Facile synthesis of shaped ZSM-5 with high-proportioned accessible acid sites toward superior coke resistance in methanol-to-hydrocarbon reaction

IF 6.7 1区工程技术 Q2 ENERGY & FUELS

Fuel Pub Date : 2025-04-26 DOI:10.1016/j.fuel.2025.135367

Lingzhen Bu, Yaquan Wang, Wenrong Liu, Kailiang Chu, Niandong Guo, Yitong Huang, Liping Qu, Xuemei Su, Xian Zhang, Yaoning Li

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Abstract

The shaped hierarchical ZSM-5 zeolites with high-proportioned accessible acid sites were directly synthesized via a one-step synthesis strategy, aimed at improving catalytic stability. The pore structure, acid distribution and acid properties could be effectively tailored just by regulating aluminum sources. The ZSM-5 synthesized with aluminum nitrate and aluminum isopropoxide possessed less accessible acid sites (despite their large acid amount), stronger acid strength and less mesopores. Regarding the ZSM-5 prepared with aluminum hydroxide, suitable acid strength, remarkably increased intracrystalline mesopores coupled with a marked increase in accessible acid sites endowed it a dramatically improved acid site efficiency (at least 3 times that of other catalysts), satisfactory yields of liquid hydrocarbons (86.84 g·g_cat^-1) and C_2-3 olefins (85.95 g·g_cat^-1), and optimal coke resistance (at least 3-fold lifetime of other catalysts) in methanol to hydrocarbon reaction. This work offers a facile strategy for tuning pore structure, acid distribution and acid properties of zeolites and paves a feasible route for the large-scale application.

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具有高比例可及酸位的异型ZSM-5在甲醇-烃反应中具有优异的抗焦性

通过一步法直接合成了具有高比例可达酸位的ZSM-5分子筛，旨在提高催化稳定性。通过调节铝源，可以有效地调整孔隙结构、酸分布和酸性质。由硝酸铝和异丙醇铝合成的ZSM-5具有较少的可达酸位（尽管酸量大），较强的酸强度和较少的介孔。以氢氧化铝为原料制备的ZSM-5，酸强度适宜，晶内介孔显著增加，酸位可达性显著增加，酸位效率显著提高（至少是其他催化剂的3倍），液相烃产率（86.84 g·gcat-1）和C2-3烯烃产率（85.95 g·gcat-1）令人满意，在甲醇中对烃类反应具有最佳的抗焦性（至少是其他催化剂寿命的3倍）。该研究为调整沸石的孔隙结构、酸分布和酸性质提供了一种简便的策略，为大规模应用铺平了可行的途径。

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来源期刊

Fuel 工程技术-工程：化工

CiteScore

12.80

自引率

20.30%

发文量

3506

审稿时长

64 days

期刊介绍： The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.