Ethylenediamine Addition Improves Performance and Suppresses Phase Instabilities in Mixed-Halide Perovskites

Margherita Taddei; Joel A. Smith; Benjamin M. Gallant; Suer Zhou; Robert J.E. Westbrook; Yangwei Shi; Jian Wang; James N. Drysdale; Declan P. McCarthy; Stephen Barlow; Seth R. Marder; Henry J. Snaith; David S. Ginger

doi:10.1021/acsenergylett.2c01998

Ethylenediamine Addition Improves Performance and Suppresses Phase Instabilities in Mixed-Halide Perovskites

Margherita Taddei, Joel A. Smith, Benjamin M. Gallant, Suer Zhou, Robert J.E. Westbrook, Yangwei Shi, Jian Wang, James N. Drysdale, Declan P. McCarthy, Stephen Barlow, Seth R. Marder, Henry J. Snaith, David S. Ginger^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Letter › peer-review

Abstract

We show that adding ethylenediamine (EDA) to perovskite precursor solutions improves the photovoltaic device performance and material stability of high-bromide-content, methylammonium-free, formamidinium cesium lead halide perovskites FA1–xCsxPb(I1–yBry)3, which are currently of interest for perovskite-on-Si tandem solar cells. Using spectroscopy and hyperspectral microscopy, we show that the additive improves film homogeneity and suppresses the phase instability that is ubiquitous in high-Br perovskite formulations, producing films that remain stable for over 100 days in ambient conditions. With the addition of 1 mol % EDA, we demonstrate 1.69 eV-gap perovskite single-junction p-i-n devices with a VOC of 1.22 V and a champion maximum-power-point-tracked power conversion efficiency of 18.8%, comparable to the best reported methylammonium-free perovskites. Using nuclear magnetic resonance (NMR) spectroscopy and X-ray diffraction techniques, we show that EDA reacts with FA+ in solution, rapidly and quantitatively forming imidazolinium cations. It is the presence of imidazolinium during crystallization which drives the improved perovskite thin-film properties.

Original language	English
Pages (from-to)	4265-4273
Number of pages	9
Journal	ACS Energy Letters
Volume	7
Issue number	12
Early online date	2 Nov 2022
DOIs	https://doi.org/10.1021/acsenergylett.2c01998
Publication status	Published - 9 Dec 2022

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Taddei, M., Smith, J. A., Gallant, B. M., Zhou, S., Westbrook, R. J. E., Shi, Y., Wang, J., Drysdale, J. N., McCarthy, D. P., Barlow, S., Marder, S. R., Snaith, H. J., & Ginger, D. S. (2022). Ethylenediamine Addition Improves Performance and Suppresses Phase Instabilities in Mixed-Halide Perovskites. ACS Energy Letters, 7(12), 4265-4273. https://doi.org/10.1021/acsenergylett.2c01998

@article{d03f61e7c0b744fa9d2222f04ae3cca9,

title = "Ethylenediamine Addition Improves Performance and Suppresses Phase Instabilities in Mixed-Halide Perovskites",

abstract = "We show that adding ethylenediamine (EDA) to perovskite precursor solutions improves the photovoltaic device performance and material stability of high-bromide-content, methylammonium-free, formamidinium cesium lead halide perovskites FA1–xCsxPb(I1–yBry)3, which are currently of interest for perovskite-on-Si tandem solar cells. Using spectroscopy and hyperspectral microscopy, we show that the additive improves film homogeneity and suppresses the phase instability that is ubiquitous in high-Br perovskite formulations, producing films that remain stable for over 100 days in ambient conditions. With the addition of 1 mol % EDA, we demonstrate 1.69 eV-gap perovskite single-junction p-i-n devices with a VOC of 1.22 V and a champion maximum-power-point-tracked power conversion efficiency of 18.8%, comparable to the best reported methylammonium-free perovskites. Using nuclear magnetic resonance (NMR) spectroscopy and X-ray diffraction techniques, we show that EDA reacts with FA+ in solution, rapidly and quantitatively forming imidazolinium cations. It is the presence of imidazolinium during crystallization which drives the improved perovskite thin-film properties.",

