Nguyen Michelle A, Zahran Elsayed M, Wilbon Azaan S, Besmer Alexander V, Cendan Vincent J, Ranson William A, Lawrence Randy L, Cohn Joshua L, Bachas Leonidas G, Knecht Marc R
Department of Chemistry, University of Miami , 1301 Memorial Drive, Coral Gables, Florida 33146, United States.
Department of Physics, University of Miami , 1320 Campo Sano Drive, Coral Gables, Florida 33146, United States.
ACS Omega. 2016 Jul 31;1(1):41-51. doi: 10.1021/acsomega.6b00076. Epub 2016 Jul 6.
We report a synthetic approach to form cubic CuO/Pd composite structures and demonstrate their use as photocatalytic materials for tandem catalysis. Pd nanoparticles were deposited onto CuO cubes, and their tandem catalytic reactivity was studied via the reductive dehalogenation of polychlorinated biphenyls. The Pd content of the materials was gradually increased to examine its influence on particle morphology and catalytic performance. Materials were prepared at different Pd amounts and demonstrated a range of tandem catalytic reactivity. H was generated via photocatalytic proton reduction initiated by CuO, followed by Pd-catalyzed dehalogenation using generated H. The results indicate that material morphology and composition and substrate steric effects play important roles in controlling the overall reaction rate. Additionally, analysis of the postreacted materials revealed that a small number of the cubes had become hollow during the photodechlorination reaction. Such findings offer important insights regarding photocatalytic active sites and mechanisms, providing a pathway toward converting light-based energy to chemical energy for sustainable catalytic reactions not typically driven via light.
我们报道了一种合成立方CuO/Pd复合结构的方法,并展示了其作为串联催化光催化材料的用途。将钯纳米颗粒沉积在氧化铜立方体上,并通过多氯联苯的还原脱卤研究了它们的串联催化反应活性。逐渐增加材料中的钯含量,以研究其对颗粒形态和催化性能的影响。制备了不同钯含量的材料,并展示了一系列的串联催化反应活性。通过氧化铜引发的光催化质子还原产生氢气,然后使用产生的氢气进行钯催化的脱卤反应。结果表明,材料形态、组成和底物空间效应在控制总反应速率中起着重要作用。此外,对反应后材料的分析表明,在光脱氯反应过程中有少量立方体变成了中空结构。这些发现为光催化活性位点和机理提供了重要见解,为将光能转化为化学能以实现通常不由光驱动的可持续催化反应提供了一条途径。