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首页> 外文期刊>Energy & environmental science >Entropic stabilization of mixed A-cation ABX(3) metal halide perovskites for high performance perovskite solar cells
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Entropic stabilization of mixed A-cation ABX(3) metal halide perovskites for high performance perovskite solar cells

机译:高性能钙钛矿太阳能电池用混合A-阳离子ABX(3)金属卤化物钙钛矿的熵稳定

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摘要

ABX(3)-type organic lead halide perovskites currently attract broad attention as light harvesters for solar cells due to their high power conversion efficiency (PCE). Mixtures of formamidinium (FA) with methylammonium (MA) as A-cations show currently the best performance. Apart from offering better solar light harvesting in the near IR the addition of methylammonium stabilizes the perovskite phase of FAPbI(3) which in pure form at room temperature converts to the yellow photovoltaically inactive delta-phase. We observe a similar phenomenon upon adding Cs+ cations to FAPbI(3). CsPbI3 and FAPbI3 both form the undesirable yellow phase under ambient condition while the mixture forms the desired black pervoskite. Solar cells employing the composition Cs(0.2)FA(0.8)PbI(2.84)Br(0.16) yield high average PCEs of over 17% exhibiting negligible hysteresis and excellent long term stability in ambient air. We elucidate here this remarkable behavior using first principle computations. These show that the remarkable stabilization of the perovskite phase by mixing the A-cations stems from entropic gains and the small internal energy input required for the formation of their solid solution. By contrast, the energy of formation of the delta-phase containing mixed cations is too large to be compensated by this configurational entropy increase. Our calculations reveal for the first time the optoelectronic properties of such mixed A-cation perovskites and the underlying reasons for their excellent performance and high stability.
机译:由于它们的高功率转换效率(PCE),ABX(3)型有机卤化铅钙钛矿目前作为太阳能电池的光收集器受到广泛关注。目前,甲酰胺(FA)与甲基铵(MA)作为A阳离子的混合物表现出最好的性能。除了在近红外条件下提供更好的太阳光采光外,甲基铵的加入还可以稳定FAPbI(3)的钙钛矿相,该钙钛矿相在室温下呈纯净形式转变为黄色的光伏钝化δ相。我们在向FAPbI(3)添加Cs +阳离子时观察到类似现象。 CsPbI3和FAPbI3在环境条件下均会形成不良的黄色相,而混合物则形成所需的黑色钙钛矿。使用组成为Cs(0.2)FA(0.8)PbI(2.84)Br(0.16)的太阳能电池可产生超过17%的高平均PCE,表现出可忽略的滞后性,并在环境空气中具有出色的长期稳定性。我们在这里使用第一原理计算来阐明这种非凡的行为。这些表明,通过混合A-阳离子使钙钛矿相具有显着的稳定性,是由于熵增加和形成固溶体所需的内部能量输入少。相反,包含混合阳离子的δ相的形成能量太大而不能被这种结构熵的增加所补偿。我们的计算首次揭示了这种混合的A-阳离子钙钛矿的光电性能及其出色性能和高稳定性的根本原因。

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  • 来源
    《Energy & environmental science》 |2016年第2期|656-662|共7页
  • 作者单位

    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Sch Basic Sci, Lab Photon & Interfaces, CH-1015 Lausanne, Switzerland;

    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Sch Basic Sci, Lab Photon & Interfaces, CH-1015 Lausanne, Switzerland;

    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Computat Chem & Biochem, CH-1015 Lausanne, Switzerland;

    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Computat Chem & Biochem, CH-1015 Lausanne, Switzerland;

    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Computat Chem & Biochem, CH-1015 Lausanne, Switzerland;

    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Sch Basic Sci, Lab Photon & Interfaces, CH-1015 Lausanne, Switzerland;

    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Sch Basic Sci, Lab Photon & Interfaces, CH-1015 Lausanne, Switzerland;

    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Lab Computat Chem & Biochem, CH-1015 Lausanne, Switzerland;

    Ecole Polytech Fed Lausanne, Inst Chem Sci & Engn, Sch Basic Sci, Lab Photon & Interfaces, CH-1015 Lausanne, Switzerland;

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