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

We report that 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. ¹H NMR methods are used to quantify the thermodynamics of ligand exchange on CsPbBr₃ QDs. Both oleic acid and oleylamine native ligands dynamically interact with the CsPbBr₃ 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 an irreversible ligand exchange. Undec-10-en-1-amine exergonically exchanges with oleylamine (K_eq = 2.52) at 25 °C. Finally, exchange occurs with carboxylic acids, phosphonic acids, and amines on CsPbBr₃ QDs without etching the nanocrystal surface; increases in steady-state PL intensities are correlated 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:: 2018-07-26

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; 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.  doi: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.  doi: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 = {We report that 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. 1H NMR methods are used to quantify the thermodynamics of ligand exchange on CsPbBr3 QDs. Both oleic acid and oleylamine native ligands dynamically interact with the CsPbBr3 QD surface, having individual surface densities of 1.2–1.7 nm–2. 10-Undecenoic acid undergoes an exergonic exchange equilibrium with bound oleate (Keq = 1.97) at 25 °C while 10-undecenylphosphonic acid undergoes an irreversible ligand exchange. Undec-10-en-1-amine exergonically exchanges with oleylamine (Keq = 2.52) at 25 °C. Finally, exchange occurs with carboxylic acids, phosphonic acids, and amines on CsPbBr3 QDs without etching the nanocrystal surface; increases in steady-state PL intensities are correlated 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         = {2018},

  month        = {7}

}

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DOI: https://doi.org/10.1002/anie.201806916

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

Abstract

Citation Formats

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