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首页> 外文期刊>RSC Advances >Cascade reaction engineering on zirconia-supported mesoporous MFI zeolites with tunable Lewis-Bronsted acid sites: a case of the one-pot conversion of furfural to gamma-valerolactone
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Cascade reaction engineering on zirconia-supported mesoporous MFI zeolites with tunable Lewis-Bronsted acid sites: a case of the one-pot conversion of furfural to gamma-valerolactone

机译：氧化锆的级联反应工程支持的中孔MFI沸石，具有可调谐路易斯 - 勃朗斯酸酸盐酸地：一种糠醛对γ-戊烯酮的单罐转化的情况

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摘要

Catalytic cascade reactions are strongly desired as a potential means of combining multistep reactions into a single catalytic reactor. Appropriate catalysts composed of multi-reactive sites to catalyze cascade reactions in a sequential fashion are central to such efforts. Here, we demonstrate a bifunctional zeolite catalyst with close proximity of Bronsted and Lewis acid sites through the synthesis of a mesoporous ZrO2[Al]MFI nanosponge (NS). The unique mesopores of the MFI-NS allow the confinement of zirconium oxide clusters (Lewis acid sites, LA) within the few-unit-cell-thin MFI aluminosilicate zeolite wall (Bronsted acid sites, BA). Such a structure is clearly distinct from the conventional MFI zeolite, where the agglomeration of zirconium oxide clusters onto the external surface area within the crystal bulk is not possible, resulting in segregated BA and LA sites on the internal and external zeolite, respectively. By bringing the BA and LA within ZrO2[Al]MFI-NS 30, we uncovered a more efficient catalytic route for the conversion of furfural (100% within 2 h) to gamma-valerolactone (GVL) (83%). This route is only evident when the long molecular diffusion path, in the most extreme case of physically mixed ZrO2-(LA) and Al-zeolites (BA) (45% of GVL yield), is eliminated. Unlike the bifunctional ZrO2-Al-beta (GVL yield of 75%), where the BA concentration is greatly compromised at the expense of LA formation, we also show that the ZrO2[Al]MFI-NS is able to maintain a high density and good stability of both types of acids.
机译：强烈需要催化级联反应作为将多体反应组合成单一催化反应器的潜在方法。由多反应部位组成的适当催化剂以促进顺序方式催化级联反应是这种努力的核心。在这里，我们通过合成介孔ZrO2 [Al] MFI纳米术（NS），证明了一种双官能沸石催化剂，其具有靠近伪造和路易斯酸部位。 MFI-NS的独特疏孔允许在少量单元 - 细胞薄MFI硅铝硅酸盐岩岩（Bronsted酸位，Ba）内限制氧化锆簇（Lewis酸部位，La）。这种结构明显不同于传统的MFI沸石，其中氧化锆簇的附聚在晶体体内的外表面积上是不可能的，导致内部和外部沸石上的隔离的Ba和La位点。通过使BA和La在ZrO2 [Al] MFI-NS 30中，我们发现更有效的催化途径，用于将糠醛（2小时内100％）转化为γ-戊内酯（GV1）（83％）。当长分子扩散路径在物理混合的ZrO2-（La）和Al-沸石（Ba）（占GVL产量的45％）的最极端情况下，该途径仅是明显的。与双官能ZrO2-Al-β（GVL产率为75％）不同，其中BA浓度以牺牲La形成为代价大大损害，我们还表明ZrO2 [Al] MFI-NS能够保持高密度和两种类型的酸稳定性。

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  • 来源
    《RSC Advances》 |2020年第58期|共11页
  • 作者

    Kim Kyung Duk; Kim Jaeheon; Teoh Wey Yang; Kim Jeong-Chul; Huang Jun; Ryoo Ryong;

  • 作者单位

    Inst Basic Sci IBS Ctr Nanomat &

    Chem React Daejeon 34141 South Korea;

    Inst Basic Sci IBS Ctr Nanomat &

    Chem React Daejeon 34141 South Korea;

    Univ New South Wales Sch Chem Engn Sydney NSW 2052 Australia;

    Inst Basic Sci IBS Ctr Nanomat &

    Chem React Daejeon 34141 South Korea;

    Univ Sydney Sch Chem &

    Biomol Engn Lab Catalysis Engn Sydney Nano Inst Sydney NSW 2006 Australia;

    Inst Basic Sci IBS Ctr Nanomat &

    Chem React Daejeon 34141 South Korea;

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  • 正文语种 eng
  • 中图分类 化学;
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