DFT Insights into the Interfacial Chemical Behavior of Hybrid LDH/GO Nanocomposites

Abstract

Hybrid layered double hydroxides (LDHs)/graphene oxide (GO) nanocomposites are novel two-dimensional (2-D) materials applied in extensive fields, which take advantages of the synergistic effect of LDH and GO at the composite interface. However, the interfacial interaction mechanism determining the LDH/GO nanocomposite properties still remains to be explored. Herein, we used density functional theory to comprehensively illustrate interfacial interactions, as well as structural and electronic properties of Mg/Al LDH/GO nanocomposites. Our results, for the first time, reveal that there exists unique water-generated chemical interaction during the LDH/GO combining process. The generated interfacial water molecules play a key role in maintaining the nanocomposites by forming complicated and diverse interfacial hydrogen bond structures. Moreover, the transfer of the hydrogen atom from LDH to the epoxy group resulting in hydroxyl was also observed. The results provide hints for interpreting previous experimental observations. There is interfacial charge transfer from LDH to GO and water molecules. The electrical properties of the LDH component in the composite can be modulated by properly varying the epoxy/ hydroxyl ratio on GO. The current results might prove to be instrumental in the design of 2-D heterostructural LDH/GO composites.

A Novel Coating System Based on Layered Double Hydroxide/HQS Hierarchical Structure for Reliable Protection of Mg Alloy: Electrochemical and Computational Perspectives

“…Besides, EDD map in Figure 7 c shows the accumulation and depletion of electrons at the interface of the Mg-Al LDH hybrid material. The charge distribution at the interface of the HQS@Mg-Al LDH composite is located on the intermolecular bonds formed with hydroxyl groups of Mg-Al LDH, suggesting that the charge transfer takes place between different active regions and Mg-Al LDH layers [ 56 ]. Overall, our findings indicate that HQS serves as a suitable linker for generating well-structured self-assemblies on LDH surfaces.…”

Electric‐Field‐Assisted Enhanced Electron Transfer to Boost Supercapacitor Negative Electrode Performance for a Fabricated Fe7S8/α‐FeOOH Nano‐Heterostructure

“…[3][4][5] However, although the supercapacitor has much significant advantages, the inferior energy density has hindered its application in practice severely. [23] Even the discussion about this field has been neglected selectively in the previous reports. The "synergistic effect" between different components has been proposed as the explanation for the obtained good property.…”

“…Obviously, this is not enough. How to realize this “synergistic effect,” which is useful for understanding the electron transfer mechanism between the electrode and the electrolyte, is still unknown . Even the discussion about this field has been neglected selectively in the previous reports.…”