Martínez-Vargas Adrián, Vásquez-López Alfonso, Antonio-Ruiz Carlos D, Cruz-Martínez Heriberto, Medina Dora I, Montejo-Alvaro Fernando
Tecnológico Nacional de México, Instituto Tecnológico del Valle de Etla, Abasolo S/N, Barrio del Agua Buena, Santiago Suchilquitongo 68230, Oaxaca, Mexico.
Instituto Politécnico Nacional, CIIDIR-OAXACA, Hornos Núm 1003, Col. Noche Buena, Santa Cruz Xoxocotlán 71230, Oaxaca, Mexico.
Materials (Basel). 2022 Jul 5;15(13):4710. doi: 10.3390/ma15134710.
Graphene with defects is a vital support material since it improves the catalytic activity and stability of nanoparticles. Here, a density functional theory study was conducted to investigate the stability, energy, and reactivity properties of NiPd (n = 1-3) clusters supported on graphene with different defects (i.e., graphene with monovacancy and pyridinic N-doped graphene with one, two, and three N atoms). On the interaction between the clusters and graphene with defects, the charge was transferred from the clusters to the modified graphene, and it was observed that the binding energy between them was substantially higher than that previously reported for Pd-based clusters supported on pristine graphene. The vertical ionization potential calculated for the clusters supported on modified graphene decreased compared with that calculated for free clusters. In contrast, vertical electron affinity values for the clusters supported on graphene with defects increased compared with those calculated for free clusters. In addition, the chemical hardness calculated for the clusters supported on modified graphene was decreased compared with free clusters, suggesting that the former may exhibit higher reactivity than the latter. Therefore, it could be inferred that graphene with defects is a good support material because it enhances the stability and reactivity of the Pd-based alloy clusters supported on PNG.
具有缺陷的石墨烯是一种重要的载体材料，因为它能提高纳米颗粒的催化活性和稳定性。在此，进行了一项密度泛函理论研究，以考察负载在具有不同缺陷的石墨烯（即具有单空位的石墨烯以及含有一个、两个和三个氮原子的吡啶型氮掺杂石墨烯）上的NiPd（n = 1 - 3）团簇的稳定性、能量和反应活性特性。关于团簇与具有缺陷的石墨烯之间的相互作用，电荷从团簇转移到改性石墨烯上，并且观察到它们之间的结合能显著高于先前报道的负载在原始石墨烯上的钯基团簇的结合能。计算得到的负载在改性石墨烯上的团簇的垂直电离势相较于自由团簇有所降低。相反，负载在具有缺陷的石墨烯上的团簇的垂直电子亲和势值相较于自由团簇有所增加。此外，计算得到的负载在改性石墨烯上的团簇的化学硬度相较于自由团簇降低，这表明前者可能比后者表现出更高的反应活性。因此，可以推断具有缺陷的石墨烯是一种良好的载体材料，因为它增强了负载在吡啶型氮掺杂石墨烯上的钯基合金团簇的稳定性和反应活性。
