethane (triphos) and tris-[2-(diphenylphosphino)ethyl]amine (NP3), either made in situ from suitable Ru(III) precursors or as molecular complexes. Preliminary mechanistic studies highlighting subtle differences due to ligand effects in the corresponding systems under study are also presented.

Triphos

Tripodal ligand

Homogeneous Catalysis

10.1039/c2dt32043f

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Citations (94)

Ruthenium-Catalyzed Hydrogen Generation from Alcohols and Formic Acid, Including Ru-Pincer-Type Complexes

Topics in organometallic chemistry (2014)

Pamela G. Alsabeh Dörthe Mellmann Henrik Junge Matthias Beller

10.1007/3418_2014_84

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Citations (20)

Hydrogen Storage in Formic Acid – Amine Adducts

CHIMIA International Journal for Chemistry (2011)

Albert Boddien Felix Gärtner Dörthe Mellmann Peter Sponholz Henrik Junge

Formic acid, containing 4.4 wt% of hydrogen, is a non-toxic liquid at ambient temperature and therefore an ideal candidate as potential hydrogen storage material. Formic acid can be generated via catalytic hydrogenation of CO2 or bicarbonate in the presence of an amine with suitable ruthenium catalysts. In addition selective dehydrogenation of formic acid amine adducts can be carried out at ambient temperatures with either ruthenium phosphine catalyst systems as well as iron-based catalysts. In detail we obtained with the [RuCl2(benzene)]2/dppe catalyst system a remarkable TON of 260,000 at room temperature. Moreover applying Fe3(CO)12 together with tribenzylphosphine and 2,2':6',2"-terpyridine under visible light irradiation a TON of 1266 was obtained, which is the highest activity known to date for selective dehydrogenation of formic acid applying non-precious metal catalysts.

Ton

10.2533/chimia.2011.214

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Citations (32)