Engineering Interfacial Charge Transfer in Dye-Sensitized Solar Cells via Nitrogen Plasma-Engineered Chitosan@PVA@CuSO4 Counter Electrodes
摘要
Utilizing polymer-based materials to develop high-performance electrochemical components represents a promising pathway toward sustainable energy technologies. In this context, nitrogen plasma–engineered Chitosan@PVA@CuSO4 (CPCS) counter electrodes (CEs) exhibit a pronounced evolution in physicochemical and photovoltaic characteristics as a function of controlled plasma exposure (0–12 min). Interestingly, plasma activation induces substantial microstructural reconfiguration, evidenced by a marked increase in surface roughness (from 5.31 to 7.55 μm) alongside a significant rise in porosity (41.7% to 60.1%), thereby establishing a highly accessible and permeable electrode architecture. Concurrently, surface energetics undergo a notable transition toward enhanced hydrophilicity, reinforcing electrolyte wettability and interfacial adhesion. These modifications are further accompanied by improved electrical conductivity and band-gap narrowing, collectively facilitating more efficient charge transport and electrocatalytic activity. As a direct consequence, the interfacial charge-transfer resistance (Rct) is significantly reduced from 46.55 Ω (CPCS0) to 12.91 Ω (CPCS9), reflecting accelerated redox kinetics at the CE/electrolyte interface. This electrochemical enhancement translates into a substantial improvement in photovoltaic performance, with power conversion efficiency (η) increasing from 4.78% to 8.01%. In parallel, the incident photon-to-current conversion efficiency (IPCE) reaches ~ 86.4%, approaching that of Pt-based counterparts. A well-defined optimization window emerges at CPCS9, where the interplay between structural ordering, surface functionalization, and interfacial charge-transfer dynamics attains a synergistic maximum. Beyond this threshold, extended plasma exposure induces partial structural deterioration, highlighting the critical importance of controlled surface engineering. Collectively, these findings establish nitrogen plasma modification as a powerful strategy for tailoring hybrid polymer–inorganic electrodes, enabling substantial enhancement in electrocatalytic efficiency without reliance on noble metals, while positioning CPCS systems as a compelling platform for high-performance DSSC applications.