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Enhancing the Stability of Methanol-to-Olefins Reaction Catalyzed by SAPO-34 Zeolite in the Presence of CO2 and Oxygen-Vacancy-Rich ZnCeZrOx
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-12-27 , DOI: 10.1021/acscatal.3c04707 Ke Ma 1 , Siyuan Zhao 1 , Meixin Dou 1 , Xiaoxun Ma 1 , Chengyi Dai 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-12-27 , DOI: 10.1021/acscatal.3c04707 Ke Ma 1 , Siyuan Zhao 1 , Meixin Dou 1 , Xiaoxun Ma 1 , Chengyi Dai 1
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In the methanol-to-olefins (MTO) reaction, coke deposition is a key factor that reduces the catalyst stability. Consequently, this work proposes a strategy: conducting the MTO reaction catalyzed by ZnCeZrOx/SAPO-34 in the presence of CO2 to suppress coke deposition and thus improve the catalyst lifetime. Under a CO2 atmosphere, compared to pristine SAPO-34, the composite catalyst of SAPO-34 and ZnCeZrOx with abundant oxygen vacancies has a 3.4 times longer lifetime and a selectivity to light olefins (C2=-C4=) of 87.1%. The results of various characterization techniques and experiments show that the oxygen vacancies of ZnCeZrOx adsorb and activate CO2, providing active oxygen species for the MTO reaction. The active oxygen species selectively oxidize formaldehyde, thereby blocking the reaction of formaldehyde and olefins to polycyclic aromatic hydrocarbons through the Prins reaction. At the same time, the active oxygen species reduce the amounts of polymethylbenzene and polymethylnaphthalene (coke deposit precursors) in situ during the reaction, thereby significantly improving catalyst stability. The above process simultaneously suppresses the aromatic-based cycle, thereby effectively adjusting the ratio of the aromatic-based cycle to the olefin-based cycle and achieving high propylene and butene selectivity. This work provides an effective strategy for improving the catalyst lifetime and controlling product distribution.
中文翻译：
提高 CO2 和富氧空位 ZnCeZrOx 存在下 SAPO-34 沸石催化的甲醇制烯烃反应的稳定性
在甲醇制烯烃（MTO）反应中，积炭是降低催化剂稳定性的关键因素。因此，本工作提出了一种策略：在CO 2存在下进行ZnCeZrO x /SAPO-34催化的MTO反应以抑制焦炭沉积，从而提高催化剂寿命。在CO 2气氛下，与原始SAPO-34相比，SAPO-34和具有丰富氧空位的ZnCeZrO x复合催化剂的寿命延长了3.4倍，对轻质烯烃的选择性（C 2 = -C 4 =）为87.1 %。各种表征技术和实验结果表明，ZnCeZrO x的氧空位吸附并活化CO 2，为MTO反应提供活性氧物种。活性氧选择性地氧化甲醛，从而阻止甲醛与烯烃通过普林斯反应生成多环芳烃。同时，活性氧物质在反应过程中原位减少了多甲苯和多甲基萘（焦炭沉积物前体）的量，从而显着提高了催化剂稳定性。上述方法同时抑制了芳族环，从而有效地调节了芳族环与烯烃环的比例，实现了丙烯和丁烯的高选择性。这项工作为提高催化剂寿命和控制产物分布提供了有效的策略。
更新日期：2023-12-27
中文翻译：
提高 CO2 和富氧空位 ZnCeZrOx 存在下 SAPO-34 沸石催化的甲醇制烯烃反应的稳定性
在甲醇制烯烃（MTO）反应中，积炭是降低催化剂稳定性的关键因素。因此，本工作提出了一种策略：在CO 2存在下进行ZnCeZrO x /SAPO-34催化的MTO反应以抑制焦炭沉积，从而提高催化剂寿命。在CO 2气氛下，与原始SAPO-34相比，SAPO-34和具有丰富氧空位的ZnCeZrO x复合催化剂的寿命延长了3.4倍，对轻质烯烃的选择性（C 2 = -C 4 =）为87.1 %。各种表征技术和实验结果表明，ZnCeZrO x的氧空位吸附并活化CO 2，为MTO反应提供活性氧物种。活性氧选择性地氧化甲醛，从而阻止甲醛与烯烃通过普林斯反应生成多环芳烃。同时，活性氧物质在反应过程中原位减少了多甲苯和多甲基萘（焦炭沉积物前体）的量，从而显着提高了催化剂稳定性。上述方法同时抑制了芳族环，从而有效地调节了芳族环与烯烃环的比例，实现了丙烯和丁烯的高选择性。这项工作为提高催化剂寿命和控制产物分布提供了有效的策略。
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