Abstract
The growth of atomically dispersed metal catalysts (ADMCs) remains a great challenge owing to the thermodynamically driven atom aggregation. Here we report a surface-limited electrodeposition technique that uses site-specific substrates for the rapid and room-temperature synthesis of ADMCs. We obtained ADMCs by the underpotential deposition of a non-noble single-atom metal onto the chalcogen atoms of transition metal dichalcogenides and subsequent galvanic displacement with a more-noble single-atom metal. The site-specific electrodeposition enables the formation of energetically favorable metal–support bonds, and then automatically terminates the sequential formation of metallic bonding. The self-terminating effect restricts the metal deposition to the atomic scale. The modulated ADMCs exhibit remarkable activity and stability in the hydrogen evolution reaction compared to state-of-the-art single-atom electrocatalysts. We demonstrate that this methodology could be extended to the synthesis of a variety of ADMCs (Pt, Pd, Rh, Cu, Pb, Bi, and Sn), showing its general scope for functional ADMCs manufacturing in heterogeneous catalysis.
Highlights
The growth of atomically dispersed metal catalysts (ADMCs) remains a great challenge owing to the thermodynamically driven atom aggregation
We approached the fabrication of ADMCs by first exploring the underpotential deposition (UPD) of Cu atoms on chemically exfoliated molybdenum disulfide, which was used as a prototypical Transition metal dichalcogenides (TMDs) substrate to demonstrate the feasibility of a site-specific UPD strategy for fabricating ADMCs
No obvious nanoparticles or clusters were discernable in Cu-SAs/MoS2, whereas elemental Cu was detected by X-ray photoelectron spectroscopy (XPS; Supplementary Fig. 4g–i), indicating the successful growth of a single atom on MoS2 by using UPD (Supplementary Note 2)[19]
Summary
The growth of atomically dispersed metal catalysts (ADMCs) remains a great challenge owing to the thermodynamically driven atom aggregation. Owing to its facile operation, mildness, large scalability, low cost, and precision[8], ED has been extensively used for the fabrication of nanomaterials and industrial applications (e.g., electroplating)[9,10] This process leads to the inevitable formation of multilayer bulk structures with nonuniform coverage (Fig. 1(i) and Supplementary Fig. 1a). We reasoned that the single-atom layer could potentially be upgraded to single atoms deposited site- on a supporting substrate for UPD (Fig. 1(iii) and Supplementary Fig. 1c) if the substrate consists of isolated active sites owing to the nonuniform work function (Supplementary Note 1). Owing to the strong coordination and electronic interaction between the depositing metal and the chalcogen sites on the substrate, the metal–support interaction is energetically favorable compared to the metal–metal interaction in the crystal lattice of the bare metal during the UPD process. This site-specific ED (SSED) method represents a major breakthrough with respect to other extremely time-consuming and procedurally demanding strategies
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