CsPbBr 3 –CdS heterostructure: stabilizing perovskite nanocrystals for photocatalysis

Kipkorir, Anthony; DuBose, Jeffrey; Cho, Junsang; Kamat, Prashant V.

doi:10.1039/D1SC04305F

Title: CsPbBr ₃ –CdS heterostructure: stabilizing perovskite nanocrystals for photocatalysis

Abstract

The instability of cesium lead bromide (CsPbBr3) nanocrystals (NCs) in polar solvents has hampered their use in photocatalysis. We have now succeeded in synthesizing CsPbBr₃–CdS heterostructures with improved stability and photocatalytic performance. While the CdS deposition provides solvent stability, the parent CsPbBr₃ in the heterostructure harvests photons to generate charge carriers. This heterostructure exhibits longer emission lifetime (τ_ave = 47 ns) than pristine CsPbBr₃ (τ_ave = 7 ns), indicating passivation of surface defects. We employed ethyl viologen (EV²⁺) as a probe molecule to elucidate excited state interactions and interfacial electron transfer of CsPbBr₃–CdS NCs in toluene/ethanol mixed solvent. The electron transfer rate constant as obtained from transient absorption spectroscopy was 9.5 × 10¹⁰ s-¹ and the quantum efficiency of ethyl viologen reduction (Φ_EV+˙) was found to be 8.4% under visible light excitation. The Fermi level equilibration between CsPbBr₃–CdS and EV²⁺/EV⁺˙ redox couple has allowed us to estimate the apparent conduction band energy of the heterostructure as -0.365 V vs. NHE. The insights into effective utilization of perovskite nanocrystals built around a quasi-type II heterostructures pave the way towards effective utilization in photocatalytic reduction and oxidation processes.

Authors:

Kipkorir, Anthony ^[1];

^[1]; Cho, Junsang ^[2];

^[3]

Radiation Laboratory, University of Notre Dame, Notre Dame, Indiana 46556, USA, Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, USA
Radiation Laboratory, University of Notre Dame, Notre Dame, Indiana 46556, USA
Radiation Laboratory, University of Notre Dame, Notre Dame, Indiana 46556, USA, Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, USA, Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana 46556, USA

Publication Date:: Wed Nov 17 00:00:00 EST 2021

Research Org.:: University of Notre Dame, IN (United States)

Sponsoring Org.:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Forgash Fellowship for Solar Energy Research

OSTI Identifier:: 1828238

Alternate Identifier(s):: OSTI ID: 1830680

Grant/Contract Number:: FC02-04ER15533

Resource Type:: Published Article

Journal Name:: Chemical Science

Additional Journal Information:: Journal Name: Chemical Science Journal Volume: 12 Journal Issue: 44; Journal ID: ISSN 2041-6520

Publisher:: Royal Society of Chemistry (RSC)

Country of Publication:: United Kingdom

Language:: English

Subject:: 14 SOLAR ENERGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats


                    Kipkorir, Anthony, DuBose, Jeffrey, Cho, Junsang, and Kamat, Prashant V. CsPbBr 3 –CdS heterostructure: stabilizing perovskite nanocrystals for photocatalysis.  United Kingdom: N. p., 2021. 
Web.  doi:10.1039/D1SC04305F.

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                    Kipkorir, Anthony, DuBose, Jeffrey, Cho, Junsang, & Kamat, Prashant V. CsPbBr 3 –CdS heterostructure: stabilizing perovskite nanocrystals for photocatalysis.  United Kingdom.  https://doi.org/10.1039/D1SC04305F

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                    Kipkorir, Anthony, DuBose, Jeffrey, Cho, Junsang, and Kamat, Prashant V. Wed .  
"CsPbBr 3 –CdS heterostructure: stabilizing perovskite nanocrystals for photocatalysis".  United Kingdom.  https://doi.org/10.1039/D1SC04305F.

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@article{osti_1828238,

  title        = {CsPbBr 3 –CdS heterostructure: stabilizing perovskite nanocrystals for photocatalysis},

  author       = {Kipkorir, Anthony and DuBose, Jeffrey and Cho, Junsang and Kamat, Prashant V.},

  abstractNote = {The instability of cesium lead bromide (CsPbBr3) nanocrystals (NCs) in polar solvents has hampered their use in photocatalysis. We have now succeeded in synthesizing CsPbBr3–CdS heterostructures with improved stability and photocatalytic performance. While the CdS deposition provides solvent stability, the parent CsPbBr3 in the heterostructure harvests photons to generate charge carriers. This heterostructure exhibits longer emission lifetime (τave = 47 ns) than pristine CsPbBr3 (τave = 7 ns), indicating passivation of surface defects. We employed ethyl viologen (EV2+) as a probe molecule to elucidate excited state interactions and interfacial electron transfer of CsPbBr3–CdS NCs in toluene/ethanol mixed solvent. The electron transfer rate constant as obtained from transient absorption spectroscopy was 9.5 × 1010 s-1 and the quantum efficiency of ethyl viologen reduction (ΦEV+˙) was found to be 8.4% under visible light excitation. The Fermi level equilibration between CsPbBr3–CdS and EV2+/EV+˙ redox couple has allowed us to estimate the apparent conduction band energy of the heterostructure as -0.365 V vs. NHE. The insights into effective utilization of perovskite nanocrystals built around a quasi-type II heterostructures pave the way towards effective utilization in photocatalytic reduction and oxidation processes.},

