Local Structural Coherence and Interfacial Charge Transfer in; ; ; Cu; 2; ; ; ; S; ; ; /; ; ; Mo; S; ; 2; ; ; Heterostructure
Journal Article
Overview
abstract
; Precise control over electronic coupling at nanoscale interfaces is critical for designing materials with tunable charge-transfer behavior and catalytic function. Heterostructures with locally coherent interfaces provide a platform for interrogating interfacial charge redistribution in coupled material systems. Here, we report; ; ; Cu; 2; ; ; ; S; ; ; /; ; ; Mo; S; ; 2; ; ; heterostructures exhibiting nanoscale crystallographic alignment, which are synthesized through a rapid thermal transformation pathway. We employed electrochemical reduction reactions to probe interfacial charge transfer, revealing shifts in product distribution attributable to modified interfacial energetics, even in the absence of optimized catalytic performance. The observed formate Faradaic efficiency suggests that interfacial electronic modulation in the heterostructure shifts product selectivity towards formate, highlighting how interface-driven electronic modulation can direct reaction pathways and influence product selectivity. Optimizing catalyst loading, architecture, and reactor configuration will be critical for future improvement. Structural and compositional integrity were confirmed through powder x-ray diffraction, x-ray photoelectron spectroscopy, and high-resolution transmission electron microscopy. Electron transfer between; ; ; Cu; 2; ; ; ; S; ; ; ; and; ; ; ; Mo; S; ; 2; ; ; domains was further evaluated by electrochemical impedance spectroscopy, while selected-area electron diffraction revealed local crystallographic alignment consistent with a local epitaxial relationship at the; ; ; Cu; 2; ; ; ; S; ; ; /; ; ; Mo; S; ; 2; ; ; heterointerface. To illustrate the broader applicability of this approach, a; ; ; Zn; S; ; /; ; ; Mo; S; ; 2; ; ; heterostructure was also synthesized using the same microwave strategy, confirming the generalizability of interfacial engineering principles across metal sulfide-; ; ; ; Mo; S; ; 2; ; ; systems. Collectively, these findings demonstrate that controlled local epitaxial alignment serves as an effective design principle for tuning interfacial energetics and catalytic reactivity in complex heterostructure materials.;
