Electric bias-induced reversible configuration of single and heteronuclear dual-atom catalysts on 1T'-MoS.

The development of substrates capable of anchoring single-atom catalysts (SACs) while enabling their dynamic reconfiguration into heteronuclear dual-atom catalysts (DACs) holds considerable promise for electrochemical synthesis, yet remains underexplored. Here we show that electrochemical desulfurization of MoS generates vacancy-rich 1T' domains, which support high loadings of Cu (7.9 wt%) and Pt (6.7 wt%) SACs that are well-positioned for dynamic sintering to form DACs. Operando X-ray absorption spectroscopy and density functional theory calculations reveal a voltage-driven, reversible transformation between individual Pt/Cu SACs and Cu-Pt DAC configurations during hydrogen evolution reaction potentials. The electric-field-induced Cu-Pt DACs exhibit superior performance in the selective hydrogenation of alkynes compared with their monometallic SAC counterparts. This work underscores vacancy-enriched 1T'-MoS as a versatile platform for high-density SAC deposition, enabling on-demand structural reconfiguration and paving the way for tailored catalyst design in electrosynthesis.