Li Houqian, Pang Jifeng, Hu Wenda, Caballero Vannessa, Sun Junming, Tan Mingwu, Hu Jian Zhi, Ni Yelin, Wang Yong
The Gene & Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University Pullman WA 99164 USA
Dalian Institute of Chemical Physics, Chinese Academy of Sciences No. 457 Zhongshan Road Dalian 116023 P.R. China.
Chem Sci. 2024 May 8;15(21):8031-8037. doi: 10.1039/d3sc06921d. eCollection 2024 May 29.
The selective formation of C-C bonds, coupled with effective removal of oxygen, plays a crucial role in the process of upgrading biomass-derived oxygenates into fuels and chemicals. However, co-feeding reactants with water is sometimes necessary to assist binding sites in catalytic reactions, thereby achieving desirable performance. Here, we report the design of a CeSnBeta catalyst featuring dual Lewis acidic sites for the efficient production of isobutene from acetone C-C coupling followed by deoxygenation. By incorporating Ce species onto SnBeta, which was synthesized through liquid-phase grafting of dealuminated Beta, we created confined dual Lewis acidic centers within Beta zeolites. The cooperative action of Ce species and framework Sn sites within this confined environment enabled selective catalysis of the acetone-to-isobutene cascade reactions, showcasing enhanced stability even without the presence of water.
碳-碳键的选择性形成，再加上有效地去除氧，在将生物质衍生的含氧化合物升级为燃料和化学品的过程中起着至关重要的作用。然而，有时需要将反应物与水共同进料以辅助催化反应中的结合位点，从而实现理想的性能。在此，我们报道了一种具有双路易斯酸性位点的CeSnBeta催化剂的设计，用于通过丙酮碳-碳偶联随后脱氧高效生产异丁烯。通过将铈物种引入经脱铝β沸石液相接枝合成的SnBeta上，我们在β沸石中创建了受限的双路易斯酸性中心。在这种受限环境中，铈物种与骨架锡位点的协同作用能够选择性催化丙酮到异丁烯的级联反应，即使在没有水的情况下也表现出增强的稳定性。
