Wu Xueting, Liu Xinyi, Song Ye, Liu Wei, Deng Ruiping, Chu Xiang, Song Shuyan, Zhang Hongjie, Wang Xiao
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China.
School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China.
J Am Chem Soc. 2025 Jun 25;147(25):21907-21915. doi: 10.1021/jacs.5c05246. Epub 2025 Jun 12.
Chemical conversion of waste plastics into valuable products holds immense significance for pollution control and resource conservation. Dual-catalyst systems exhibit improved overall efficiency compared with conventional bifunctional catalysts in hydrocracking processes, but they continue to grapple with the issues of high noble metal loadings and the necessity for meticulously controlled synthesis steps. Herein, we propose a minimalist design for a dual-catalyst system that combines exceptional catalytic efficiency, minimal noble metal consumption, and a streamlined synthesis process. Specifically, Ce-modified HY (CeHY) and CeO-supported Rh (Rh-CeO) were directly blended as catalysts for low-density polyethylene (LDPE) hydrocracking. This blend achieves an ultrahigh liquid fuel formation rate of 3132 g/g/h, surpassing the previously reported dual-catalyst systems. Mechanistic analysis reveals that the enhanced performance mainly originates from unique interactions between CeO and Rh, which allows the coexistence of Rh single atoms (Rh) and Rh nanoparticles (Rh). These served as active sites for adsorbing olefin intermediates and activating H, respectively, thereby promoting the hydrogenation step. More significantly, considering the structural similarity between CeHY and commercial fluid catalytic cracking (FCC) catalysts, we further performed the catalysis using SOY-8 (a commercial FCC catalyst) and Rh-CeO, achieving equally excellent catalytic performance. The following 40-fold scale-up experiment firmly confirms the practical application prospect of our physically mixed catalytic system.
将废塑料化学转化为有价值的产品对于污染控制和资源保护具有重大意义。在加氢裂化过程中,与传统双功能催化剂相比,双催化剂体系展现出更高的整体效率,但它们仍面临着高贵金属负载量以及合成步骤需精细控制的问题。在此,我们提出一种双催化剂体系的极简设计,该体系兼具卓越的催化效率、最低的贵金属消耗以及简化的合成过程。具体而言,将铈改性的HY(CeHY)和氧化铈负载的铑(Rh-CeO)直接混合作为低密度聚乙烯(LDPE)加氢裂化的催化剂。这种混合物实现了3132 g/g/h的超高液体燃料生成速率,超过了先前报道的双催化剂体系。机理分析表明,性能的提升主要源于氧化铈与铑之间独特的相互作用,这使得铑单原子(Rh)和铑纳米颗粒(Rh)能够共存。它们分别作为吸附烯烃中间体和活化氢的活性位点,从而促进加氢步骤。更重要的是,考虑到CeHY与商业流化催化裂化(FCC)催化剂在结构上的相似性,我们进一步使用SOY-8(一种商业FCC催化剂)和Rh-CeO进行催化,获得了同样优异的催化性能。接下来的40倍放大实验有力地证实了我们物理混合催化体系的实际应用前景。