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Efficient conversion of lignin to alkylphenols over highly stable inverse spinel MnFeO catalysts

《化学科学与工程前沿（英文）》 2023年第17卷第8期页码 1085-1095 doi: 10.1007/s11705-022-2236-1

摘要： The aromatic properties of lignin make it a promising source of valuable chemicals and fuels. Developing efficient and stable catalysts to effectively convert lignin into high-value chemicals is challenging. In this work, MnFe₂O₄ spinel catalysts with oxygen-rich vacancies and porous distribution were synthesized by a simple solvothermal process and used to catalyze the depolymerization of lignin in an isopropanol solvent system. The specific surface area was 110.5 m²∙g^–1, which substantially increased the active sites for lignin depolymerization compared to Fe₃O₄. The conversion of lignin reached 94%, and the selectivity of alkylphenols exceeded 90% after 5 h at 250 °C. Underpinned by characterizations, products, and density functional theory analysis, the results showed that the catalytic performance of MnFe₂O₄ was attributed to the composition of Mn and Fe with strong Mn–O–Fe synergy. In addition, the cycling experiments and characterization showed that the depolymerized lignin on MnFe₂O₄ has excellent cycling stability. Thus, our work provides valuable insights into the mechanism of lignin catalytic depolymerization and paves the way for the industrial-scale application of this process.

关键词： lignin depolymerization spinel catalysts hydrogenation

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Catalytic fast pyrolysis of walnut shell for alkylphenols production with nitrogen-doped activated carbon

Shanwei Ma, Hang Li, Guan Zhang, Tahir Iqbal, Kai Li, Qiang Lu

《环境科学与工程前沿（英文）》 2021年第15卷第2期 doi: 10.1007/s11783-020-1317-y

摘要： Abstract • N-doped activated carbon was prepared for catalytic pyrolysis of walnut shell. • Alkylphenols were selectively produced from catalytic pyrolysis process. • The alkylphenols yield increased by 8.5 times under the optimal conditions. • Formation mechanism of alkylphenols was proposed. Alkylphenols are a group of valuable phenolic compounds that can be derived from lignocellulosic biomass. In this study, three activated carbons (ACs) were prepared for catalytic fast pyrolysis (CFP) of walnut shell to produce alkylphenols, including nitrogen-doped walnut shell-derived activated carbon (N/WSAC), nitrogen-doped rice husk-derived activated carbon (N/RHAC) and walnut shell-derived activated carbon (WSAC). Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) experiments were carried out to reveal the influences of AC type, pyrolytic temperature, and AC-to-walnut shell (AC-to-WS) ratio on the product distributions. Results showed that with nitrogen doping, the N/WSAC possessed stronger capability than WSAC toward the alkylphenols production, and moreover, the N/WSAC also exhibited better effects than N/RHAC to prepare alkylphenols. Under the catalysis of N/WSAC, yields of alkylphenols were significantly increased, especially phenol, cresol and 4-ethylphenol. As the increase of pyrolytic temperature, the alkylphenols yield first increased and then decreased, while high selectivity could be obtained at low pyrolytic temperatures. Such a trend was also observed as the AC-to-WS ratio continuously increased. The alkylphenols production achieved a maximal yield of 44.19 mg/g with the corresponding selectivity of 34.7% at the pyrolytic temperature of 400°C and AC-to-WS ratio of 3, compared with those of only 4.67 mg/g and 6.1% without catalyst. In addition, the possible formation mechanism of alkylphenols was also proposed with the catalysis of N/WSAC.

关键词： Pyrolysis Walnut shell Alkylphenols Nitrogen-doped activated carbon