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Reversible hydrogenation of carbon dioxide to formic acid using a Mn-pincer complex in the presence of lysine

Author

Listed:
  • Duo Wei

    (Leibniz-Institut für Katalyse e.V.)

  • Rui Sang

    (Leibniz-Institut für Katalyse e.V.)

  • Peter Sponholz

    (APEX Energy Teterow GmbH)

  • Henrik Junge

    (Leibniz-Institut für Katalyse e.V.)

  • Matthias Beller

    (Leibniz-Institut für Katalyse e.V.)

Abstract

Efficient hydrogen storage and release are essential for effective use of hydrogen as an energy carrier. In principle, formic acid could be used as a convenient hydrogen storage medium via reversible CO2 hydrogenation. However, noble metal-based catalysts are currently needed to facilitate the (de)hydrogenation, and the CO2 produced during hydrogen release is generally released, resulting in undesirable emissions. Here we report an α-amino acid-promoted system for reversible CO2 hydrogenation to formic acid using a Mn-pincer complex as a homogeneous catalyst. We observe good stability and reusability of the catalyst and lysine as the amino acid at high productivities (CO2 hydrogenation: total turnover number of 2,000,000; formic acid dehydrogenation: total turnover number of 600,000). Employing potassium lysinate, we achieve >80% H2 evolution efficiency and >99.9% CO2 retention in ten charge–discharge cycles, avoiding CO2 re-loading steps between each cycle. This process was scaled up by a factor of 18 without obvious drop of the productivity.

Suggested Citation

  • Duo Wei & Rui Sang & Peter Sponholz & Henrik Junge & Matthias Beller, 2022. "Reversible hydrogenation of carbon dioxide to formic acid using a Mn-pincer complex in the presence of lysine," Nature Energy, Nature, vol. 7(5), pages 438-447, May.
    • Handle: RePEc:nat:natene:v:7:y:2022:i:5:d:10.1038_s41560-022-01019-4
    DOI: 10.1038/s41560-022-01019-4
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    References listed on IDEAS

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    1. Daniel Forberg & Tobias Schwob & Muhammad Zaheer & Martin Friedrich & Nobuyoshi Miyajima & Rhett Kempe, 2016. "Single-catalyst high-weight% hydrogen storage in an N-heterocycle synthesized from lignin hydrogenolysis products and ammonia," Nature Communications, Nature, vol. 7(1), pages 1-6, December.
    2. Saravanakumar Elangovan & Jacob Neumann & Jean-Baptiste Sortais & Kathrin Junge & Christophe Darcel & Matthias Beller, 2016. "Efficient and selective N-alkylation of amines with alcohols catalysed by manganese pincer complexes," Nature Communications, Nature, vol. 7(1), pages 1-8, November.
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    Cited by:

    1. Rui Sang & Carolin Amber Martina Stein & Thomas Schareina & Yuya Hu & Alexander Léval & Jonas Massa & Volkan Turan & Peter Sponholz & Duo Wei & Ralf Jackstell & Henrik Junge & Matthias Beller, 2024. "Development of a practical formate/bicarbonate energy system," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    2. Xianxian Qin & Jiejie Li & Tian-Wen Jiang & Xian-Yin Ma & Kun Jiang & Bo Yang & Shengli Chen & Wen-Bin Cai, 2024. "Disentangling heterogeneous thermocatalytic formic acid dehydrogenation from an electrochemical perspective," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    3. Yingqi Liu & Zhiyuan Zhang & Junyang Tan & Biao Chen & Bingyi Lu & Rui Mao & Bilu Liu & Dashuai Wang & Guangmin Zhou & Hui-Ming Cheng, 2024. "Deciphering the contributing motifs of reconstructed cobalt (II) sulfides catalysts in Li-CO2 batteries," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    4. Yanzhe Shi & Bingcheng Luo & Rui Sang & Dandan Cui & Ye Sun & Runqi Liu & Zili Zhang & Yifei Sun & Henrik Junge & Matthias Beller & Xiang Li, 2024. "Combination of nanoparticles with single-metal sites synergistically boosts co-catalyzed formic acid dehydrogenation," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    5. Wan Nor Roslam Wan Isahak & Muhammad Nizam Kamaruddin & Zatil Amali Che Ramli & Khairul Naim Ahmad & Waleed Khalid Al-Azzawi & Ahmed Al-Amiery, 2022. "Decomposition of Formic Acid and Acetic Acid into Hydrogen Using Graphitic Carbon Nitride Supported Single Metal Catalyst," Sustainability, MDPI, vol. 14(20), pages 1-18, October.
    6. Duo Wei & Xinzhe Shi & Henrik Junge & Chunyu Du & Matthias Beller, 2023. "Carbon neutral hydrogen storage and release cycles based on dual-functional roles of formamides," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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