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Lignin depolymerisation by nickel supported layered-double hydroxide catalysts
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DOI：10.1039/c3gc42138d.png)
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摘要
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Lignin depolymerisation is traditionally facilitated with homogeneous acid or alkaline catalysts. Given the effectiveness of homogeneous basic catalysts for lignin depolymerisation, here, heterogeneous solid-base catalysts are screened for C-O bond cleavage using a model compound that exhibits a common arylether linkage in lignin. Hydrotalcite (HTC), a layered double hydroxide (LDH), is used as a support material as it readily harbours hydroxide anions in the brucite-like layers, which are hypothesised to participate in catalysis. A 5 wt% Ni/HTC catalyst is particularly effective at C-O bond cleavage of a model dimer at 270 degrees C without nickel reduction, yielding products from C-O bond cleavage identical to those derived from a base-catalysed mechanism. The 5% Ni-HTC catalyst is shown to depolymerise two types of biomass-derived lignin, namely Organosolv and ball-milled lignin, which produces alkyl-aromatic products. X-ray photoelectron spectroscopy and energy dispersive X-ray spectroscopy show that the nickel is well dispersed and converts to a mixed valence nickel oxide upon loading onto the HTC support. The structure of the catalyst was characterised by scanning and transmission electron microscopy and X-ray diffraction, which demonstrates partial dehydration upon reaction, concomitant with a base-catalysed mechanism employing hydroxide for C-O bond cleavage. However, the reaction does not alter the overall catalyst microstructure, and nickel does not appreciably leach from the catalyst. This study demonstrates that nickel oxide on a solid-basic support can function as an effective lignin depolymerisation catalyst without the need for external hydrogen and reduced metal, and suggests that LDHs offer a novel, active support in multifunctional catalyst applications.
Keyword:
MG-AL HYDROTALCITE
O BOND-CLEAVAGE
ARYL ETHERS
PHENOL HYDROGENATION
ALDOL CONDENSATION
VANADIUM CATALYST
XANTPHOS CATALYST
AEROBIC OXIDATION
CO CHEMISORPTION
BASE CATALYSTS
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期刊
IF:
9.2
论文数:
1.3W
被引数:
7.6W
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