Vertically aligned p-silicon nanowire （SiNW） arrays have been extensively investigated in recent years as promising photocathodes for solar-driven hydrogen evolution. However, the fabrication of SiNW photocathodes w...Vertically aligned p-silicon nanowire （SiNW） arrays have been extensively investigated in recent years as promising photocathodes for solar-driven hydrogen evolution. However, the fabrication of SiNW photocathodes with both high photoelectrocatalytic activity and long-term operational stability using a simple and affordable approach is a challenging task. Herein, we report conformal and continuous deposition of a di-cobalt phosphide （C02P） layer on lithography- patterned highly ordered SiNW arrays via a cost-effective drop-casting method followed by a low-temperature phosphorization treatment. The as-deposited C02P layer consists of crystalline nanoparticles and has an intimate contact with SiNWs, forming a well-defined SiNW@Co2P core/shell nanostructure. The conformal and continuous Co2P layer functions as a highly efficient catalyst capable of substantially improving the photoelectrocatalytic activity for the hydrogen evolution reaction （HER） and effectively passivates the SiNWs to protect them from photo-oxidation, thus prolonging the lifetime of the electrode. As a consequence, the SiNW@Co2P photocathode with an optimized C02P layer thickness exhibits a high photocurrent density of -21.9 mA·cm^-2 at 0 V versus reversible hydrogen electrode and excellent operational stability up to 20 h for solar-driven hydrogen evolution, outperforming many nanostructured silicon photocathodes reported in the literature. The combination of passivation and catalytic functions in a single continuous layer represents a promising strategy for designing high-performance semiconductor photoelectrodes for use in solar-driven water splitting, which may simplify fabrication procedures and potentially reduce production costs.展开更多
文摘Vertically aligned p-silicon nanowire （SiNW） arrays have been extensively investigated in recent years as promising photocathodes for solar-driven hydrogen evolution. However, the fabrication of SiNW photocathodes with both high photoelectrocatalytic activity and long-term operational stability using a simple and affordable approach is a challenging task. Herein, we report conformal and continuous deposition of a di-cobalt phosphide （C02P） layer on lithography- patterned highly ordered SiNW arrays via a cost-effective drop-casting method followed by a low-temperature phosphorization treatment. The as-deposited C02P layer consists of crystalline nanoparticles and has an intimate contact with SiNWs, forming a well-defined SiNW@Co2P core/shell nanostructure. The conformal and continuous Co2P layer functions as a highly efficient catalyst capable of substantially improving the photoelectrocatalytic activity for the hydrogen evolution reaction （HER） and effectively passivates the SiNWs to protect them from photo-oxidation, thus prolonging the lifetime of the electrode. As a consequence, the SiNW@Co2P photocathode with an optimized C02P layer thickness exhibits a high photocurrent density of -21.9 mA·cm^-2 at 0 V versus reversible hydrogen electrode and excellent operational stability up to 20 h for solar-driven hydrogen evolution, outperforming many nanostructured silicon photocathodes reported in the literature. The combination of passivation and catalytic functions in a single continuous layer represents a promising strategy for designing high-performance semiconductor photoelectrodes for use in solar-driven water splitting, which may simplify fabrication procedures and potentially reduce production costs.
