Quantifying the Thermodynamics of Ligand Binding to CsPbBr3 Quantum Dots

Smock, Sara R.; Williams, Travis J.; Brutchey, Richard L.

doi:10.1002/anie.201806916

Title: Quantifying the Thermodynamics of Ligand Binding to CsPbBr₃ Quantum Dots

Abstract

Abstract Cesium lead halide perovskites are an emerging class of quantum dots (QDs) that have shown promise in a variety of applications; however, their properties are highly dependent on their surface chemistry. To this point, the thermodynamics of ligand binding remain unstudied. Herein, ¹ H NMR methods were used to quantify the thermodynamics of ligand exchange on CsPbBr ₃ QDs. Both oleic acid and oleylamine native ligands dynamically interact with the CsPbBr ₃ QD surface, having individual surface densities of 1.2–1.7 nm ⁻² . 10‐Undecenoic acid undergoes an exergonic exchange equilibrium with bound oleate ( K _eq =1.97) at 25 °C while 10‐undecenylphosphonic acid undergoes irreversible ligand exchange. Undec‐10‐en‐1‐amine exergonically exchanges with oleylamine ( K _eq =2.52) at 25 °C. Exchange occurs with carboxylic acids, phosphonic acids, and amines on CsPbBr ₃ QDs without etching of the nanocrystal surface; increases in the steady‐state PL intensities correlate with more strongly bound conjugate base ligands.

Authors:

Smock, Sara R. ^[1]; Williams, Travis J. ^[2];

^[1]

Univ. of Southern California, Los Angeles, CA (United States)
Univ. of Southern California, Los Angeles, CA (United States). Loker Hydrocarbon Inst.

Publication Date:: Thu Jul 26 00:00:00 EDT 2018

Research Org.:: Univ. of Southern California, Los Angeles, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1582645

Alternate Identifier(s):: OSTI ID: 1463200

Grant/Contract Number:: SC0006812; FG02‐11ER46826

Resource Type:: Accepted Manuscript

Journal Name:: Angewandte Chemie (International Edition)

Additional Journal Information:: Journal Name: Angewandte Chemie (International Edition); Journal Volume: 57; Journal Issue: 36; Journal ID: ISSN 1433-7851

Publisher:: Wiley

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CsPbBr3; ligands; NMR spectroscopy; perovskites; quantum dots

Citation Formats


                    Smock, Sara R., Williams, Travis J., and Brutchey, Richard L. Quantifying the Thermodynamics of Ligand Binding to CsPbBr3 Quantum Dots.  United States: N. p., 2018. 
Web.  doi:10.1002/anie.201806916.

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                    Smock, Sara R., Williams, Travis J., & Brutchey, Richard L. Quantifying the Thermodynamics of Ligand Binding to CsPbBr3 Quantum Dots.  United States.  https://doi.org/10.1002/anie.201806916

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                    Smock, Sara R., Williams, Travis J., and Brutchey, Richard L. Thu .  
"Quantifying the Thermodynamics of Ligand Binding to CsPbBr3 Quantum Dots".  United States.  https://doi.org/10.1002/anie.201806916.  https://www.osti.gov/servlets/purl/1582645.

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@article{osti_1582645,

  title        = {Quantifying the Thermodynamics of Ligand Binding to CsPbBr3 Quantum Dots},

  author       = {Smock, Sara R. and Williams, Travis J. and Brutchey, Richard L.},

  abstractNote = {Abstract Cesium lead halide perovskites are an emerging class of quantum dots (QDs) that have shown promise in a variety of applications; however, their properties are highly dependent on their surface chemistry. To this point, the thermodynamics of ligand binding remain unstudied. Herein, 1 H NMR methods were used to quantify the thermodynamics of ligand exchange on CsPbBr 3 QDs. Both oleic acid and oleylamine native ligands dynamically interact with the CsPbBr 3 QD surface, having individual surface densities of 1.2–1.7 nm −2 . 10‐Undecenoic acid undergoes an exergonic exchange equilibrium with bound oleate ( K eq =1.97) at 25 °C while 10‐undecenylphosphonic acid undergoes irreversible ligand exchange. Undec‐10‐en‐1‐amine exergonically exchanges with oleylamine ( K eq =2.52) at 25 °C. Exchange occurs with carboxylic acids, phosphonic acids, and amines on CsPbBr 3 QDs without etching of the nanocrystal surface; increases in the steady‐state PL intensities correlate with more strongly bound conjugate base ligands.},

  doi          = {10.1002/anie.201806916},

  journal      = {Angewandte Chemie (International Edition)},

  number       = 36,

  volume       = 57,

  place        = {United States},

  year         = {Thu Jul 26 00:00:00 EDT 2018},

  month        = {Thu Jul 26 00:00:00 EDT 2018}

}

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Title: Quantifying the Thermodynamics of Ligand Binding to CsPbBr3 Quantum Dots

Abstract

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