Sun Wenjuan, Yang Zhenglong, Xu Yanbin, Shi Yawei, Shen Yongjie, Liu Guozhu
School of Chemistry and Materials Science, Ludong University 264025 Yantai Shandong Province China
State Key Laboratory of Separation Membranes and Membrane Processes, School of Environmental Science and Engineering, Tiangong University Tianjin 300387 China.
RSC Adv. 2020 Mar 31;10(22):12772-12779. doi: 10.1039/d0ra01576h. eCollection 2020 Mar 30.
Subnanometric Pd clusters confined within zeolite crystals was fabricated using zeolitic seeds with premade [PdCl(PPh)(PPh)] clusters under hydrothermal conditions. Characterization of the Pd@Beta catalysts indicate that the Pd clusters confined in the channels of Beta zeolite exhibit better dispersion and stronger interaction with the zeolite support, leading to stabilized Pd species after heat treatment by high temperature. In the model reaction of toluene combustion, the Pd@Beta outperforms both zeolite-supported Pd nanoparticles prepared by conventional impregnation of Pd/Beta and Pd/Beta. Temperatures for achieving toluene conversion of 5%, 50% and 98% of Pd@Beta are 136, 169 and 187 °C at SV = 60 000 mL g h, respectively. Pd@Beta could also maintain the catalytic reaction for more than 100 h at 230 °C without losing its activity, an important issue for practical applications. The metal-containing zeolitic seed directed synthesis of metal clusters inside zeolites endows the catalysts with excellent catalytic activity and high metal stability, thus providing potential avenues for the development of metal-encapsulated catalysts for VOCs removal.
在水热条件下,使用含有预制的[PdCl(PPh)(PPh)]簇的沸石晶种制备了限制在沸石晶体中的亚纳米级钯簇。对Pd@Beta催化剂的表征表明,限制在Beta沸石通道中的钯簇表现出更好的分散性以及与沸石载体更强的相互作用,从而在高温热处理后得到稳定的钯物种。在甲苯燃烧的模型反应中,Pd@Beta的性能优于通过传统浸渍法制备的沸石负载钯纳米颗粒以及Pd/Beta。在空速SV = 60 000 mL g h时,Pd@Beta实现甲苯转化率为5%、50%和98%的温度分别为136、169和187 °C。Pd@Beta在230 °C下还能保持催化反应100 h以上而不丧失活性,这对实际应用来说是一个重要问题。通过含金属的沸石晶种定向合成沸石内部的金属簇,赋予了催化剂优异的催化活性和高金属稳定性,从而为开发用于挥发性有机化合物去除的金属封装催化剂提供了潜在途径。