2026-10-12T07:30:31Z https://api.figshare.com/v2/oai

oai:figshare.com:article/33803280 2026-09-15T15:34:41Z category_146 category_915 category_272 category_873 category_45 category_734 category_69 portal_63 item_type_2 month_year_09_2026

Surface Compositional Reconstruction of Sb₂Se₃ Thin Films with Simultaneously Enhanced Charge Transport and Light Trapping Enabling Efficient Photocathodes Shuo Chen (260745) Hanhua Zhang (20576522) Muhammad Abbas (423159) Jasim Yousaf (23203556) Jun Zhao (59250) Yuexing Chen (378833) Jingting Luo (6330422) Zhenghua Su (1570972) Guangxing Liang (6492881) Space Science Physical Sciences not elsewhere classified Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified Sociology Biological Sciences not elsewhere classified Inorganic Chemistry water splitting thanks promising photocathode semiconductor photoelectric property advantages photocathodes remains limited passivation strategy regulated 72 %, setting surface compositional reconstruction like band alignment cds buffer layer induce photovoltage losses rhe </ sub 4 </ sub 3 </ sub 2 </ sub v </ j </ </ sub surface exhibits like light )/ cds trapping microstructure thin films targeted post relatively shallow optimized mo mitigating deep level defects highest reported favorable spike diffusion kinetics conversion efficiency complex deep cell solar Antimony selenide (Sb₂Se₃) is a promising photocathode semiconductor for photoelectrochemical (PEC) water splitting thanks to its cost-effectiveness and photoelectric property advantages. However, the performance of Sb₂Se₃ photocathodes remains limited by a low onset potential (<i>V</i>_on), mainly associated with complex deep-level defects that induce photovoltage losses. Herein, we introduce a targeted post-passivation strategy regulated by the diffusion kinetics of a highly reactive gaseous sulfur source. It induces surface compositional reconstruction, mitigating deep-level defects by transforming them into relatively shallow-level defects. Meanwhile, the Sb₂Se₃(S) layer formed via surface compositional reconstruction enables a favorable spike-like band alignment with the CdS buffer layer and reduces charge transfer resistance. In addition, the resulting Sb₂Se₃(S) surface exhibits a groove-like light-trapping microstructure, thereby enhancing photon utilization. As a result, the optimized Mo/Sb₂Se₃(S)/CdS/SnO₂/Pt photocathode overcomes the trade-off between photocurrent and photovoltage, achieving the highest reported <i>V</i>_on of 0.62 <i>V</i>_RHE among Sb₂Se₃-based photocathodes, together with a high photocurrent density (<i>J</i>_ph) of 26.81 mA cm^–2, and a half-cell solar to-hydrogen (HC-STH) conversion efficiency of 5.62%. When coupled with a BiVO₄ photoanode, it further delivers a record unbiased STH efficiency of 2.72%, setting a benchmark in Sb₂Se₃-based tandem cells for PEC processed solar hydrogen production. 2026-09-15T00:00:00Z Dataset Media 10.1021/acsnano.6c13107.s002 https://figshare.com/articles/media/Surface_Compositional_Reconstruction_of_Sb_sub_2_sub_Se_sub_3_sub_Thin_Films_with_Simultaneously_Enhanced_Charge_Transport_and_Light_Trapping_Enabling_Efficient_Photocathodes/33803280 CC BY-NC 4.0