Surface reconstruction, reorganizing the surface atoms or structure, is a promising strategy to manipulate materials' electrical, electrochemical, and surface catalytic properties. Herein, a rapid surface reconstruction of indium sulfide (In2S3) is demonstrated via a high-temperature flame treatment to improve its charge collection properties. The flame process selectively transforms the In2S3 surface into a diffusionless In2O3 layer with high crystallinity. Additionally, it controllably generates bulk sulfur vacancies within a few seconds, leading to surface-reconstructed In2S3 (sr-In2S3). When using those sr-In2S3 as photoanode for photoelectrochemical water splitting devices, these dual functions of surface In2O3/bulk In2S3 reduce the charge recombination in the surface and bulk region, thus improving photocurrent density and stability. With optimized surface reconstruction, the sr-In2S3 photoanode demonstrates a significant photocurrent density of 8.5 mA cm−2 at 1.23 V versus a reversible hydrogen electrode (RHE), marking a 2.5-fold increase compared to pristine In2S3 (3.5 mA cm−2). More importantly, the sr-In2S3 photoanode exhibits an impressive photocurrent density of 7.3 mA cm−2 at 0.6 V versus RHE for iodide oxidation reaction. A practical and scalable surface reconstruction is also showcased via flame treatment. This work provides new insights for surface reconstruction engineering in sulfide-based semiconductors, making a breakthrough in developing efficient solar-fuel energy devices.
Y.J.J., R.T., and S.N. contributed equally to this work. This research was supported by the Basic Science Research Program through the National Research Foundation of Korea, funded by the Ministry of Science, ICT, and Future Planning (Grant No. NRF\\u20102021R1A4A1031357). This work was also supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (Grant No. RS\\u20102023\\u201000246524 and RS\\u20102024\\u201000345042).