期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 282, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119569
关键词
Intermetallic compound; Layered double hydroxides; Atomically-ordered sites; Furfural; Structure-selectivity correlation
资金
- National Natural Science Foundation of China [NSFC: 21871021, 21521005]
- National Key Research and Development Program [2017YFA0206804]
- Fundamental Research Funds for the Central Universities [XK1802-6, XK1803-05]
- China Postdoctoral Science Foundation [2019M660412]
This study demonstrates the superior catalytic performance of a NiMo intermetallic compound (IMC) catalyst in furfural hydrodeoxygenation (HDO) to 2-methylfuran (2-MF), highlighting the decisive effect of atomically-ordered active sites on activation of oxygen-containing functional groups and product selectivity. The ordered Ni-Mo bimetallic sites in IMC facilitate the activation and cleavage of C-OH bonds in intermediates, leading to enhanced production of 2-MF, which can potentially be extended to catalytic upgrading of biomass-derived platform molecules.
Activation of oxygen-containing functional groups plays a key role in sustainable biomass upgrading and conversion. In this work, a NiMo intermetallic compound (IMC) catalyst was prepared based on layered double hydroxides (LDHs) precursors, which displayed prominent catalytic performance for furfural hydrodeoxygenation (HDO) to 2-methylfuran (2-MF) (yield: 99 %) at a rather low hydrogen pressure (0.1 MPa), significantly superior to NiMo alloy, monometallic Ni and other Ni-based catalysts ever reported. CO-IR, STEM, EXAFS and XANES give direct evidences that the atomically-ordered Ni/Mo sites in NiMo IMC determine the uniform bridging-type adsorption mode of C = O bond in furfural whilst adsorption of furan ring is extremely suppressed. In situ FT-IR and DFT calculation further substantiate that ordered Ni-Mo bimetallic sites of IMC, in contrast to the random atomic sequence in NiMo alloy, facilitate the activation and cleavage of C-OH bond in the intermediate (furfuryl alcohol, FOL), accounting for the production of 2-MF. This work demonstrates the decisive effect of atomically-ordered active sites in IMC catalyst on activation of oxygen-containing functional groups and product selectivity, which can be extended to catalytic upgrading of biomass-derived platform molecules.
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