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Synergy of ultra-low-loaded ruthenium with alumina stimulating the catalytic hydrogenation of levulinic acid into γ-valerolactone
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-06-02 , DOI: 10.1016/j.cej.2023.143869
Zhenzhen Liu , Xueying Gao , Guoyong Song

Herein we report an efficient and recyclable catalyst combining extremely low-loaded Ru and abundant alumina supported on nitrogen-doped carbon (NC) for hydrogenation of cellulose-derived levulinic acid (LA) into valuable γ-valerolactone (GVL). The as-fabricated Ru0.18/Al2O3/NC shows extraordinarily catalytic efficiency in transforming LA to GVL under solvent-free conditions, achieving up to a 1.77 × 105 turnover number (TON) and a 26400 h−1 turnover frequency (TOF) in a single batch reaction, which is far better than other heterogeneous catalysts and comparable to the best optimized homogenous catalysts. This catalyst demonstrates a good stability and reusability, whose catalytic performance can be maintained in 22 times recycled reactions, thus reaching a 106-level value of total TONs. These results highlight the importance of the synergistic effects between infrequent Ru and abundant alumina, and provide an up-and-coming way to design more active and stable low Ru loading catalyst for such a transformation.



中文翻译:

超低载量钌与氧化铝协同促进乙酰丙酸催化加氢生成γ-戊内酯

在此,我们报道了一种高效且可回收的催化剂,将极低负载量的钌和丰富的氧化铝结合在氮掺杂碳(NC)上,用于将纤维素衍生的乙酰丙酸(LA)氢化成有价值的γ-戊内酯(GVL)。所制备的 Ru 0.18 /Al 2 O 3 /NC 在无溶剂条件下将 LA 转化为 GVL 时表现出非凡的催化效率,实现高达 1.77 × 10 5的周转数 (TON) 和 26400 h -1单批反应中的周转频率(TOF)远优于其他多相催化剂,可与最佳优化的均相催化剂相媲美。该催化剂表现出良好的稳定性和可重复使用性,在22次循环反应中仍能保持催化性能,从而达到10 6级的总TON值。这些结果凸显了稀有Ru和丰富氧化铝之间协同效应的重要性,并为设计更活性和稳定的低Ru负载催化剂用于此类转化提供了一种有前景的方法。

更新日期:2023-06-02
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