Shape-selective synthesis of para-xylene through tandem CO2 hydrogenation and toluene methylation over ZnCeZrOx/MCM-22 catalyst

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis Pub Date : 2025-06-01 DOI:10.1016/S1872-2067(25)64668-7

Jie Tuo , Zhenteng Sheng , Xianchen Gong , Qi Yang , Peng Wu , Hao Xu

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引用次数: 0

Abstract

Selective synthesis of value-added xylenes and para-xylene (PX) by CO₂ hydrogenation reduces the dependence on fossil resource and relieves the environment burden derived from the greenhouse gas CO₂. Herein, modified MCM-22 zeolite combined with ZnCeZrO_x solid solution is reported to catalyze the tandem CO₂ hydrogenation and toluene methylation reaction at a relatively low temperature (< 603 K), showing xylene selectivity of 92.4% and PX selectivity of 62% (PX/X, 67%) in total aromatics at a CO₂ conversion of 7.7%, toluene conversion of 23.6% and low CO selectivity of 11.6%, as well as giving high STY of xylene (302.0 mg·h^–1·g_cat^–1) and PX (201.6 mg·h^–1·g_cat^–1). The outstanding catalytic performances are closely related to decreased pore sizes and eliminated external surface acid sites in modified MCM-22, which promoted zeolite shape-selectivity and suppressed secondary reactions.

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ZnCeZrOx/MCM-22催化剂上CO2加氢和甲苯甲基化串联合成对二甲苯

通过CO2加氢选择性合成附加值二甲苯和对二甲苯（PX），降低了对化石资源的依赖，减轻了温室气体CO2带来的环境负担。本文报道了改性MCM-22沸石与ZnCeZrOx固溶体结合，在较低温度下催化CO2加氢-甲苯甲基化反应(<；在CO2转化率为7.7%、甲苯转化率为23.6%、低CO选择性为11.6%的条件下，二甲苯的选择性为92.4%，PX的选择性为62% (PX/X为67%)，二甲苯的选择性为302.0 mg·h-1·gcat-1， PX的选择性为201.6 mg·h-1·gcat-1)。改性后的MCM-22具有优异的催化性能，这与改性后的MCM-22减小了分子筛孔径，消除了外表面酸位密切相关，从而提高了分子筛的形状选择性，抑制了二次反应。

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来源期刊

Chinese Journal of Catalysis 工程技术-工程：化工

CiteScore

25.80

自引率

10.30%

发文量

235

审稿时长

1.2 months

期刊介绍： The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.