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最新Science: 阳离子反应性抑制钙钛矿降解

2024/11/4 11:46:36 admin 阅读 31【次】

钙钛矿太阳能模块(PSMs)虽然具有出色的光电转换效率(PCEs)，但长期运行的稳定性仍存在问题。由于湿气、热和光照等外部因素引起的退化问题仍然存在。特别是，三维钙钛矿的热和光诱导相降解限制了PSM的稳定性。

基于上述情况，华北电力大学丁勇、洛桑联邦理工学院Mohammad Khaja Nazeeruddin教授、Paul J.Dyson教授、赵康宁、西湖大学王睿研究员以及常州圣盛精工设备有限公司Jiang Sheng等人通过在钙钛矿前驱体溶液(PPS)中引入添加剂，改善了钙钛矿薄膜的质量和光伏(PV)性能选择。他们选择[Dmei]Cl作为添加剂，在PPS中引入[Dmei]Cl后，通过核磁共振(NMR)光谱观察到[Dmei]+阳离子的信号消失。制备的PSMs在27.2cm²的开口面积上实现了23.2%的认证PCE。封装后的PSM在85℃和85%相对湿度下、1.0-sun光照条件下，经过1900小时的最大功率点跟踪后，保留了初始PCE的87.0%。

结果分析， [MTTZ]+阳离子的原位形成增加了碘空位的形成能和碘化物和铯离子的迁移能垒，抑制了非辐射复合、热分解和相分离过程。[MTTZ]+阳离子和[DMA]+阳离子的原位形成通过NMR光谱得到证实，且通过XRD和STEM分析进一步揭示了其在钙钛矿薄膜中的存在。

Fig. 1. Reaction mechanism, morphology, elemental mapping, and crystal lattice of the [Dmei]Cl perovskite films. (A) Proposed mechanism for the in situ formation of the [MTTZ]+ and [DMA]+ cations. (B) Secondary electron image of the [Dmei]Cl film obtained using HIM. The red circle highlights 1D grains.(C) HIM-SIMS elemental mapping of 35Cl in blue and 127I in cyan. (D) Overlap elemental mapping of 133Cs in green and 208Pb in red. (E) High-resolution transmission electron microscopy (TEM) image of the [Dmei]Cl film. (F) Expansion of the pink dashed square in (E) corresponding to 1D perovskite. (G) Expansion of the green dashed square in (E) corresponding to 3D perovskite in the bulk region (left), and the corresponding interplanar spacing (right). (H) Expansion of the red dashed square in (E) corresponding to 3D perovskite in the edge region (left), and the corresponding interplanar spacing (right).

Fig. 2. In situ conductivity and local crystal structure of the perovskite films during thermal aging. The evolution of c-AFM maps at different heating intervals for the (A) control and (B) [Dmei]Cl films. (C) Comparison between experimental and calculated differential PDF spectra of fresh perovskite films. The contribution of the perovskite and SnO2 phases is highlighted in pink and orange, respectively, according to the simulation pattern of SnO2 and Cs0.05MA0.05FA0.9PbI3 perovskite. (D) Normalized Pb LIII edge x-ray absorption coefficient [m(E)] for the control and [Dmei]Cl films without and with thermal aging at 100°C for 24 hours. XAS spectra and fitting in R-space for (E) the control film before and after aging, and (F) the [Dmei]Cl film before and after aging. The dashed lines represent the experimentally determined data, and the solid blue lines correspond to simulated data. (G) The simulated Pb–I bond lengths and (H) Pb–I coordination numbers of the control and [Dmei]Cl films before and after aging.

Fig. 3. Light stress on the PL peak intensity and position of the perovskite films. In situ PL intensity maps on the same region of the (A) control and (B) [Dmei]Cl films over time under white-light illumination with an intensity of 450 mW cm−2 (equivalent to 4.5 suns). The corresponding PL peak position of the (C) control and (D) [Dmei]Cl films. Scale bars, 2 mm

Fig. 4. PV performance and long-term operational stability of PSMs. (A) The certified current-voltage (I-V) curves from forward and reverse scans of a [Dmei]Cl PSM with an aperture area of 27.2 cm2 from NPVM, China. (B) The certified stabilized efficiency of a [Dmei]Cl PSM. The inset in (B) is the relative spectral responsivity curve.(C) ISOS-L-1 stability protocols of the encapsulated PSMs measured under MPP tracking and continuous light irradiation with a white light-emitting diode (LED) lamp,100 mW·cm2 under ambient conditions. The initial PCE of the control and [Dmei]Cl PSMs are 21.3 and 23.1%, respectively. (D) The encapsulated PSMs measured under MPP tracking and continuous light irradiation with a white LED lamp,100 mW·cm2 at 85°C and 85% RH. The initial PCE of the control and [Dmei]Cl PSMs are 21.3 and 23.2%, respectively. (E) Schematic showing the roles of [MTTZ]+ and [DMA]+ in the 3D perovskite matrix.

本文来源：DOI: 10.1126/science.ado6619
https://www.science.org/doi/10.1126/science.ado6619

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