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MOF-Assisted Synthesis of Highly Mesoporous Cr2O3/SiO2 Nanohybrids for Efficient Lewis-Acid-Catalyzed Reactions
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2020-10-19 , DOI: 10.1021/acsami.0c15344 Fengfeng Chen 1 , Kui Shen 1 , Yitao Yang 1 , Haigen Huang 1 , Yingwei Li 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2020-10-19 , DOI: 10.1021/acsami.0c15344 Fengfeng Chen 1 , Kui Shen 1 , Yitao Yang 1 , Haigen Huang 1 , Yingwei Li 1
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The facile fabrication of porous solid acids is highly desired for replacing hazardous liquid acids for many acid-catalyzed reactions in the industry. Herein, we present a bottom-up strategy to construct ultrastable mesoporous Cr2O3/SiO2 nanohybrids (denoted as Meso-Cr–Si–O) with highly dispersed Lewis acid sites by pyrolysis of a SiO2@MIL-101 precursor prepared via nanocasting by a reverse double-solvent approach, which can guarantee the efficient encapsulation of SiO2 nanoparticles (NPs) inside the MIL-101 pores. The pore environment of Meso-Cr–Si–O can be well tuned by simply controlling the amount of silica within the MIL-101 pores and the pyrolysis temperature. Pyridine adsorption experiments demonstrate that the density of Lewis acidic sites in the obtained Meso-Cr–Si–O is much higher than that of MIL-101-derived Cr2O3 NPs. Benefitting from its highly mesoporous nanostructure with abundant acid sites, the optimal Meso-Cr–Si–O exhibits a significantly improved catalytic activity for the Lewis-acid-catalyzed Meerwein–Ponndorf–Verley reduction of cyclohexanone with 4.5 times higher yield of cyclohexanol than that of the MIL-101-derived Cr2O3 NPs, representing the first efficient Cr2O3-based catalytic system for this reaction.
中文翻译：
MOF辅助合成高介孔的Cr 2 O 3 / SiO 2纳米杂化物以有效进行路易斯酸催化反应
对于工业中许多酸催化反应而言，非常需要容易地制备多孔固体酸来代替有害液体酸。在这里，我们提出了一种自下而上的策略，通过热解制备的SiO 2 @ MIL-101前驱体来构建具有高度分散的路易斯酸位的超稳定介孔Cr 2 O 3 / SiO 2纳米杂化物（表示为Meso-Cr–Si–O）。通过反向双溶剂方法进行纳米浇铸，可以确保SiO 2的有效包封MIL-101孔内的纳米颗粒（NP）。只需控制MIL-101孔内的二氧化硅含量和热解温度，就可以很好地调节Meso-Cr-Si-O的孔环境。吡啶吸附实验表明，所得Meso-Cr-Si-O中Lewis酸性位点的密度远高于MIL-101衍生的Cr 2 O 3 NPs。得益于其高度介孔的纳米结构和丰富的酸位，最佳的Meso-Cr-Si-O表现出路易斯酸催化的Meerwein-Ponndorf-Verley还原环己酮的催化活性显着提高，比环己醇的收率高4.5倍。源自MIL-101的Cr 2 O 3 NP，代表第一个有效的Cr 2基于O 3的催化体系用于该反应。
更新日期：2020-10-29
中文翻译：
MOF辅助合成高介孔的Cr 2 O 3 / SiO 2纳米杂化物以有效进行路易斯酸催化反应
对于工业中许多酸催化反应而言，非常需要容易地制备多孔固体酸来代替有害液体酸。在这里，我们提出了一种自下而上的策略，通过热解制备的SiO 2 @ MIL-101前驱体来构建具有高度分散的路易斯酸位的超稳定介孔Cr 2 O 3 / SiO 2纳米杂化物（表示为Meso-Cr–Si–O）。通过反向双溶剂方法进行纳米浇铸，可以确保SiO 2的有效包封MIL-101孔内的纳米颗粒（NP）。只需控制MIL-101孔内的二氧化硅含量和热解温度，就可以很好地调节Meso-Cr-Si-O的孔环境。吡啶吸附实验表明，所得Meso-Cr-Si-O中Lewis酸性位点的密度远高于MIL-101衍生的Cr 2 O 3 NPs。得益于其高度介孔的纳米结构和丰富的酸位，最佳的Meso-Cr-Si-O表现出路易斯酸催化的Meerwein-Ponndorf-Verley还原环己酮的催化活性显着提高，比环己醇的收率高4.5倍。源自MIL-101的Cr 2 O 3 NP，代表第一个有效的Cr 2基于O 3的催化体系用于该反应。
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