author = "Margherita Taddei and Smith, {Joel A.} and Gallant, {Benjamin M.} and Suer Zhou and Westbrook, {Robert J.E.} and Yangwei Shi and Jian Wang and Drysdale, {James N.} and McCarthy, {Declan P.} and Stephen Barlow and Marder, {Seth R.} and Snaith, {Henry J.} and Ginger, {David S.}",

year = "2022",

month = dec,

day = "9",

doi = "10.1021/acsenergylett.2c01998",

language = "English",

volume = "7",

pages = "4265--4273",

journal = "ACS Energy Letters",

issn = "2380-8195",

publisher = "American Chemical Society",

number = "12",

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TY - JOUR

T1 - Ethylenediamine Addition Improves Performance and Suppresses Phase Instabilities in Mixed-Halide Perovskites

AU - Taddei, Margherita

AU - Smith, Joel A.

AU - Gallant, Benjamin M.

AU - Zhou, Suer

AU - Westbrook, Robert J.E.

AU - Shi, Yangwei

AU - Wang, Jian

AU - Drysdale, James N.

AU - McCarthy, Declan P.

AU - Barlow, Stephen

AU - Marder, Seth R.

AU - Snaith, Henry J.

AU - Ginger, David S.

PY - 2022/12/9

Y1 - 2022/12/9

N2 - We show that adding ethylenediamine (EDA) to perovskite precursor solutions improves the photovoltaic device performance and material stability of high-bromide-content, methylammonium-free, formamidinium cesium lead halide perovskites FA1–xCsxPb(I1–yBry)3, which are currently of interest for perovskite-on-Si tandem solar cells. Using spectroscopy and hyperspectral microscopy, we show that the additive improves film homogeneity and suppresses the phase instability that is ubiquitous in high-Br perovskite formulations, producing films that remain stable for over 100 days in ambient conditions. With the addition of 1 mol % EDA, we demonstrate 1.69 eV-gap perovskite single-junction p-i-n devices with a VOC of 1.22 V and a champion maximum-power-point-tracked power conversion efficiency of 18.8%, comparable to the best reported methylammonium-free perovskites. Using nuclear magnetic resonance (NMR) spectroscopy and X-ray diffraction techniques, we show that EDA reacts with FA+ in solution, rapidly and quantitatively forming imidazolinium cations. It is the presence of imidazolinium during crystallization which drives the improved perovskite thin-film properties.

AB - We show that adding ethylenediamine (EDA) to perovskite precursor solutions improves the photovoltaic device performance and material stability of high-bromide-content, methylammonium-free, formamidinium cesium lead halide perovskites FA1–xCsxPb(I1–yBry)3, which are currently of interest for perovskite-on-Si tandem solar cells. Using spectroscopy and hyperspectral microscopy, we show that the additive improves film homogeneity and suppresses the phase instability that is ubiquitous in high-Br perovskite formulations, producing films that remain stable for over 100 days in ambient conditions. With the addition of 1 mol % EDA, we demonstrate 1.69 eV-gap perovskite single-junction p-i-n devices with a VOC of 1.22 V and a champion maximum-power-point-tracked power conversion efficiency of 18.8%, comparable to the best reported methylammonium-free perovskites. Using nuclear magnetic resonance (NMR) spectroscopy and X-ray diffraction techniques, we show that EDA reacts with FA+ in solution, rapidly and quantitatively forming imidazolinium cations. It is the presence of imidazolinium during crystallization which drives the improved perovskite thin-film properties.

U2 - 10.1021/acsenergylett.2c01998

DO - 10.1021/acsenergylett.2c01998

M3 - Letter

SN - 2380-8195

VL - 7

SP - 4265

EP - 4273

JO - ACS Energy Letters

JF - ACS Energy Letters

IS - 12

ER -

Ethylenediamine Addition Improves Performance and Suppresses Phase Instabilities in Mixed-Halide Perovskites

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