期刊
CHEMSUSCHEM
卷 13, 期 18, 页码 4945-4953出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202000764
关键词
heterogeneous catalysis; hydrogenation; mesoporous materials; platinum; reaction mechanisms
资金
- EPSRC [EP/K036548/1, EP/K014706/1]
- Johnson Matthey
- Royal Society
- European Union Seventh Framework Programme (FP7/2007-2013) [604307]
- EPSRC [EP/K014706/1, EP/G007594/4, EP/K036548/2] Funding Source: UKRI
Hydrodeoxygenation (HDO) is a promising technology to upgrade fast pyrolysis bio-oils but it requires active and selective catalysts. Here we explore the synergy between the metal and acid sites in the HDO of anisole, a model pyrolysis bio-oil compound, over mono- and bi-functional Pt/(Al)-SBA-15 catalysts. Ring hydrogenation of anisole to methoxycyclohexane occurs over metal sites and is structure sensitive; it is favored over small (4 nm) Pt nanoparticles, which confer a turnover frequency (TOF) of approximately 2000 h(-1)and a methoxycyclohexane selectivity of approximately 90 % at 200 degrees C and 20 bar H-2; in contrast, the formation of benzene and the desired cyclohexane product appears to be structure insensitive. The introduction of acidity to the SBA-15 support promotes the demethyoxylation of the methoxycyclohexane intermediate, which increases the selectivity to cyclohexane from 15 to 92 % and the cyclohexane productivity by two orders of magnitude (from 15 to 6500 mmol g(Pt)(-1) h(-1)). Optimization of the metal-acid synergy confers an 865-fold increase in the cyclohexane production per gram of Pt and a 28-fold reduction in precious metal loading. These findings demonstrate that tuning the metal-acid synergy provides a strategy to direct complex catalytic reaction networks and minimize precious metal use in the production of bio-fuels.
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