Journal
CHEMSUSCHEM
Volume 13, Issue 17, Pages 4409-4419Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201903286
Keywords
biomass; heterogeneous catalysis; iridium; rhenium; supported catalysts
Funding
- National Natural Science Foundation of China [21878288, 21690080, 21690083, 21721004]
- DNL Cooperation Fund CAS [DNL180302]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17020100]
- National Key R&D Program of China [2016YFA0202801, 2018YFB1501402]
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The direct transformation of lignin into fuels and chemicals remains a huge challenge because of the recalcitrant and complicated structure of lignin. In this study, rhenium oxide-modified iridium supported on SiO2 (Ir-ReOx/SiO2) is employed for the one-pot conversion of various lignin model compounds and lignin feedstocks into naphthenes. Up to 100 % yield of cyclohexane from model compounds and 44.3 % yield of naphthenes from lignin feedstocks are achieved. 2 D HSQC NMR spectroscopy before and after the reaction confirms the activity of Ir-ReOx/SiO2 in the cleavage of the C-O bonds and hydrodeoxygenation of the depolymerized products. H-2 temperature-programmed reduction, temperature-programmed desorption of NH3, IR spectroscopy of pyridine adsorption, X-ray photoelectron spectroscopy, X-ray absorption fine structure analysis, and control experiments reveal that a synergistic effect between Ir and ReOx in Ir-ReOx/SiO2 plays a crucial role in the high performance; ReOx is mainly responsible for the cleavage of C-O bonds, whereas Ir is responsible for hydrodeoxygenation and saturation of the benzene rings. This methodology opens up an energy-efficient route for the direct conversion of lignin into valuable naphthenes.
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