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Towards Lead-free Perovskite Solar Cells
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摘要
Despite CH_3NH_3PbI_3 perovskite solar cells have recently exhibited a significan improvement in efficiency, the Sn-based perovskite solar cells still suffer from low efficiency and poor stability that derived from the oxidation of Sn~(2+) [1-4].Here, a series CH_3NH_3Pb_((1-x))Sn_xI_3(0≤x≤1) perovskite thin films with full coverage were obtained via molecular self-assembly process.We demonstrated that the electronic properties of CH_3NH_3Pb_((1-x))Sn_xI_3(0≤x≤1) perovskite films, i.e., defect state density, carrier concentration, mobility and energy level, could be controllable by tuning the composition ratio of Pb/Sn.The external quantum efficiency(EQE) of as-prepared solar cells were demonstrated to extend a broad absorption minimum over 50% in the wavelength range from 350 to 950 nm accompanied by a noteworthy absorption onset up to 1050 nm.The CH_3NH_3Pb_(0.75)Sn_(0.25)I_3 perovskite solar cells with inverted structure were consequently realized with maximum power conversion efficiency(PCE) over 14%, which displayed hysteresis-free effect and stabilized power output(SPO) over 12% within 200 s at 0.6 V forward bias.Likewise, we further investigated the surface and bulk recombination lifetime of carriers, as well as the transient photovoltage decay curves of devices, which were favorable to clearly understand the carrier dynamics and optimize the Sn-Pb mixed perovskite solar cells.Importantly, the modified hybrid Sn-Pb perovskite solar cells were demonstrated to own superior stability and efficiency when exposed to the ambien environment without encapsulation.The present study is favorable to overcome the intractable issue concerning the toxic Pb element in perovskite solar cells and step forward toward realizing the lead-free perovskite solar cells with high efficiency.
Despite CH_3NH_3PbI_3 perovskite solar cells have recently exhibited a significan improvement in efficiency, the Sn-based perovskite solar cells still suffer from low efficiency and poor stability that derived from the oxidation of Sn~(2+) [1-4].Here, a series CH_3NH_3Pb_((1-x))Sn_xI_3(0≤x≤1) perovskite thin films with full coverage were obtained via molecular self-assembly process.We demonstrated that the electronic properties of CH_3NH_3Pb_((1-x))Sn_xI_3(0≤x≤1) perovskite films, i.e., defect state density, carrier concentration, mobility and energy level, could be controllable by tuning the composition ratio of Pb/Sn.The external quantum efficiency(EQE) of as-prepared solar cells were demonstrated to extend a broad absorption minimum over 50% in the wavelength range from 350 to 950 nm accompanied by a noteworthy absorption onset up to 1050 nm.The CH_3NH_3Pb_(0.75)Sn_(0.25)I_3 perovskite solar cells with inverted structure were consequently realized with maximum power conversion efficiency(PCE) over 14%, which displayed hysteresis-free effect and stabilized power output(SPO) over 12% within 200 s at 0.6 V forward bias.Likewise, we further investigated the surface and bulk recombination lifetime of carriers, as well as the transient photovoltage decay curves of devices, which were favorable to clearly understand the carrier dynamics and optimize the Sn-Pb mixed perovskite solar cells.Importantly, the modified hybrid Sn-Pb perovskite solar cells were demonstrated to own superior stability and efficiency when exposed to the ambien environment without encapsulation.The present study is favorable to overcome the intractable issue concerning the toxic Pb element in perovskite solar cells and step forward toward realizing the lead-free perovskite solar cells with high efficiency.
引文
[1]Kojima A,Teshima K,Shirai Y,Miyasaka T,J.Am.Chem.Soc.2009,131,6050;
    [2]Yang W S,Noh J H,Jeon N J,Kim Y C,Ryu S,Seo J,Seok S I,Science 2015,348,1234;
    [3]Li W,Fan J,Li J,Mai Y,Wang L,J.Am.Chem.Soc.2015,137,10399.
    [4]Hao F,Stoumpos C C,Kanatzidis M G,J.Am.Chem.Soc.2015,137,11445.

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