Synthesis of Novel Aluminum Gallium Dihydrogen Phosphate Metal-Inorganic Framework and Its Catalytic Preparation of Butanolal from Acetaldehyde

Abstract

Abstract: Here, a novel aluminum-gallium-phosphate (GAHPO) metal-inorganic framework structure was prepared by hydrothermal method, and it was fully characterized by single crystal X-ray diffraction, powder X-ray diffraction, IR spectroscopy, and gravimetric analysis-differential scanning calorimeter (TG-DSC). Single crystal X-ray diffraction results show that GAHPO is attributed to the trigonal system and Rc3 space group. Al(Ga)O₆ octahedra and PO₄ tetrahedral structures is distorted to form one-dimensional chains, and then is stacked into three-dimensional metal-inorganic frameworks through hydrogen bonding. TG-DSC shows that GAHPO is of high thermal stability, with the initial decomposition temperature of 240 ℃. Compared with aluminum phosphate, the introduction of Ga³⁺ distorted the AlPO₄ lattice, thus weakening and elongating the Al—O bond, which makes more acid catalytic sites exposed and enhanced the catalytic activity. The experiment shows that when the reaction temperature is 60 ℃, and the catalyst dosage is 10% of acetaldehyde, GAHPO could catalyze the condensation of acetaldehyde to produce butanolal with good conversion rate (47%) and excellent selectivity (>99%). The reaction mechanism of acetaldehyde condensation catalyzed by GAHPO was investigated using scavengers, NH₃-TPD and specially designed derivatives to confirm the reactive sites of the catalyst and the substrate. This work provides a feasible way for novel aluminum inorganic framework structures and the catalytic applications.

Key words: aluminum-gallium-phosphate, hydrothermal synthesis, metal-inorganic framework, lattice distortion, catalysis, aldol condensation

CLC Number:

O643.3

CAO Yupeng, ZHANG Hanjie, HUANG Jiqing, GUO Wei, GONG Xubin, FANG Tao. Synthesis of Novel Aluminum Gallium Dihydrogen Phosphate Metal-Inorganic Framework and Its Catalytic Preparation of Butanolal from Acetaldehyde[J]. JOURNAL OF SYNTHETIC CRYSTALS, 2024, 53(4): 714-720.

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