以HZSM-5为原料,采用γ-氨丙基三乙氧基硅烷(APTES)改性与高温氨气掺氮的两步法制备了氮化HZSM-5分子筛.采用元素分析、N2吸附、X射线衍射、原位漫反射红外等技术对材料的结构性能进行了研究.结果表明,经APTES改性后的掺氮HZSM-5分子筛的晶型结构保持完整,且孔结构保持良好.原位漫反射红外实验表明,改性的掺氮分子筛存在不同的氮物种,氮原子取代或部分取代氧原子,以-NH2、-NH-的形式进入分子筛骨架,形成Si-NH2、Si-NH-Al以及Si-NH2-Al物种.由此,提出了相应的掺氮机理:高温焙烧的过程中,有机胺的分解产生活性位,与氨气一起参与氮化反应,生成了相应的氮物种.程序升温脱附实验表明改性后的分子筛的强酸位急剧减少,而碱量增加.这种两步制备法有效地促进了氮原子的掺杂并进入骨架.
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