Germanium Halides Serving as Ideal Precursors: Designing a More Effective and Less Toxic Route to High-Optoelectronic-Quality Metal Halide Perovskite Nanocrystals

Xiaochen Wang; Tianxin Bai; Bin Yang; Ruiling Zhang; Daoyuan Zheng; Junke Jiang; Shuxia Tao; Feng Liu; Ke Li Han

doi:10.1021/acs.nanolett.1c03527

Germanium Halides Serving as Ideal Precursors: Designing a More Effective and Less Toxic Route to High-Optoelectronic-Quality Metal Halide Perovskite Nanocrystals

Xiaochen Wang, Tianxin Bai, Bin Yang, Ruiling Zhang, Daoyuan Zheng, Junke Jiang, Shuxia Tao, Feng Liu (Corresponding author), Ke Li Han (Corresponding author)

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Abstract

The three-precursors approach has proven to be advantageous for obtaining high-quality metal halide perovskite nanocrystals (PNCs). However, the current halide precursors of choice are mainly limited to those highly toxic organohalides, being unfavorable for large-scale and sustainable use. Moreover, most of the resulting PNCs still suffer from low quality in terms of photoluminescence quantum yield (PLQY). Herein we present all-inorganic germanium salts, GeX4 (X = Cl, Br, I), serving as robust and less hazardous alternatives that are capable of ensuring improved material properties for both Pb-based and Pb-free PNCs. Importantly, unlike most of the other inorganic halide sources, the GeX4 compound does not deliver the Ge element into the final compositions, whereas the PLQY and phase stability of the resulting nanocrystals are significantly improved. Theoretical calculations suggest that Ge halide precursors provide favorable conditions in both dielectric environment and thermodynamics, which jointly contribute to the formation of size-confined defect-suppressed nanoparticles.

Original language	English
Pages (from-to)	636-643
Number of pages	8
Journal	Nano Letters
Volume	22
Issue number	2
DOIs	https://doi.org/10.1021/acs.nanolett.1c03527
Publication status	Published - 26 Jan 2022

Bibliographical note

Funding Information:
This work was conducted by the Fundamental Research Center of Artificial Photosynthesis, financially supported by the National Natural Science Foundation of China (Nos. 22088102 and 22179072) and the Qilu Youth Scholar Funding of Shandong University (No. 62460082163114). S.T. and J.J. acknowledge funding by the Computational Sciences for Energy Research tenure track program of Shell and NWO (No. 15CST04-2), as well as the NWO START-UP from The Netherlands.

Funding

This work was conducted by the Fundamental Research Center of Artificial Photosynthesis, financially supported by the National Natural Science Foundation of China (Nos. 22088102 and 22179072) and the Qilu Youth Scholar Funding of Shandong University (No. 62460082163114). S.T. and J.J. acknowledge funding by the Computational Sciences for Energy Research tenure track program of Shell and NWO (No. 15CST04-2), as well as the NWO START-UP from The Netherlands.

Keywords

Colloidal Synthesis
Germanium Halides
Lead-Free Perovskite
Perovskite Nanocrystals

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10.1021/acs.nanolett.1c03527

26/7/22pdfFinal published version, 4.77 MBLicence: TAVERNE

Cite this

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title = "Germanium Halides Serving as Ideal Precursors: Designing a More Effective and Less Toxic Route to High-Optoelectronic-Quality Metal Halide Perovskite Nanocrystals",

abstract = "The three-precursors approach has proven to be advantageous for obtaining high-quality metal halide perovskite nanocrystals (PNCs). However, the current halide precursors of choice are mainly limited to those highly toxic organohalides, being unfavorable for large-scale and sustainable use. Moreover, most of the resulting PNCs still suffer from low quality in terms of photoluminescence quantum yield (PLQY). Herein we present all-inorganic germanium salts, GeX4 (X = Cl, Br, I), serving as robust and less hazardous alternatives that are capable of ensuring improved material properties for both Pb-based and Pb-free PNCs. Importantly, unlike most of the other inorganic halide sources, the GeX4 compound does not deliver the Ge element into the final compositions, whereas the PLQY and phase stability of the resulting nanocrystals are significantly improved. Theoretical calculations suggest that Ge halide precursors provide favorable conditions in both dielectric environment and thermodynamics, which jointly contribute to the formation of size-confined defect-suppressed nanoparticles.",

