Organic and Nano Group (ONG), Department of Chemistry, Faculty of Science, University of Maragheh, PO BOX 55181-83111, Maragheh, Iran.
Organic and Nano Group (ONG), Department of Chemistry, Faculty of Science, University of Maragheh, PO BOX 55181-83111, Maragheh, Iran.
J Colloid Interface Sci. 2020 May 1;567:126-135. doi: 10.1016/j.jcis.2020.01.087. Epub 2020 Feb 1.
Ultra-small nano-sized palladium particles were successfully stabilized within the pores of diamine groups grafted open metal site metal-organic frameworks of Cr-MIL-101; coordinated diamine groups of ethylene diamine (ED) and propyl diamine (PD) on the active site of chromium units of Cr-MIL-101. The physiochemical properties of the Pd@Cr-MOFs were investigated using FTIR, XRD, SEM/EDX mapping, TEM, BET, and AAS. The Cr-MIL-101 stabilized ultra-small Pd nanoparticles, Pd@(ethylene diamine)/Cr-MIL-101, and Pd@(propyl diamine)/Cr-MIL-101, displayed catalytic activity for clean dehydrogenation of formic acid and generation of hydrogen at room temperature. The resultant Pd@ED/Cr-MIL-101 catalyst indicates high catalytic activity with turnover frequency (TOF) of 583 h at 328 K, which is superior to most of the reported catalysts, including Pd@PD/Cr-MIL-101 with TOF 532 h. Our studies open up a new method to the design of an ultra-small metal nanoparticle for the catalytic dehydrogenation of HCOOH.
成功地将超小纳米钯粒子稳定在接枝有二胺基团的开金属位金属有机骨架的孔内；二胺基团与 Cr-MIL-101 中铬单元的活性位点配位，二胺基团为乙二胺（ED）和丙二胺（PD）。使用 FTIR、XRD、SEM/EDX 映射、TEM、BET 和 AAS 研究了 Pd@Cr-MOFs 的物理化学性质。Cr-MIL-101 稳定的超小 Pd 纳米粒子、Pd@（乙二胺）/Cr-MIL-101 和 Pd@（丙二胺）/Cr-MIL-101 在室温下对甲酸的清洁脱氢和氢气的生成表现出催化活性。所得的 Pd@ED/Cr-MIL-101 催化剂在 328 K 时具有 583 h-1 的高催化活性，高于大多数报道的催化剂，包括 Pd@PD/Cr-MIL-101 的 532 h-1。我们的研究为设计用于 HCOOH 催化脱氢的超小金属纳米粒子开辟了一条新途径。
