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Title: Synthesis, Characterization, and Stability Studies of Ge-Based Perovskites of Controllable Mixed Cation Composition, Produced with an Ambient Surfactant-Free Approach

Abstract

In this study, we have applied a facile, ligand-free, ambient synthesis protocol toward the fabrication of not only a series of lead-free Ge-based perovskites with the general formulation of MA 1-xFA xGeI 3 (where x was changed from 0, 0.25, 0.5, 0.75, to 1) but also CsGeI 3. Specifically, our methodology for producing ABX 3 systems is generalizable, regardless of the identity of either the A site cation or the X site halide ion. Moreover, it incorporates many advantages, including (i) the possibility of efficiently generating pure Ge-based perovskite particles of any desired chemical composition, (ii) the use of readily available, commercial precursors and comparatively lower toxicity solvents, (iii) the practicality of scale up, and (iv) the elimination of the need for any superfluous organic surface ligands or surfactants. In addition to providing mechanistic insights into their formation, we have examined the chemical composition, crystallite size, morphology, surface attributes, oxidation states, and optical properties of our as-prepared perovskites using a combination of diffraction, microscopy, and spectroscopy techniques. Specifically, we noted that the optical band gap could be reliably tuned as a function of chemical composition, via the identity of the A site cation. Moreover, we have probed their stability, notmore » only under standard storage conditions but also, for the first time, when subjected to both e-beam- and X-ray-induced degradation, using cumulative data from sources such as synchrotron-based scanning hard X-ray microscopy. Importantly, of relevance for the potential practical incorporation of these Pb-free perovskites, our work has emphasized the possibility of controlling the chemical composition within Ge-based perovskites as a means of rationally tuning their observed band gaps and optical behavior.« less

Authors:
 [1];  [1];  [2];  [2]; ORCiD logo [3];  [3]; ORCiD logo [1]
  1. State Univ. of New York (SUNY), Stony Brook, NY (United States). Dept. of Chemistry
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Publication Date:
Research Org.:
Stony Brook Univ., NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1571538
Alternate Identifier(s):
OSTI ID: 1573215
Grant/Contract Number:  
SC0012704
Resource Type:
Published Article
Journal Name:
ACS Omega
Additional Journal Information:
Journal Volume: 4; Journal Issue: 19; Journal ID: ISSN 2470-1343
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Yue, Shiyu, McGuire, Scott C., Yan, Hanfei, Chu, Yong S., Cotlet, Mircea, Tong, Xiao, and Wong, Stanislaus S. Synthesis, Characterization, and Stability Studies of Ge-Based Perovskites of Controllable Mixed Cation Composition, Produced with an Ambient Surfactant-Free Approach. United States: N. p., 2019. Web. doi:10.1021/acsomega.9b02203.
Yue, Shiyu, McGuire, Scott C., Yan, Hanfei, Chu, Yong S., Cotlet, Mircea, Tong, Xiao, & Wong, Stanislaus S. Synthesis, Characterization, and Stability Studies of Ge-Based Perovskites of Controllable Mixed Cation Composition, Produced with an Ambient Surfactant-Free Approach. United States. doi:10.1021/acsomega.9b02203.
Yue, Shiyu, McGuire, Scott C., Yan, Hanfei, Chu, Yong S., Cotlet, Mircea, Tong, Xiao, and Wong, Stanislaus S. Tue . "Synthesis, Characterization, and Stability Studies of Ge-Based Perovskites of Controllable Mixed Cation Composition, Produced with an Ambient Surfactant-Free Approach". United States. doi:10.1021/acsomega.9b02203.
@article{osti_1571538,
title = {Synthesis, Characterization, and Stability Studies of Ge-Based Perovskites of Controllable Mixed Cation Composition, Produced with an Ambient Surfactant-Free Approach},
author = {Yue, Shiyu and McGuire, Scott C. and Yan, Hanfei and Chu, Yong S. and Cotlet, Mircea and Tong, Xiao and Wong, Stanislaus S.},
abstractNote = {In this study, we have applied a facile, ligand-free, ambient synthesis protocol toward the fabrication of not only a series of lead-free Ge-based perovskites with the general formulation of MA1-xFAxGeI3 (where x was changed from 0, 0.25, 0.5, 0.75, to 1) but also CsGeI3. Specifically, our methodology for producing ABX3 systems is generalizable, regardless of the identity of either the A site cation or the X site halide ion. Moreover, it incorporates many advantages, including (i) the possibility of efficiently generating pure Ge-based perovskite particles of any desired chemical composition, (ii) the use of readily available, commercial precursors and comparatively lower toxicity solvents, (iii) the practicality of scale up, and (iv) the elimination of the need for any superfluous organic surface ligands or surfactants. In addition to providing mechanistic insights into their formation, we have examined the chemical composition, crystallite size, morphology, surface attributes, oxidation states, and optical properties of our as-prepared perovskites using a combination of diffraction, microscopy, and spectroscopy techniques. Specifically, we noted that the optical band gap could be reliably tuned as a function of chemical composition, via the identity of the A site cation. Moreover, we have probed their stability, not only under standard storage conditions but also, for the first time, when subjected to both e-beam- and X-ray-induced degradation, using cumulative data from sources such as synchrotron-based scanning hard X-ray microscopy. Importantly, of relevance for the potential practical incorporation of these Pb-free perovskites, our work has emphasized the possibility of controlling the chemical composition within Ge-based perovskites as a means of rationally tuning their observed band gaps and optical behavior.},
doi = {10.1021/acsomega.9b02203},
journal = {ACS Omega},
number = 19,
volume = 4,
place = {United States},
year = {2019},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1021/acsomega.9b02203

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