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Benzylammonium‐Mediated Formamidinium Lead Iodide Perovskite Phase Stabilization for Photovoltaics

Anwar Qasem M Alanazi, Masaud Hassan S Almalki, Felix Thomas Eickemeyer, David Lyndon Emsley, Michael Graetzel, Ulf Anders Hagfeldt, Dominik Józef Kubicki, Jovana Milic, Aditya Mishra, Dan Ren, Zaiwei Wang, Shaik Mohammed Zakeeruddin, Hong Zhang

There is an ongoing surge of interest in the use of formamidinium (FA) lead iodide perovskites in photovoltaics due to their exceptional optoelectronic properties. However, thermodynamic instability of the desired cubic perovskite (α-FAPbI3) phase at ambient conditions leads to the formation of a yellow non-perovskite (δ-FAPbI3) phase that compromises its utility. A stable α-FAPbI3 perovskite phase is achieved by employing benzylammonium iodide (BzI) and the microscopic structure is elucidated by using solid-state NMR spectroscopy and X-ray scattering measurements. Perovskite solar cells based on the FAPbI3(BzI)0.25 composition achieve power conversion efficiencies exceeding 20%, which is accompanied by enhanced shelf-life and operational stability, maintaining 80% of the performance after one year at ambient conditions.

2021

Compositional Engineering of Perovskite Light Absorbers for Enhanced Stability and Performance through 2D/3D Interfacing

Anwar Qasem M Alanazi

The semiconducting hybrid-organic inorganic halide perovskites have excellent optical and electronic properties that attract the interest of scientists and researchers. Perovskite solar cells have seen the most rising-rate in the chart of solar cell efficiency from 3 to over 25% in less than ten years. In the last three years, most researchers have been focusing on the Î±-FAPbI3-based perovskite solar cells due to having a lower bandgap (1.45 eV) which is closer to the Shockley-Queisser optimum (1.1- 1.4eV) to gain high efficiency. A distinctive feature of FAPbI3 is that it is more thermally stable compared to MAPbI3. However, the Î±-FAPbI3 perovskite is not stable at room temperature as it converts to the undesirable ÎŽ-phase. The 2D- Ruddlesden-Popper-phase-doped 3D FAPbI3 enhancing the stability of the structure, albeit the bandgap is increased rendering a less optimal bandgap. The main achievement of this thesis is discovering that the doping of FAPbI3 with large alkyl ammonium moieties enhances efficiency and stability while maintaining the bandgap of pure Î±-FAPbI3 perovskite phase. I describe the resulting composition by the formula (A)xFAPbI3, where A represents the large alkyl ammonium iodide species. I study the stabilization of Î±-FAPbI3 via doping with 5-amino valeric acid hydroiodide (AVAI). By using solid-state NMR, we demonstrate the atomic-level interaction between this molecular modulator and the perovskite lattice and propose a structural model of the stabilized three-dimensional structure, further aided by density functional theory (DFT) calculations. We find the presence of AVAI produces highly crystalline films with large, micrometer-sized grains and enhanced charge-carrier lifetimes, as probed by transient absorption spectroscopy. Optical measurements confirm that there is no effect on the bandgap of FAPbI3 after doping. The devices based on (AVAI)0.25FAPbI3 exhibit superior operational stability in comparison with neat FAPbI3 while achieving power conversion efficiency of 19%. A similar approach based on benzylammonium iodide (BzI) has been used. The structural and optical characterization of films based on (BzI)xFAPbI3 composition demonstrate that there is no 2D phase forming under these conditions. Moreover, solid-state NMR results show BzI interacting on the atomic level with Î±-FAPbI3 by binding to the 3D perovskite through hydrogen bonding interaction and stabilizing it against the detrimental Î±-to-ÎŽ phase transition. Perovskite solar cells based on the (BzI)0.25FAPbI3composition achieve power conversion efficiencies exceeding 20%, which is accompanied by enhanced shelf-life and operational stability, maintaining 80% of the performance after one year at ambient conditions.Finally, films based on (BzI)0.25FAPbI3 compositions are further investigated upon aging under the ambient conditions, as they show an unexpected transition from black to red color without transition to expected yellow ÎŽ phase, unlike the reference FAPbI3. I perform different measurements to investigate the nature of this red phase as a function of annealing temperature compare these properties to the corresponding Ruddlesden-Popper phase (Bz2FAn-1PbnI3n+1). The red phase was found to be a mixture of a 2D phase (n = 2) Bz2FAPb2I7 and ÎŽ-FAPbI3, which acts as a barrier to the Î±-to-ÎŽ phase transition.

EPFL2021

Atomic-Level Microstructure of Efficient Formamidinium-Based Perovskite Solar Cells Stabilized by 5-Ammonium Valeric Acid Iodide Revealed by Multinuclear and Two-Dimensional Solid-State NMR

Anwar Qasem M Alanazi, Essa Awadh R Alharbi, Marine Eva Fedora Bouduban, David Lyndon Emsley, Fabrizio Giordano, Michael Graetzel, Farzaneh Jahanbakhshi, Dominik Józef Kubicki, Jovana Milic, Marko Mladenovic, Jacques-Edouard Moser, Daniel Prochowicz, Dan Ren, Ursula Röthlisberger, Shaik Mohammed Zakeeruddin

Chemical doping of inorganic–organic hybrid perovskites is an effective way of improving the performance and operational stability of perovskite solar cells (PSCs). Here we use 5-ammonium valeric acid iodide (AVAI) to chemically stabilize the structure of α-FAPbI3. Using solid-state MAS NMR, we demonstrate the atomic-level interaction between the molecular modulator and the perovskite lattice and propose a structural model of the stabilized three-dimensional structure, further aided by density functional theory (DFT) calculations. We find that one-step deposition of the perovskite in the presence of AVAI produces highly crystalline films with large, micrometer-sized grains and enhanced charge-carrier lifetimes, as probed by transient absorption spectroscopy. As a result, we achieve greatly enhanced solar cell performance for the optimized AVA-based devices with a maximum power conversion efficiency (PCE) of 18.94%. The devices retain 90% of the initial efficiency after 300 h under continuous white light illumination and maximum-power point-tracking measurement.

2019