Phosphoric acid-modified commercial kieselguhr supported palladium nanoparticles as efficient catalysts for low-temperature hydrodeoxygenation of lignin derivatives in water
Abstract:Efficient production of high value-added chemicals and biofuels via low-temperature chemoselective HDO of lignin derivatives in water is still of challenge. Here, we construct a low-cost, active and stable Pd/PCE...
“…Vanillin is a typically lignin-derived aldehyde that can be manufactured on an industrial scale from biomass and converted into 2-methoxy-4-methylphenol (MMP), which has versatile applications in the fragrance industry and shows promise as an intermediate compound for pharmaceuticals. , To date, a considerable number of effective catalysts have been explored for the hydrodeoxygenation (HDO) of vanillin. − However, most of them used noble metals as the main component, resulting in their application being limited by high prices, which has drawn attention to reusable earth-abundant transition metal-based catalysts. − …”
Selective deoxygenation of chemicals using non-noble
metal-based
catalysts poses a significant challenge toward upgrading biomass-derived
oxygenates into advanced fuels and fine chemicals. Herein, we report
a bifunctional core–shell catalyst (Ni@Al3-mSiO2) consisting of Ni nanoparticles closely encapsulated by the
Al-doped mesoporous silica shell that achieves 100% vanillin conversion
and >99% yield of 2-methoxy-4-methylphenol under 1 MPa H2 at 130 °C in water. Due to the unique mesoporous core–shell
structure, no significant decrease in catalytic activity was observed
after 10 recycles. Furthermore, incorporating Al atoms into the silica
shell significantly increased the number of acidic sites. Density
functional theory calculations reveal the reaction pathway of the
vanillin hydrodeoxygenation process and uncover the intrinsic influence
of the Al sites. This work not only provides an efficient and cost-effective
bifunctional hydrodeoxygenation catalyst but also offers a new synthetic
protocol to rationally design promising non-noble metal catalysts
for biomass valorization or other widespread applications.
“…Vanillin (VAN) is regarded as a typical platform molecule derived from lignin. Selective conversion of VAN to 2-methoxy-4-methylphenol (MMP) has recently gained great attention since the produced MMP can be used as a promising substrate in biofuels and pharmaceuticals. − Many heterogeneous Pd-based catalysts have been designed for the efficient production of MMP from VAN. ,,− Zhang et al reported that >99% selectivity of MMP was obtained from VAN catalyzed by a 2.0 wt % Pd@NH 2 -UiO-66 catalyst at 100 °C for 1 h, and such an excellent catalytic performance was attributed to the synergistic catalysis between Pd nanoparticles (NPs) and the special metal–organic framework carrier . Lv et al reported that >99% MMP selectivity was achieved over a superhydrophilic mesoporous sulfonated melamine-formaldehyde catalyst at 110 °C for 2 h .…”
Selective and efficient low-temperature hydrodeoxygenation (HDO) of lignin derivatives in water for the production of valuable biofuel and chemicals is still challenging. Herein, we reported biomass carbon-supported ultrafine Pd nanoparticles as highly active and stable catalysts for low-temperature HDO of vanillin (a typical lignin-derived compound) to 2-methoxy-4methylphenol (MMP). We found that the abundant carboxyl groups on the resultant catalyst greatly accelerated the conversion of the generated intermediate (vanillyl alcohol, VAL), and then, the synergistic catalysis between carboxyl groups and Pd nanoparticles promoted the efficient production MMP through a free-radical pathway. Other lignin derivatives with different functional groups were also efficiently converted to the corresponding products over the prepared catalyst. This work may provide a new idea for designing a biomass-derived catalyst for efficient transformation of various lignin derivatives to produce value-added biofuels and chemicals.
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