Han Jian, Zhang Zongji, Hao Zongrui, Li Guicun, Liu Tong
College of Materials Science and Engineering, Qingdao University of Science and Technology, Zhengzhou Rd 53, Qingdao 266000, PR China; School of Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, PR China.
College of Materials Science and Engineering, Qingdao University of Science and Technology, Zhengzhou Rd 53, Qingdao 266000, PR China.
J Colloid Interface Sci. 2021 Apr;587:736-742. doi: 10.1016/j.jcis.2020.11.033. Epub 2020 Nov 13.
Selective dehydrogenation of formic acid is regarded as a universal strategy for providing a clean energy carrier (hydrogen, H) to reduce the dependence on fossil fuel. In this work, ultrafine PdAg nanoparticles (NPs) are successfully immobilized on NH-functionalized metal-organic framework MIL-101(Cr) by a facile wet-reduction method. By virtue of amine group, the size of obtained PdAg NPs can be controlled into 2.2 nm, which are monodispersed on NH-MIL-101(Cr) surface. In addition, the resulting PdAg NPs/NH-MIL-101(Cr) catalyst systems demonstrate excellent catalytic activity for formic acid decomposition in mild condition, the turn over frequency (TOF) value can achieve as high as 1475 h at 323 K, which is comparable to most of the reported noble metal heterogeneous catalysts for this catalytic reaction under similar conditions. The excellent catalytic kinetics is mainly attributed to the ultrafine size and high dispersion of PdAg NPs. Also, the amine group from NH-MIL-101(Cr) support facilitates the OH bond dissociation of formic acid and improves the kinetics of formic acid decomposition.
甲酸的选择性脱氢被视为一种提供清洁能源载体（氢气，H）以减少对化石燃料依赖的通用策略。在这项工作中，通过简便的湿还原法成功地将超细钯银纳米颗粒（NPs）固定在NH功能化的金属有机框架MIL-101（Cr）上。借助胺基，所得钯银纳米颗粒的尺寸可控制在2.2纳米，它们单分散在NH-MIL-101（Cr）表面。此外，所得的钯银纳米颗粒/NH-MIL-101（Cr）催化剂体系在温和条件下对甲酸分解表现出优异的催化活性，在323K时的周转频率（TOF）值可高达1475 h⁻¹，这与大多数报道的用于该催化反应的贵金属多相催化剂在类似条件下相当。优异的催化动力学主要归因于钯银纳米颗粒的超细尺寸和高分散性。此外，来自NH-MIL-101（Cr）载体的胺基促进了甲酸的OH键解离并改善了甲酸分解的动力学。
