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The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/admi.202200179. solar cells. [2] Recently, perovskite solar cells (PSCs) have gained enormous attention owing to their tunable energy bandgap, long charge carrier diffusion length, and high absorption coefficient. [3] The photoelectric conversion efficiency (PCE) of PSCs has increased rapidly from 3.8% to 25.5% certified by the National Renewable Energy Laboratory of the United States. [4] Its rapid progress has never been seen before in the history of photovoltaic development. However, many obstacles should be overcome for its large-scale commercialization, such as the currentvoltage hysteresis effect, long-term instability (lifetime), and degradation under oxygen-rich or humidity. [5] In the preparation process of the perovskite layer, many point defects will appear such as vacancies, interstitial, or anti-site atoms (MAPbI 3 , e.

Recently, perovskites have garnered great attention owing to their outstanding characteristics, such as tunable bandgap, rapid absorption reaction, low cost and solution-based processing, leading to the development of high-quality and low-cost photovoltaic devices. However, the key challenges, such as stability, large-area processing, and toxicity, hinder the commercialization of perovskite solar cells (PSCs). In recent years, several studies have been carried out to overcome these issues and realize the commercialization of PSCs. Herein, the stability and photovoltaic efficiency improvement strategies of perovskite solar cells are briefly summarized from several directions, such as precursor doping, selection of hole/electron transport layer, tandem solar cell structure, and graphene-based PSCs. According to reference and analysis, we present our perspective on the future research directions and challenges of PSCs.

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The high-density defect states existing at the grain boundaries and heterojunction interfaces induce nonradiative charge recombination and ion migration processes within perovskite film, which seriously impair the device efficiency and stability. Here, we propose a novel synergistic ion-anchoring passivation (SIP) strategy for high-performance perovskite solar cells, by designing a multifunctional molecule to heal the charged defects via electrostatic interactions. The anion and cation species of the multifunctional molecule are rationally screened via highthroughput DFT simulation and experimental verification, which act as efficient surface passivation agents to heal the lead-and iodine-related defects. As a result, the defect-less perovskite films deliver encouraging device power conversion efficiency >24% with negligible hysteresis. A remarkable open-circuit voltage (Voc) of 1.17 V was obtained with a Voc deficit of 370 mV, featuring the outstanding defect-passivation capability of the SIP strategy. Moreover, the SIP-treated devices show exceptional ambient stability and maintain 70% of the initial efficiency after 150 h of high humidity exposure (relative humidity 70%−80%). Our results highlight the importance of the rational design of passivation agents to realize high-performance perovskite electronics.

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