Ding Shengzhe, Fernandez Ainaga Dario Luis, Hu Min, Qiu Boya, Khalid Ushna, D'Agostino Carmine, Ou Xiaoxia, Spencer Ben, Zhong Xiangli, Peng Yani, Hondow Nicole, Theodoropoulos Constantinos, Jiao Yilai, Parlett Christopher M A, Fan Xiaolei
Department of Chemical Engineering, The University of Manchester, Manchester, M13 9PL, UK.
Institute of Catalysis Science, Beijing Research Institute of Chemical Industry, Sinopec, Beijing, 100013, China.
Nat Commun. 2024 Sep 4;15(1):7718. doi: 10.1038/s41467-024-51925-2.
Spatial control over features within multifunctional catalysts can unlock efficient one-pot cascade reactions, which are themselves a pathway to aviation biofuels via hydrodeoxygenation. A synthesis strategy that encompasses spatial orthogonality, i.e., one in which different catalytic species are deposited exclusively within discrete locations of a support architecture, is one solution that permits control over potential interactions between different sites and the cascade process. Here, we report a Pd doped hierarchical zeolite, in which Pd nanoparticles are selectively deposited within the mesopores, while acidity is retained solely within the micropores of ZSM-5. This spatial segregation facilitates hydrodeoxygenation while suppressing undesirable decarboxylation and decarbonation, yielding significant enhancements in activity (30.6 vs 3.6 mol mol h) and selectivity (C:C 5.2 vs 1.9) relative to a conventionally prepared counterpart (via wet impregnation). Herein, multifunctional material design can realise efficient fatty acid hydrodeoxygenation, thus advancing the field and inspiring future developments in rationalised catalyst design.
对多功能催化剂内的特征进行空间控制可以实现高效的一锅串联反应，而这种反应本身就是通过加氢脱氧生产航空生物燃料的一条途径。一种包含空间正交性的合成策略，即不同催化物种仅沉积在载体结构的离散位置内的策略，是一种能够控制不同位点之间潜在相互作用以及串联过程的解决方案。在此，我们报道了一种钯掺杂的分级沸石，其中钯纳米颗粒选择性地沉积在中孔内，而酸性仅保留在ZSM-5的微孔中。这种空间分离促进了加氢脱氧，同时抑制了不良的脱羧和脱碳反应，相对于传统制备的对应物（通过湿浸渍法），活性（30.6对3.6 mol mol h）和选择性（C:C 5.2对1.9）有显著提高。在此，多功能材料设计可以实现高效的脂肪酸加氢脱氧，从而推动该领域的发展，并为合理的催化剂设计带来未来的发展灵感。
