通过嵌入 Ag 和 Pd 金属纳米团簇开发用于高效 CO 捕获的 55-77 石墨烯片的理论见解。

Theoretical insights on the development of a 55-77 graphene sheet by embedding Ag and Pd metal nanoclusters for efficient CO capture.

机构信息

Molecular Simulation Laboratory, Department of Physics, Bharathiar University, Coimbatore, 641046, Tamil Nadu, India.

Chemical Engineering, Indian Institute of Technology Bombay, Maharashtra, India.

出版信息

J Mol Graph Model. 2023 Nov;124:108573. doi: 10.1016/j.jmgm.2023.108573. Epub 2023 Jul 25.

DOI:10.1016/j.jmgm.2023.108573

PMID:37523943

Abstract

Recent advancements in two-dimensional (2D) allotropes of carbon materials and their usage as superior CO adsorbents can decrease the detrimental impact of CO on climate change. With the use of quantum chemical calculations, the effect of metal clusters (Ag and Pd) on the structural and electrical characteristics of 55-77 2D graphene sheet is examined in the current work with an aim towards enhancing CO capture capacity. The findings revealed that the binding energy (E) of the 55-77 sheet decoration with Pd metal clusters are greater owing to chemisorption by 1.17 eV, 1.69 eV, 0.27 eV, and 1.58 eV than the decoration with Ag clusters. Moreover, CO molecules adsorb on the Pd cluster decorated systems having -0.35 eV, 0.83 eV, 1.53 eV, and -0.98 eV greater adsorption energies than on the Ag decorated 55-77 sheet due to a stronger charge transfer. Further, the findings of an atoms in molecules (AIM) study show that the interaction between CO and Pd decorated 55-77 sheet is partially covalent and non-covalent, confirming the greater charge transfer between the CO molecule and Pd decorated 55-77 systems. Moreover, the CO adsorption on Pd decorated 55-77 systems is clearly demonstrated by non-covalent interaction (NCI) analysis to be a strong electrostatic interaction at sign(λ)ρ = -0.05 a.u, and this is further supported by an electron localization function (ELF) map. The highest CO adsorption capacity is obtained for 55-77/Pd+CO with the value of 6.27 wt % which concludes 55-77 sheet with Pd decoration is a more suitable structure for CO adsorption than the Ag decorated system.

摘要

最近二维（2D）碳材料同素异形体的进展及其作为优异 CO 吸附剂的应用，可以降低 CO 对气候变化的不利影响。本研究采用量子化学计算，考察了金属团簇（Ag 和 Pd）对 55-77 二维石墨烯片结构和电性的影响，旨在提高 CO 捕获能力。结果表明，Pd 金属团簇修饰的 55-77 片的结合能（E）由于化学吸附而比 Ag 团簇大 1.17 eV、1.69 eV、0.27 eV 和 1.58 eV。此外，由于更强的电荷转移，CO 分子吸附在 Pd 团簇修饰的体系上的吸附能比吸附在 Ag 修饰的 55-77 片上的吸附能大 -0.35 eV、0.83 eV、1.53 eV 和 -0.98 eV。此外，分子中原子（AIM）研究的结果表明，CO 和 Pd 修饰的 55-77 片之间的相互作用部分是共价和非共价的，这证实了 CO 分子和 Pd 修饰的 55-77 体系之间更强的电荷转移。此外，通过非共价相互作用（NCI）分析清楚地表明，CO 在 Pd 修饰的 55-77 体系上的吸附是一种强静电相互作用，在 sign(λ)ρ=-0.05 a.u 处，这进一步得到电子局域函数（ELF）图的支持。对于 55-77/Pd+CO，获得了最高的 CO 吸附容量 6.27 wt%，这表明 Pd 修饰的 55-77 片是一种比 Ag 修饰体系更适合 CO 吸附的结构。