Directional Construction of Active Naphthalenic Species within SAPO-34 Crystals toward More Efficient Methanol-to-Olefin Conversion.
Directional Construction of Active Naphthalenic Species within SAPO-34 Crystals toward More Efficient Methanol-to-Olefin Conversion.
复制标题
DOI：
10.1021/jacs.2c10495
复制
发表时间：
2022-10
影响因子：
15
通讯作者：
Chang Wang;Liu Yang;Mingbin Gao;Xue-Man Shao;W. Dai;Guangjun Wu;N. Guan;Zhaochao Xu;Mao Ye;Landong Li
中科院分区：
文献类型：
--
作者：
Chang Wang;Liu Yang;Mingbin Gao;Xue-Man Shao;W. Dai;Guangjun Wu;N. Guan;Zhaochao Xu;Mao Ye;Landong Li
烯烃选择性和催化剂寿命是工业甲醇制烯烃催化剂的两个关键指标。目前，很难同时获得高烯烃选择性和长催化剂寿命。在此基础上，提出了一种将预焦化和水蒸汽相结合的方法，在SAPO-34催化剂的晶中心定向构建萘系活性物种，不仅可以使催化剂的烯烃选择性提高到89%以上，而且可以使催化剂的寿命延长3.7倍。结构照明显微镜，原位紫外-可见光谱，和在线质谱阐明的时空分布和演化的萘物种在预煮和蒸煮过程中。这种“一石二鸟”的策略适用于含粘结剂的工业SAPO-34催化剂，展示了其在甲醇制烯烃工业中的光明前景。
Olefin selectivity and catalyst lifetime are two key metrics for industrial methanol-to-olefin catalysts. Currently, it is very difficult to obtain high olefin selectivity and long catalyst lifetime at the same time. Herein, a feasible strategy combining precoking and steaming to directionally construct the active naphthalenic species within the crystal center of the SAPO-34 catalyst has been developed, which can not only promote the lower olefin selectivity to ∼89% (ethylene and propylene) but also prolong the catalyst lifetime by ∼3.7-fold in the methanol-to-olefin conversion. Structured illumination microscopy, in situ ultraviolet-visible spectroscopy, and online mass spectrometry elucidate the spatiotemporal distribution and evolution of the naphthalenic species during the precoking and steaming processes. This one-stone-two-birds strategy is applicable to a commercial SAPO-34 catalyst containing a binder, demonstrating its bright prospect in the methanol-to-olefin industry.