La3+阳离子交换催化乙酰丙酸水相加氢提高沸石Y的水热稳定性,RSC Advances

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La3+阳离子交换催化乙酰丙酸水相加氢提高沸石Y的水热稳定性
RSC Advances ( IF 3.9 ) Pub Date : 2021-1-29 , DOI: 10.1039/d0ra08907a
Hue-Tong Vu ₁ , Michael Goepel ₁ , Roger Gläser ₁

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La ³⁺阳离子交换可提高双功能沸石 Pt/Y 催化剂在以甲酸 (FA) 为氢源的乙酰丙酸 (LA) 水相加氢中的水热稳定性和催化活性。沸石Y( n _Si / n _Al = 16)的La ³⁺阳离子交换在水溶液和固态都进行。通过在自生压力下于 473 K暴露于反应混合物（0.2 mol L ^-1 LA，0.6 mol L ^{-1 FA）24 h 探测到的含 La}³⁺沸石 Y的水热稳定性随着 La 含量的增加而提高。La 含量最高的材料 (0.5 mmol g ^-1) 是最稳定的，在水热处理后保留了 25% 的初始比微孔体积，而未改性的沸石 Y 完全失去了其微孔性。使用 DRIFTS 的新程序是量化水热处理后 Y 型沸石骨架降解的有用补充工具。^{La 3+}阳离子交换后的双功能 Pt/Y 催化剂在LA 加氢生成 γ-戊内酯 (GVL) 方面比母体 Y-沸石更具活性，LA 转化率显着提高，即94%对42%，并且24 小时后的GVL 产率，即72%对34%。

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Improving the hydrothermal stability of zeolite Y by La3+ cation exchange as a catalyst for the aqueous-phase hydrogenation of levulinic acid

La³⁺ cation exchange is shown to improve the hydrothermal stability and catalytic activity of bifunctional zeolite Pt/Y catalysts in the aqueous-phase hydrogenation of levulinic acid (LA) with formic acid (FA) as hydrogen source. La³⁺ cation exchange of zeolite Y (n_Si/n_Al = 16) was conducted both in aqueous solution and in the solid state. The hydrothermal stability of La³⁺-containing zeolite Y probed by exposure to the reaction mixture (0.2 mol L⁻¹ LA, 0.6 mol L⁻¹ FA) at 473 K under autogenous pressure for 24 h improves with increasing La content. The material exhibiting the highest La content (0.5 mmol g⁻¹) is the most stable with a preservation of 25% of the initial specific micropore volume after the hydrothermal treatment, whereas unmodified zeolite Y completely loses its microporosity. A new procedure using DRIFTS is a useful supplementary tool for quantifying the framework degradation of Y-type zeolites after hydrothermal treatment. Bifunctional Pt/Y catalysts after La³⁺ cation exchange are more active than the parent Y-zeolite for the hydrogenation of LA to γ-valerolactone (GVL), with significant enhancements in LA conversion, i.e., 94% vs. 42%, and GVL yield, i.e., 72% vs. 34%., after 24 h.

更新日期：2021-01-29

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