本研究探討了以固態裂解法和氨氣氮化法合成氮化鎵並測試其對甲烷轉化為乙腈（ACN）之能力，固態裂解法將氮源與硝酸鎵前驅物進行超音波前處理，其中氮源包括三聚氰胺、蜜勒胺和g-C3N4，然後在800 °C下進行鍛燒；氨氣氮化法的氮化鎵觸媒通過含浸-鍛燒-氮化製備。製備的觸媒通過X光繞射（XRD）、X光吸收光譜（XAS）、氮氣等溫吸脫附（BET）、傅立葉轉換紅外光譜（FTIR）和X射線光電子能譜（XPS）進行鑑定。觸媒的活性在水平連續式固定化填充床反應器中進行測試，研究了鎵擔載量（固態裂解法製備觸媒為5% 和50%，氨氣氮化法製備觸媒為1%、3%、5% 和10%）、進料中加入H2和NH3以及載體（SiO2、S1和HZ）對觸媒的影響。在鍛燒後觀察到表面殘留CN物質，這些物質參與了甲烷轉化成ACN的反應，且氮化鎵小型晶體的存在可以提高ACN的產率，ACN通過甲基化表面的CN物質來生成。進料中H2和NH3的存在通過與甲烷的競爭吸附抑制了甲烷的轉化和ACN的產量，在甲烷轉化反應過程中，碳物質同時被生成，這些物質與氮化鎵表面的氮反應，形成了促進甲烷合成ACN的CN物質。

This work presented the synthesis of GaN by solid-state pyrolysis and ammonia nitridation methods and tested for methane conversion to acetonitrile (ACN). Nitrogen sources, including melamine, melem, and g-C3N4, were sonicated with gallium nitrate precursor and pyrolyzed at 800 °C. The ammonia-nitridized GaN catalysts were prepared by the impregnation-calcination-nitridation method. The prepared catalysts were characterized by X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), nitrogen adsorption (BET), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS) techniques. The activity of the catalysts was tested in a horizontal fixed-bed flow reactor. The effect of Ga loading (5 and 50% for solid-state made catalysts and 1, 3, 5, and 10% for ammonia nitridation catalysts), presence of H2 and NH3 in the feed, and supports (SiO2, S1, and HZ) were investigated. Surface CN residual species were observed after pyrolysis, which participated in methane conversion to ACN. The ACN productivity could be enhanced with the presence of small GaN crystallites. ACN was produced by methylation of surface CN species. The presence of H2 and NH3 in the feed stream suppressed both methane conversion and ACN productivity by competitive adsorption with methane. During the methane conversion reaction, carbonaceous species were concurrently produced. Such species interacted with the surface nitrogen of GaN, forming CN species that facilitated the ACN synthesis from methane.

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