  doi          = {10.1039/D1SC04305F},

  journal      = {Chemical Science},

  number       = 44,

  volume       = 12,

  place        = {United Kingdom},

  year         = {Wed Nov 17 00:00:00 EST 2021},

  month        = {Wed Nov 17 00:00:00 EST 2021}

}

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One-Pot Synthesis of Highly Stable CsPbBr 3 @SiO 2 Core–Shell Nanoparticles journal, July 2018

Mechanisms for Adsorption of Methyl Viologen on CdS Quantum Dots journal, February 2014

Seeded Growth of Highly Luminescent CdSe/CdS Nanoheterostructures with Rod and Tetrapod Morphologies journal, October 2007

Recent Advances in Quantum Dot Surface Chemistry journal, February 2014

Bidentate Ligand-Passivated CsPbI 3 Perovskite Nanocrystals for Stable Near-Unity Photoluminescence Quantum Yield and Efficient Red Light-Emitting Diodes journal, December 2017

Surface Chemistry Matters. How Ligands Influence Excited State Interactions between CsPbBr 3 and Methyl Viologen journal, May 2020

Principles of Fluorescence Spectroscopy book, January 2006

Perspectives on the Physical Chemistry of Semiconductor Nanocrystals journal, January 1996

Metal Semiconductor Heterostructures for Photocatalytic Conversion of Light Energy journal, March 2015

Core–Shell CsPbBr 3 @CdS Quantum Dots with Enhanced Stability and Photoluminescence Quantum Yields for Optoelectronic Devices journal, July 2020

Ultrafast Interfacial Electron and Hole Transfer from CsPbBr 3 Perovskite Quantum Dots journal, September 2015

State of the Art and Prospects for Halide Perovskite Nanocrystals journal, June 2021

Effect of Surface Ligand on Charge Separation and Recombination at CsPbI 3 Perovskite Quantum Dot/TiO 2 Interfaces journal, August 2019

The Surface Chemistry and Structure of Colloidal Lead Halide Perovskite Nanocrystals journal, January 2021

New understanding on the different photocatalytic activity of wurtzite and zinc-blende CdS journal, September 2016

Water resistant CsPbX 3 nanocrystals coated with polyhedral oligomeric silsesquioxane and their use as solid state luminophores in all-perovskite white light-emitting devices journal, January 2016

A Nanocrystal Catalyst Incorporating a Surface Bound Transition Metal to Induce Photocatalytic Sequential Electron Transfer Events journal, July 2021

Complete ultrafast charge carrier dynamics in photo-excited all-inorganic perovskite nanocrystals (CsPbX 3 ) journal, January 2017

Ultrafast Exciton Dynamics in Colloidal CsPbBr 3 Perovskite Nanocrystals: Biexciton Effect and Auger Recombination journal, February 2017

Perovskite Photocatalysis. Methyl Viologen Induces Unusually Long-Lived Charge Carrier Separation in CsPbBr 3 Nanocrystals journal, December 2019

CsPbBr 3 /ZnS Core/Shell Type Nanocrystals for Enhancing Luminescence Lifetime and Water Stability journal, May 2020

Photocatalysis with CdSe Nanoparticles in Confined Media: Mapping Charge Transfer Events in the Subpicosecond to Second Timescales journal, February 2009

Highly stable, luminescent core–shell type methylammonium–octylammonium lead bromide layered perovskite nanoparticles journal, January 2016

Probing Perovskite Photocatalysis. Interfacial Electron Transfer between CsPbBr 3 and Ferrocene Redox Couple journal, September 2019

Solar-Driven Metal Halide Perovskite Photocatalysis: Design, Stability, and Performance journal, March 2020

On the crystal structure of colloidally prepared CsPbBr 3 quantum dots journal, January 2016

Photoelectrochemistry in particulate systems. 4. Photosensitization of a titanium dioxide semiconductor with a chlorophyll analog journal, March 1986

Highly Luminescent Monodisperse CdSe and CdSe/ZnS Nanocrystals Synthesized in a Hexadecylamine−Trioctylphosphine Oxide−Trioctylphospine Mixture journal, April 2001

Quantum Dot Sensitized Solar Cells. A Tale of Two Semiconductor Nanocrystals: CdSe and CdTe journal, May 2009

