Wu Bo, Wang Tuo, Liu Bin, Li Huimin, Wang Yunlong, Wang Shujie, Zhang Lili, Jiang Shaokun, Pei Chunlei, Gong Jinlong
School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, China.
Key Laboratory for Green Chemical Technology of Ministry of Education, Tianjin University, Tianjin, 300072, China.
Nat Commun. 2022 Aug 1;13(1):4460. doi: 10.1038/s41467-022-32099-1.
Protective layers are essential for Si-based photocathodes to achieve long-term stability. The conventionally used inorganic protective layers, such as TiO, need to be free of pinholes to isolate Si from corrosive solution, which demands extremely high-quality deposition techniques. On the other hand, organic hydrophobic protective layers suffer from the trade-off between current density and stability. This paper describes the design and fabrication of a discontinuous hybrid organic protective layer with controllable surface wettability. The underlying hydrophobic layer induces the formation of thin gas layers at the discontinuous pores to isolate the electrolyte from Si substrate, while allowing Pt co-catalyst to contact the electrolyte for water splitting. Meanwhile, the surface of this organic layer is modified with hydrophilic hydroxyl groups to facilitate bubble detachment. The optimized photocathode achieves a stable photocurrent of 35 mA/cm for over 110 h with no trend of decay.
对于硅基光阴极而言,保护层对于实现长期稳定性至关重要。传统使用的无机保护层,如二氧化钛,需要无针孔才能将硅与腐蚀性溶液隔离开来,这需要极高质量的沉积技术。另一方面,有机疏水保护层在电流密度和稳定性之间存在权衡。本文描述了一种具有可控表面润湿性的不连续混合有机保护层的设计与制备。底层疏水层在不连续孔隙处诱导形成薄气层,以将电解质与硅基底隔离开,同时允许铂助催化剂与电解质接触以进行水分解。与此同时,该有机层的表面用亲水性羟基进行修饰,以促进气泡脱离。优化后的光阴极在超过110小时内实现了35 mA/cm²的稳定光电流,且无衰减趋势。