Spontaneous chemical functionalization via coordination of Au single atoms on monolayer MoS ₂

Abstract

Surface functionalization of metallic and semiconducting 2D transition metal dichalcogenides (TMDs) have mostly relied on physi- and chemi-sorption at defect sites, which can diminish the potential applications of the decorated 2D materials, as structural defects can have substantial drawbacks on the electronic and optoelectronic characteristics. Here, we demonstrate a spontaneous defect-free functionalization method consisting of attaching Au single atoms to monolayers of semiconducting MoS2(1H) via S-Au-Cl coordination complexes. This strategy offers an effective and controllable approach for tuning the Fermi level and excitation spectra of MoS2 via p-type doping and enhancing the thermal boundary conductance of monolayer MoS2, thus promoting heat dissipation. The coordination-based method offers an effective and damage-free route of functionalizing TMDs and can be applied to other metals and used in single-atom catalysis, quantum information devices, optoelectronics, and enhanced sensing.

Direct Atomic Layer Deposition of Ultrathin Aluminum Oxide on Monolayer MoS2 Exfoliated on Gold: The Role of the Substrate

“…[36,37] In the case of 1L MoS 2 on Au, a strong electron transfer to the substrate is guessed, which overcompensates the native n-type doping, resulting in a net p-type behavior. [34,38] This is consistent with several literature reports showing a transition from n-to p-type doping for MoS 2 layers functionalized with an AuCl 3 solution, [39] single Au atoms, [40] Au thin films, [41] as well as for MoS 2 deposited by gold nanoparticles-assisted CVD. [42] The tensile strain for 1L MoS 2 on Au can be ascribed to the lattice mismatch between MoS 2 and the Au surface, mostly exposing (111) orientation.…”

CO2 reduction on single-atom Ir catalysts with chemical functionalization

“…However, AuCl 3 can be stably anchored. 26 The calculated barriers E a = 0.13 eV for bare Au and E a = 0.63 eV for AuCl 3 (Fig. S1, ESI †) obviously demonstrate that AuCl 3 on MoS 2 is considerably more stable than bare Au.…”

“…Recently, a spontaneous defect-free functionalization method attaching Au on the MoS 2 monolayer via a S-Au-Cl coordination complex has been demonstrated. 26 On the MoS 2 surface, the Au coordination complex is synthesized without the presence of additional defects by taking advantage of the lone pair electrons of S atoms. Since the coordination number of reactive centers has been considered an important factor in the structureactivity relationship of SACs, 27 this coordination-based method offers a damage-free route for functionalizing 2D materials.…”

Relation Between Coordination and Lewis‐Acid Property of MOF‐Derived Mononuclear Zn(II) Catalyst Toward Epoxide Hydroxylation

“…Meanwhile, a corresponding slight shift to lower binding energy of P2p have been observed taking an order of ZIF-8-P-900 (131.90 eV) < ZIF-8-P-800 (131.94 eV) < ZIF-8-P-700 (132.03 eV) (Figure 2d). Results infer that a bond exists between the surface Zn and P in the P coordinated samples, [34] demonstrating the successful integration of the coordinated P into the ZnÀ N/PÀ C samples.…”