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ZrO2 Promoted the Depolymerization of Lignin into Phenolic Monomers over 15Ni/SiO2–Al2O3–ZrO2 Catalyst
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2024-09-12 , DOI: 10.1021/acssuschemeng.4c03896 Dayi Guo 1 , Shuai Wang 1 , Shuailong Dong 1 , Junfeng Feng 1, 2 , Hui Pan 1, 2
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2024-09-12 , DOI: 10.1021/acssuschemeng.4c03896 Dayi Guo 1 , Shuai Wang 1 , Shuailong Dong 1 , Junfeng Feng 1, 2 , Hui Pan 1, 2
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Catalytic hydrogenation of lignin is one of the most effective methods for valorization of lignin to downstream aromatic compounds. However, the overhydrogenation of benzene rings during lignin hydrogenation could lower the selectivity of monomer aromatics. In this study, novel composite catalysts of Ni loaded on Zr-modified SiO2–Al2O3 support (Ni/SA-Zr) were prepared by simple wet impregnation methods for the reductive depolymerization of lignin. The as-prepared catalyst exhibited high catalytic activity to achieve 66.7% yield of lignin oil and 60.5% lignin monomer. Also, the phenolic selectivity was up to 80.1% under optimal conditions (catalyst 15Ni/SA-Zr, 260 °C, 2 MPa H2, 4 h). The presence of ZrO2 not only improved the catalytic activity of the Ni/SA-Zr catalyst but also inhibited the hydrogenation of the benzene ring. The characterization of the Ni/SA-Zr catalyst showed that the introduction of ZrO2 was beneficial to the dispersion of metallic Ni on the surface of the catalyst. In addition, the interaction between the Ni metal and the support was weakened due to the presence of ZrO2, which was believed to be the main reason for the high activity of the Ni/SA-Zr catalyst in the lignin depolymerization. The results of X-ray photoelectron spectrometry analysis showed that electron-rich Ni species favored the adsorption of hydrogen. However, excess ZrO2 would reduce the activity of the catalyst. The two-dimensional 13C–1H heteronuclear single quantum correlation-nuclear magnetic resonance characterization of lignin samples before and after the depolymerization reaction confirmed that lignin was converted to monomeric phenols effectively. Based on the reaction path of the lignin model compound 2-phenoxy-1-phenylethanol, a possible reaction path of lignin depolymerization was proposed.
中文翻译：
ZrO2 在 15Ni/SiO2–Al2O3–ZrO2 催化剂上促进木质素解聚成酚类单体
木质素催化加氢是将木质素转化为下游芳香族化合物的最有效方法之一。然而，木质素加氢过程中苯环的过度加氢会降低单体芳烃的选择性。本研究采用简单的湿浸渍方法制备了负载于Zr改性SiO 2 -Al 2 O 3载体(Ni/SA-Zr)的新型复合催化剂，用于木质素的还原解聚。所制备的催化剂表现出较高的催化活性，木质素油收率达到66.7%，木质素单体收率达到60.5%。在最佳条件下（催化剂15Ni/SA-Zr，260℃，2MPa H 2 ，4h），酚类选择性高达80.1%。 ZrO 2的存在不仅提高了Ni/SA-Zr催化剂的催化活性，而且抑制了苯环的加氢反应。 Ni/SA-Zr催化剂的表征表明，ZrO 2的引入有利于金属Ni在催化剂表面的分散。此外，由于ZrO 2的存在，Ni金属与载体之间的相互作用减弱，这被认为是Ni/SA-Zr催化剂在木质素解聚中具有高活性的主要原因。 X射线光电子能谱分析结果表明，富电子的Ni物种有利于氢的吸附。然而，过量的ZrO 2会降低催化剂的活性。 解聚反应前后木质素样品的二维13 C- 1 H 异核单量子关联-核磁共振表征证实木质素有效地转化为单体酚。基于木质素模型化合物2-苯氧基-1-苯基乙醇的反应路径，提出了木质素解聚可能的反应路径。
更新日期：2024-09-12
中文翻译：
ZrO2 在 15Ni/SiO2–Al2O3–ZrO2 催化剂上促进木质素解聚成酚类单体
木质素催化加氢是将木质素转化为下游芳香族化合物的最有效方法之一。然而，木质素加氢过程中苯环的过度加氢会降低单体芳烃的选择性。本研究采用简单的湿浸渍方法制备了负载于Zr改性SiO 2 -Al 2 O 3载体(Ni/SA-Zr)的新型复合催化剂，用于木质素的还原解聚。所制备的催化剂表现出较高的催化活性，木质素油收率达到66.7%，木质素单体收率达到60.5%。在最佳条件下（催化剂15Ni/SA-Zr，260℃，2MPa H 2 ，4h），酚类选择性高达80.1%。 ZrO 2的存在不仅提高了Ni/SA-Zr催化剂的催化活性，而且抑制了苯环的加氢反应。 Ni/SA-Zr催化剂的表征表明，ZrO 2的引入有利于金属Ni在催化剂表面的分散。此外，由于ZrO 2的存在，Ni金属与载体之间的相互作用减弱，这被认为是Ni/SA-Zr催化剂在木质素解聚中具有高活性的主要原因。 X射线光电子能谱分析结果表明，富电子的Ni物种有利于氢的吸附。然而，过量的ZrO 2会降低催化剂的活性。 解聚反应前后木质素样品的二维13 C- 1 H 异核单量子关联-核磁共振表征证实木质素有效地转化为单体酚。基于木质素模型化合物2-苯氧基-1-苯基乙醇的反应路径，提出了木质素解聚可能的反应路径。
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