Abstract

Hydrogen is playing an increasingly larger role in clean energy technologies and the emerging hydrogen economy. However, efficient and selective H2 production from renewable resources is rare so far. Herein, we describe a dehydrogenation route that is applicable to various kinds of non-food-related biomass and daily waste, such as wheat straw, corn straw, rice straw, reed, bagasse, bamboo sawdust, cardboard and newspaper. H2 yields up to 95% were achieved by a one-pot, two-step reaction with a 69 ppm molecularly defined iridium catalyst bearing an imidazoline moiety from formic acid, which was in turn obtained via a 1 v% dimethyl sulfoxide-promoted hydrolysis–oxidation of biomass. Formation of the unwanted side products CO and CH4 was no more than 22 and 2 ppm, respectively, while CO2 was captured as carbonate. The resulting hydrogen gas can be directly applied in proton exchange membrane fuel cells.

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Change history

  • 30 July 2018

    In the version of this Article originally published, there were several errors in Table 1: in structure 1, the NH group bonded to the Ir should have been a H atom; the NR2 group bonded to the Ir should have been NH; in structures 2, 4 and 5, the OH groups bonded to the Ir atoms should have been OH2 groups; in structure 6 the OH2 group bonded to Ir was erroneously bonded with the below N; and in structure 10, the N=N bond should have been N–N. In structure 12 of Fig. 4, the CH2 between the two oxygen atoms should have been a CH group. Finally, the affiliations within the Supplementary Information were not consistent with those of the main text, a new Supplementary Information file has been uploaded.

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Acknowledgements

This work was supported by National Nature Science Foundation of China (nos. 21472145 and 21305117) and a Leibniz fellowship. We thank W.-F. Tian, K.-H. He, Xi’an Jiaotong University for their help during the experiments. We thank L. Wang, Institute of Pulp and Paper Technology, Hubei University of Technology, China for affording various raw biomass and daily waste. We thank H.-J. Jiao, Leibniz-Institut für Katalyse e.V. an der Universität Rostock, Z.-J. Shi, Fudan University for helpful discussion. We thank Wattecs Lab Equipment Co., Ltd. for strong support on autoclaves and constant pressure gas collectors.

Author information

Author notes

  1. These authors contributed equally: Ping Zhang and Yan-Jun Guo.

Affiliations

  1. Center for Organic Chemistry, Frontier Institute of Science and Technology, Xi’an Jiaotong University, Xi’an, China

    • Ping Zhang
    • , Yan-Jun Guo
    • , Yu-Rou Zhao
    •  & Yang Li
  2. Chemistry and Chemical Engineering College, Xianyang Normal University, Xianyang, China

    • Ping Zhang
    •  & Jun Chang
  3. Leibniz-Institut für Katalyse e.V. an der Universität Rostock, Rostock, Germany

    • Jianbin Chen
    • , Henrik Junge
    •  & Matthias Beller

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Contributions

Y.L. and M.B. conceived this project. P.Z., Y.-J.G., Y.-R.Z. and J.C. performed the experiments and analysed the data. J.C. synthesized the precursors of catalysts 5 and 6. P.Z., Y.-J.G., H.J., M.B. and Y.L. wrote the manuscript.

Competing interests

The authors declare no competing interests.

Corresponding authors

Correspondence to Matthias Beller or Yang Li.

Supplementary information

  1. Supplementary Information

    Supplementary Methods; Supplementary Tables 1–8; Supplementary Figures 1–36; Supplementary references

  2. Crystallographic data

    Crystallographic data for compound [Cp*CF3IrCl2]2, CCDC reference 1522237

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DOI

https://doi.org/10.1038/s41929-018-0062-0