Composition, Morphology, and Interface Engineering of 3D Cauliflower-Like Porous Carbon-Wrapped Metal Chalcogenides...

Designing a low-cost, highly efficient, and stable electrocatalyst that can synergistically speed up the reduction of polysulfide electrolytes while operative for long periods in the open air is critical for the practical application of quantum dot-sensitized solar cells (QDSSCs), but it remains a challenging task. Herein, a simple, straightforward, and two-step nanocomposite engineering approach that simultaneously combines metallic copper chalcogenides (MC) either Cu_{2- x} S or Cu_{2- x} Se with S, N dual-doped carbon (SNC) sources for devising high-quality counter electrode (CE) film are reported. First, the hierarchically assembled MC nanostructures are obtained using microwave-assisted synthesis. Second, these MCs are embedded within an ordered macro-meso-microporous carbon matrix to obtain Cu_{2- x} S@C or Cu_{2- x} SeS@C CE. These CEs are demonstrated to have composition dependents crystal structure, surface morphologies, photovoltaic performance, and electrochemical properties. In terms of power conversion efficiency (PCE), the Cu_{2- x} SeS@C (9.89%) and Cu_{2- x} S@C-CE (8.96%) constructed QDSSCs outperform both Cu_{2- x} Se (8.96%) and Cu_{2- x} S-constructed (7.79%) QDSSCs, respectively. The enhanced PCE could be attributed to the synergistic interaction of S and N dopants with MC interfaces that can not only enrich electric conductivity, and a higher surface-to-volume ratio but also offers a 3D network for superior charge transport at the interface.