Highly Active ZnO-ZrO2 Aerogels Integrated with H-ZSM-5 for Aromatics Synthesis from Carbon Dioxide,ACS Catalysis

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Highly Active ZnO-ZrO2 Aerogels Integrated with H-ZSM-5 for Aromatics Synthesis from Carbon Dioxide
ACS Catalysis ( IF 11.3 ) Pub Date : 2019-12-10 , DOI: 10.1021/acscatal.9b04309
Cheng Zhou ₁ , Jiaqing Shi ₁ , Wei Zhou ₁ , Kang Cheng ₁ , Qinghong Zhang ₁ , Jincan Kang ₁ , Ye Wang ₁

Affiliation

Bifunctional catalysis coupling CO₂ to methanol and methanol to hydrocarbons is a promising strategy for the direct hydrogenation of CO₂ into high-value chemicals. However, bifunctional catalysts suffer from low productivity due to the inertness of CO₂ and high activation energy of C–C coupling. Herein, we report a highly active bifunctional catalyst consisting of a ZnO-ZrO₂ aerogel and zeolite H-ZSM-5 for the hydrogenation of CO₂ into aromatics with 76% selectivity at a single-pass CO₂ conversion of 16%. The selectivity of CH₄ is lower than 1% at the same time. The space–time yield of aromatic hydrocarbons is as high as 0.24 g g_oxide^–1 h^–1 under the reaction conditions of 340 °C and 40 bar over ae-ZnO-ZrO₂/H-ZSM-5 catalyst, which outperforms the previously reported catalysts, including modified Fischer–Tropsch catalysts. We demonstrate that the ZnO-ZrO₂ aerogel catalyst, which is prepared by a combined sol–gel and subsequent supercritical drying method, not only possesses high surface area but also provides large amounts of oxygen vacancies. The formation rate of the methanol intermediate over ZnO-ZrO₂ is dominated by the total amount of oxygen vacancies. Moreover, the stable performance of the bifunctional catalyst under industrially relevant conditions suggests promising prospects for industrial applications.

中文翻译：

结合H-ZSM-5的高活性ZnO-ZrO ₂气凝胶，用于二氧化碳的芳烃合成

双功能催化耦合CO ₂至甲醇和甲醇的烃是直接氢化CO的有希望的策略₂转化成高价值化学品。但是，由于CO ₂的惰性和CC连接的高活化能，双功能催化剂的生产率较低。本文中，我们报道了由ZnO-ZrO ₂气凝胶和H-ZSM-5沸石组成的高活性双功能催化剂，可将CO ₂加氢成芳烃，其单程CO ₂转化率为16％，选择性为76 ％。同时CH ₄的选择性低于1％。芳烃的时空产率高达0.24 gg_氧化物在ae -ZnO-ZrO ₂ / H-ZSM-5催化剂上，在340°C和40 bar的反应条件下^–1 h ^–1，其性能优于以前报道的催化剂，包括改性的费-托催化剂。我们证明了通过组合的溶胶-凝胶法和随后的超临界干燥方法制备的ZnO-ZrO ₂气凝胶催化剂，不仅具有高的表面积，而且还提供了大量的氧空位。甲醇中间体在ZnO-ZrO _2上的形成速率主要由氧空位的总量决定。此外，双官能催化剂在工业上相关条件下的稳定性能表明工业应用前景广阔。

更新日期：2019-12-11

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