Effect of n-Butanol Cofeeding on the Methanol to Aromatics Conversion over Ga-Modified Nano H-ZSM-5 and Its Mechanistic Interpretation,ACS Catalysis

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Effect of n-Butanol Cofeeding on the Methanol to Aromatics Conversion over Ga-Modified Nano H-ZSM-5 and Its Mechanistic Interpretation
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-01-19 00:00:00 , DOI: 10.1021/acscatal.7b03457
Weili Dai _{1,

2} , Liu Yang ₁ , Chuanming Wang ₃ , Xin Wang ₁ , Guangjun Wu _{1,

2} , Naijia Guan _{1,

2} , Utz Obenaus ₄ , Michael Hunger ₄ , Landong Li _{1,

2}

Affiliation

Ga-modified nano H-ZSM-5 zeolites with different Ga contents were prepared and applied as methanol-to-aromatics (MTA) catalysts. The Ga introduction can strongly increase the selectivity to aromatics but also decrease the catalyst lifetime simultaneously. Upon the cofeeding of n-butanol with methanol, a significant prolongation of the catalyst lifetime from 18 to ca. 50 h can be achieved. According to several spectroscopic results, e.g., TGA, GC–MS, in situ UV/vis, and solid-state MAS NMR spectroscopy, the addition of n-butanol during the MTA conversion shows no impact on the deactivation mechanism but can influence the dual-cycle mechanism. Namely, n-butanol preferentially adsorbs on Brønsted acid sites over methanol, followed by dehydration into n-butene. The formed n-butene can directly participate in the olefin-based cycle and, therefore, significantly alter the proportions of the dual-cycle mechanism. These results provide mechanistic insights into the roles of n-butanol cofeeding in the MTA conversion and exemplify a simple but efficient strategy to prolonged the catalyst lifetime, which is crucial to the industrial application.

中文翻译：

的效果Ñ丁醇共进料在甲醇以芳烃转化过Ga的改性纳米H-ZSM-5及其机理阐释

制备了具有不同Ga含量的Ga改性纳米H-ZSM-5沸石，并将其用作甲醇制芳烃（MTA）催化剂。Ga的引入可以极大地提高对芳族化合物的选择性，但是同时降低了催化剂的寿命。当正丁醇与甲醇共同进料时，催化剂的寿命从18显着延长到大约10分钟。可以达到50小时。根据TGA，GC-MS，原位UV / vis和固态MAS NMR光谱等光谱结果，MTA转化过程中添加正丁醇对失活机理没有影响，但会影响双重循环机制。即，正丁醇比甲醇优先吸附在布朗斯台德酸位上，然后脱水成正丁烯。形成的正丁烯可以直接参与基于烯烃的循环，因此会显着改变双循环机理的比例。这些结果为正丁醇共进料在MTA转化中的作用提供了机械方面的见解，并举例说明了延长催化剂寿命的简单而有效的策略，这对工业应用至关重要。

更新日期：2018-01-19

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