Antimony sulfide is an emerging 1D nontoxic Earth-abundant photovoltaic material with favorable wide bandgap as a suitable top-cell candidate for multijunction tandem solar cells. However, the current fabrication technology for Sb 2 S 3 solar cells relies heavily on a high-purity Sb 2 S 3 source, which limits its large-scale deployment. Therefore, it is attractive to fabricate the Sb 2 S 3 solar cells directly from the raw stibnite source, which can be cost effective by avoiding the complicated, costly purification and refinement process of the stibnite ore, while reducing process-emitted pollution. Herein, high-quality Sb 2 S 3 films (thickness: ≈1 μm) by the vapor transport deposition of raw stibnite ore powder are obtained, followed by a sulfurization process to remove the surface oxides and facilitate alkali element redistribution. In this way, the particle size is increased from ≈500 nm to ≈1.5 μm, the carrier concentration of the Sb 2 S 3 film is increased from ≈10 15 to ≈10 16 cm −3 , and the power conversion efficiency of Sb 2 S 3 solar cell is increased by more than two times. Through the elemental distribution analysis, it is found that it is the redistribution of alkali elements introduced from the natural stibnite ore that induces the grain growth, contributes toward defect suppression, and leads toward enhanced device performance.
Chen Xiao,Shu Xiaoxuan,Zhou Jiacheng,Wan Lei,Xiao Peng,Fu Yuchen,Ye Junzhi,Huang Yi-Teng,Yan Bin,Xue Dingjiang,Chen Tao,Chen Jiejie,Hoye Robert L. Z.,Zhou Ru
Indoor photovoltaics (IPVs) have attracted increasing attention for sustainably powering Internet of Things (IoT) electronics. Sb 2 S 3 is a promising IPV candidate material with a bandgap of ~1.75 eV, which is near the optimal value for indoor energy harvesting. However, the performance of Sb 2 S 3 solar cells is limited by nonradiative recombination, which is dependent on the quality of the absorber films. Additive engineering is an effective strategy to fine tune the properties of solution-processed films. This work shows that the addition of monoethanolamine (MEA) into the precursor solution allows the nucleation and growth of Sb 2 S 3 films to be controlled, enabling the deposition of high-quality Sb 2 S 3 absorbers with reduced grain boundary density, optimized band positions, and increased carrier concentration. Complemented with computations, it is revealed that the incorporation of MEA leads to a more efficient and energetically favorable deposition for enhanced heterogeneous nucleation on the substrate, which increases the grain size and accelerates the deposition rate of Sb 2 S 3 films. Due to suppressed carrier recombination and improved charge-carrier transport in Sb 2 S 3 absorber films, the MEA-modulated Sb 2 S 3 solar cell yields a power conversion efficiency (PCE) of 7.22% under AM1.5 G illumination, and an IPV PCE of 17.55% under 1000 lux white light emitting diode (WLED) illumination, which is the highest yet reported for Sb 2 S 3 IPVs. Furthermore, we construct high performance large-area Sb 2 S 3 IPV minimodules to power IoT wireless sensors, and realize the long-term continuous recording of environmental parameters under WLED illumination in an office. This work highlights the great prospect of Sb 2 S 3 photovoltaics for indoor energy harvesting.