Crystallization modulation and defect passivation in carbon-based perovskite solar cells using multifunctional group additive

Recently, carbon-based perovskite solar cells have attracted wide attention in academia and industry because of their simple preparation process, low cost, and adaptability to roll-to-roll industrial production. The combination of ternary perovskite composition and carbon electrode configuration is expected to meet the requirements of device performance and stability. However, low grain size, and high density of grain boundary and surface defect states result in serious non-radiative recombination, which is one of the main gaps between the carbon-based perovskite solar cells and metal-electrode-based devices. Based on the consideration of crystal tuning and defect passivation of ternary CsFAMA thin films, the additive molecule 5-(Difluoromethoxy)-2-mercapto-1H-benzimidazole (DMB) with multifunctional groups were introduced into the film. XRD show that the (100) and (200) crystal plane orientation growth directed by the DMB additive lead to the formation of the micro-sized perovskite. XPS suggests that DMB not only modulates the crystallization of the films but also exists at the grain boundaries, and realizes the passivation of undercoordinated Pb2+ defects and inhibits the generation of Pb0. The defect state density is significantly reduced, and the carrier lifetime is greatly improved. The possible mechanism for perovskite crystal growth as well as defect passivation based on Lewis acid-base coordination and hydrogen bond was also proposed. After the introduction of DMB, a power conversion efficiency of 14.40% was achieved, which was 13.4% higher than that of the control device. After nearly 1200 h of environmental stability test, the DMB modified device still retained 95% of the original efficiency. This work emphasizes the feasibility of simultaneously realizing the crystallization modulation and defect passivation of carbon-based perovskite solar cells using the additive with multifunctional groups, and provides a reference for the commercialization of carbon-based perovskite solar cells.