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Boosting Conversion of CO2 to Light Olefins over MgO-Promoted ZnZrO/SAPO-34 Bifunctional Catalyst
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2023-06-01 , DOI: 10.1021/acs.iecr.3c00465 Lizhi Zhang 1, 2 , Zhihua Cao 1 , Ziliang Gao 3 , Wenming Liu 1 , Yiru Mao 1 , Miao Li 1 , Honggen Peng 1, 2, 3
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2023-06-01 , DOI: 10.1021/acs.iecr.3c00465 Lizhi Zhang 1, 2 , Zhihua Cao 1 , Ziliang Gao 3 , Wenming Liu 1 , Yiru Mao 1 , Miao Li 1 , Honggen Peng 1, 2, 3
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CO2 hydrogenation to produce light olefins is a hopeful route to the cyclic utilization of CO2. Although metal oxide/zeolite bifunctional catalysts show outstanding performance for CO2 hydrogenation to olefins, they still expect to further improve its performance. Here, a ternary metal oxide solid solution catalyst by incorporating MgO into ZnZrO to adjust the acid and redox active sites and coupled with SAPO-34 zeolite (noted as Mg-ZnZrO/SAPO-34) was developed. The Mg-ZnZrO/SAPO-34 catalyst exhibits light olefins yield of 5.7% that higher than those of ZnZrO/SAPO-34 catalyst (4.5%) at 390 °C. The results discovered that the introduction of MgO can neutralize the strong acid site of zeolite and generate more oxygen vacancies, and exhibit superior ability to adsorb and activate CO2 and H2. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) demonstrate that carbonate formation by CO2 adsorption of doped MgO and participation in the reaction to form more HCOO* and CH3O* species on the Mg-ZnZrO/SAPO-34 catalyst. The strategy via adjusting the acid intensity and the content of oxygen vacancies developed in this work supplies a guideline to design high-performance catalysts for CO2 utilization.
中文翻译：
MgO 促进的 ZnZrO/SAPO-34 双功能催化剂促进 CO2 向轻质烯烃的转化
CO 2加氢制低碳烯烃是CO 2循环利用的一条有希望的途径。尽管金属氧化物/沸石双功能催化剂对 CO 2表现出突出的性能加氢制烯烃，他们仍然期望进一步提高其性能。在这里，开发了一种三元金属氧化物固溶体催化剂，通过将 MgO 掺入 ZnZrO 以调节酸和氧化还原活性位点并与 SAPO-34 沸石偶联（记为 Mg-ZnZrO/SAPO-34）。在 390 °C 时，Mg-ZnZrO/SAPO-34 催化剂的轻质烯烃产率为 5.7%，高于 ZnZrO/SAPO-34 催化剂（4.5%）。结果发现，MgO的引入可以中和沸石的强酸性部位，产生更多的氧空位，表现出优异的吸附和活化CO 2和H 2的能力。原位漫反射红外傅立叶变换光谱 (DRIFTS) 表明 CO 2形成碳酸盐Mg-ZnZrO/SAPO-34 催化剂吸附掺杂的 MgO 并参与反应形成更多的 HCOO* 和 CH 3 O* 物种。在这项工作中开发的通过调节酸强度和氧空位含量的策略为设计用于 CO 2利用的高性能催化剂提供了指导。
更新日期：2023-06-01
中文翻译：
MgO 促进的 ZnZrO/SAPO-34 双功能催化剂促进 CO2 向轻质烯烃的转化
CO 2加氢制低碳烯烃是CO 2循环利用的一条有希望的途径。尽管金属氧化物/沸石双功能催化剂对 CO 2表现出突出的性能加氢制烯烃，他们仍然期望进一步提高其性能。在这里，开发了一种三元金属氧化物固溶体催化剂，通过将 MgO 掺入 ZnZrO 以调节酸和氧化还原活性位点并与 SAPO-34 沸石偶联（记为 Mg-ZnZrO/SAPO-34）。在 390 °C 时，Mg-ZnZrO/SAPO-34 催化剂的轻质烯烃产率为 5.7%，高于 ZnZrO/SAPO-34 催化剂（4.5%）。结果发现，MgO的引入可以中和沸石的强酸性部位，产生更多的氧空位，表现出优异的吸附和活化CO 2和H 2的能力。原位漫反射红外傅立叶变换光谱 (DRIFTS) 表明 CO 2形成碳酸盐Mg-ZnZrO/SAPO-34 催化剂吸附掺杂的 MgO 并参与反应形成更多的 HCOO* 和 CH 3 O* 物种。在这项工作中开发的通过调节酸强度和氧空位含量的策略为设计用于 CO 2利用的高性能催化剂提供了指导。
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