Continuous Hydrogen Generation from Formic Acid: Highly Active and Stable Ruthenium Catalysts

Authors

  • Albert Boddien,

    1. Leibniz-Institut für Katalyse e.V. an der Universität Rostock, Albert Einstein Str. 29a, 18059 Rostock, Germany, Fax: (+49)-381-1281-51113; phone: (+49)-381-1281-113
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  • Björn Loges,

    1. Leibniz-Institut für Katalyse e.V. an der Universität Rostock, Albert Einstein Str. 29a, 18059 Rostock, Germany, Fax: (+49)-381-1281-51113; phone: (+49)-381-1281-113
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  • Henrik Junge,

    1. Leibniz-Institut für Katalyse e.V. an der Universität Rostock, Albert Einstein Str. 29a, 18059 Rostock, Germany, Fax: (+49)-381-1281-51113; phone: (+49)-381-1281-113
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  • Felix Gärtner,

    1. Leibniz-Institut für Katalyse e.V. an der Universität Rostock, Albert Einstein Str. 29a, 18059 Rostock, Germany, Fax: (+49)-381-1281-51113; phone: (+49)-381-1281-113
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  • James R. Noyes,

    1. Leibniz-Institut für Katalyse e.V. an der Universität Rostock, Albert Einstein Str. 29a, 18059 Rostock, Germany, Fax: (+49)-381-1281-51113; phone: (+49)-381-1281-113
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  • Matthias Beller

    1. Leibniz-Institut für Katalyse e.V. an der Universität Rostock, Albert Einstein Str. 29a, 18059 Rostock, Germany, Fax: (+49)-381-1281-51113; phone: (+49)-381-1281-113
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Abstract

The ruthenium-catalyzed decomposition of formic acid was investigated with respect to continuous hydrogen generation and long-term stability of the catalytic systems. A highly active and stable system is presented, which was studied in batch and continuous modes for up to two months. The optimized catalyst system containing N,N-dimethyl-n-hexylamine with an in situ generated catalyst from (benzene)ruthenium dichloride dimer [RuCl2(benzene)]2 and 6 equivalents of 1,2-bis(diphenylphosphino)ethane (dppe) reached at room temperature a total turnover number (TON) of approximatly 260,000 with average turnover frequency (TOF) of about 900 h−1. Only hydrogen and carbon dioxide were detected in the produced gas mixture which makes this system applicable for direct use in fuel cells.

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