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author = "Xiaochen Wang and Tianxin Bai and Bin Yang and Ruiling Zhang and Daoyuan Zheng and Junke Jiang and Shuxia Tao and Feng Liu and Han, {Ke Li}",

note = "Funding Information: This work was conducted by the Fundamental Research Center of Artificial Photosynthesis, financially supported by the National Natural Science Foundation of China (Nos. 22088102 and 22179072) and the Qilu Youth Scholar Funding of Shandong University (No. 62460082163114). S.T. and J.J. acknowledge funding by the Computational Sciences for Energy Research tenure track program of Shell and NWO (No. 15CST04-2), as well as the NWO START-UP from The Netherlands. ",

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AU - Wang, Xiaochen

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AU - Yang, Bin

AU - Zhang, Ruiling

AU - Zheng, Daoyuan

AU - Jiang, Junke

AU - Tao, Shuxia

AU - Liu, Feng

AU - Han, Ke Li

N1 - Funding Information: This work was conducted by the Fundamental Research Center of Artificial Photosynthesis, financially supported by the National Natural Science Foundation of China (Nos. 22088102 and 22179072) and the Qilu Youth Scholar Funding of Shandong University (No. 62460082163114). S.T. and J.J. acknowledge funding by the Computational Sciences for Energy Research tenure track program of Shell and NWO (No. 15CST04-2), as well as the NWO START-UP from The Netherlands.

PY - 2022/1/26

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N2 - The three-precursors approach has proven to be advantageous for obtaining high-quality metal halide perovskite nanocrystals (PNCs). However, the current halide precursors of choice are mainly limited to those highly toxic organohalides, being unfavorable for large-scale and sustainable use. Moreover, most of the resulting PNCs still suffer from low quality in terms of photoluminescence quantum yield (PLQY). Herein we present all-inorganic germanium salts, GeX4 (X = Cl, Br, I), serving as robust and less hazardous alternatives that are capable of ensuring improved material properties for both Pb-based and Pb-free PNCs. Importantly, unlike most of the other inorganic halide sources, the GeX4 compound does not deliver the Ge element into the final compositions, whereas the PLQY and phase stability of the resulting nanocrystals are significantly improved. Theoretical calculations suggest that Ge halide precursors provide favorable conditions in both dielectric environment and thermodynamics, which jointly contribute to the formation of size-confined defect-suppressed nanoparticles.

AB - The three-precursors approach has proven to be advantageous for obtaining high-quality metal halide perovskite nanocrystals (PNCs). However, the current halide precursors of choice are mainly limited to those highly toxic organohalides, being unfavorable for large-scale and sustainable use. Moreover, most of the resulting PNCs still suffer from low quality in terms of photoluminescence quantum yield (PLQY). Herein we present all-inorganic germanium salts, GeX4 (X = Cl, Br, I), serving as robust and less hazardous alternatives that are capable of ensuring improved material properties for both Pb-based and Pb-free PNCs. Importantly, unlike most of the other inorganic halide sources, the GeX4 compound does not deliver the Ge element into the final compositions, whereas the PLQY and phase stability of the resulting nanocrystals are significantly improved. Theoretical calculations suggest that Ge halide precursors provide favorable conditions in both dielectric environment and thermodynamics, which jointly contribute to the formation of size-confined defect-suppressed nanoparticles.

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Germanium Halides Serving as Ideal Precursors: Designing a More Effective and Less Toxic Route to High-Optoelectronic-Quality Metal Halide Perovskite Nanocrystals

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