Perfection of Perovskite Grain Boundary Passivation by Rhodium Incorporation for Efficient and Stable Solar Cells

Organic cation and halide anion defects are omnipresent in the perovskite films, which will destroy perovskite electronic structure and downgrade the properties of devices. Defect passivation in halide perovskites is crucial to the application of solar cells. Herein, tiny amounts of trivalent rhodium ion incorporation can help the nucleation of perovskite grain and passivate the defects in the grain boundaries, which can improve efficiency and stability of perovskite solar cells. Through first-principle calculations, rhodium ion incorporation into the perovskite structure can induce ordered arrangement and tune bandgap. In experiment, rhodium ion incorporation with perovskite can contribute to preparing larger crystalline and uniform film, reducing trap-state density and enlarging charge carrier lifetime. After optimizing the content of 1% rhodium, the devices achieved an efficiency up to 20.71% without obvious hysteresis, from 19.09% of that pristine perovskite. In addition, the unencapsulated solar cells maintain 92% of its initial efficiency after 500 h in dry air. This work highlights the advantages of trivalent rhodium ion incorporation in the characteristics of perovskite solar cells, which will promote the future industrial application. [Image: see text] ELECTRONIC SUPPLEMENTARY MATERIAL: The online version of this article (10.1007/s40820-020-00457-7) contains supplementary material, which is available to authorized users.