We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO₂ reduction reaction (CO₂RR) via Mo–S bridging bonds sites in S_v–In₂S₃@2H–MoTe₂. The X-ray absorption near-edge structure shows that the formation of S_v–In₂S₃@2H–MoTe₂ adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface. The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption, time-resolved, and in situ diffuse reflectance–Infrared Fourier transform spectroscopy. A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_v–In₂S₃@2H–MoTe₂(5) photogenerated carrier concentration relative to pristine S_v–In₂S₃. Benefiting from lower carrier transport activation energy, an internal quantum efficiency of 94.01% at 380 nm was used for photocatalytic CO₂RR. This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO₂RR.

Layered transition-metal dichalcogenides based on VIB elements have attracted substantial attention for their applications in energy storage and conversion. However, few studies have concentrated on VB element dichalcogenides. Herein, we report that trifunctional 2H-TaS₂ nanoflakes exhibit high performance when applied in supercapacitors, hydrogen evolution reactions (HER) and oxygen evolution reactions (OER). Notably, TaS₂ nanoflakes delivered a large volumetric capacitance (502 F cm⁻³ at the scan rate of 10 mV s⁻¹) and remarkable cycling stability (over 91% after 5000 cycles). TaS₂ nanoflakes also exhibited remarkable catalytic performances in HER and OER processes, showing very small overpotentials and Tafel slopes, which are far better than those of the previously reported TaS₂ electrocatalysts. Furthermore, TaS₂ is highly stable in both alkaline and acidic electrolyte solutions. This work offers a new concept to design VB element-based electrodes for future energy storage and conversion applications.