Efficient and Stable Luminescence from Mn 2+ in Core and Core–Isocrystalline Shell CsPbCl 3 Perovskite Nanocrystals journal, May 2017

Metal halide perovskite nanomaterials: synthesis and applications journal, January 2017

Photocatalytic and Photoelectrochemical Degradation of Organic Compounds with All-Inorganic Metal Halide Perovskite Quantum Dots journal, January 2019

Enhanced Stability and Tunable Photoluminescence in Perovskite CsPbX 3 /ZnS Quantum Dot Heterostructure journal, April 2017

CdSe/CdS Nanorod Photocatalysts: Tuning the Interfacial Charge Transfer Process through Shell Length journal, July 2015

Challenges and Opportunities in Designing Perovskite Nanocrystal Heterostructures journal, June 2020

Efficient and Selective Photocatalytic Oxidation of Benzylic Alcohols with Hybrid Organic–Inorganic Perovskite Materials journal, February 2018

All Inorganic Halide Perovskites Nanosystem: Synthesis, Structural Features, Optical Properties and Optoelectronic Applications journal, January 2017

Synthesis and Micrometer-Scale Assembly of Colloidal CdSe/CdS Nanorods Prepared by a Seeded Growth Approach journal, October 2007

Semiconductor Surface Chemistry as Holy Grail in Photocatalysis and Photovoltaics journal, March 2017

Novel B-site Cd2+ doped CsPbBr3 quantum dot glass toward strong fluorescence and high stability for wLED journal, September 2020

Strongly emissive perovskite nanocrystal inks for high-voltage solar cells journal, December 2016

Switchable Anion Exchange in Polymer-Encapsulated APbX 3 Nanocrystals Delivers Stable All-Perovskite White Emitters journal, July 2021

Ultrafast Charge Separation in Two-Dimensional CsPbBr 3 Perovskite Nanoplatelets journal, January 2019

Facile Synthesis of ZnS−AgInS 2 Solid Solution Nanoparticles for a Color-Adjustable Luminophore journal, October 2007

Mechanistic Understanding and Rational Design of Quantum Dot/Mediator Interfaces for Efficient Photon Upconversion journal, November 2020

Metal Halide Perovskite Nanocrystals: Synthesis, Post-Synthesis Modifications, and Their Optical Properties journal, February 2019

Synthesis and Properties of Biocompatible Water-Soluble Silica-Coated CdSe/ZnS Semiconductor Quantum Dots † journal, September 2001

Mechanism of Efficient Viologen Radical Generation by Ultrafast Electron Transfer from CdS Quantum Dots journal, March 2018

Nanocrystals of Cesium Lead Halide Perovskites (CsPbX 3 , X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut journal, February 2015

Synthesis of highly luminescent wurtzite CdSe/CdS giant-shell nanocrystals using a fast continuous injection route journal, January 2014

Luminescence Photophysics in Semiconductor Nanocrystals journal, November 1998

Title: CsPbBr ₃ –CdS heterostructure: stabilizing perovskite nanocrystals for photocatalysis

Perovskite Nanocrystal Heterostructures: Synthesis, Optical Properties, and Applications
journal, August 2020

Strain-Driven Stacking Faults in CdSe/CdS Core/Shell Nanorods
journal, March 2018

Improving the Stability of CsPbBr ₃ Nanocrystals in Ethanol by Capping with PbBr ₂ -Adlayers
journal, April 2019

Halide Perovskite Nanocrystal Photocatalysts for CO ₂ Reduction: Successes and Challenges
journal, July 2020

Synthesis and characterization of nearly monodisperse CdE (E = sulfur, selenium, tellurium) semiconductor nanocrystallites
journal, September 1993

Step-Wise Synthesis of InP/ZnS Core−Shell Quantum Dots and the Role of Zinc Acetate
journal, February 2009

Hierarchical Arrays of Cesium Lead Halide Perovskite Nanocrystals through Electrophoretic Deposition
journal, June 2018

Band Edge Energies and Excitonic Transition Probabilities of Colloidal CsPbX ₃ (X = Cl, Br, I) Perovskite Nanocrystals
journal, September 2016

Highly Luminescent and Stable Halide Perovskite Nanocrystals
journal, February 2019

One-Pot Synthesis of Highly Stable CsPbBr ₃ @SiO ₂ Core–Shell Nanoparticles
journal, July 2018

Mechanisms for Adsorption of Methyl Viologen on CdS Quantum Dots
journal, February 2014

Seeded Growth of Highly Luminescent CdSe/CdS Nanoheterostructures with Rod and Tetrapod Morphologies
journal, October 2007

Recent Advances in Quantum Dot Surface Chemistry
journal, February 2014

Bidentate Ligand-Passivated CsPbI ₃ Perovskite Nanocrystals for Stable Near-Unity Photoluminescence Quantum Yield and Efficient Red Light-Emitting Diodes
journal, December 2017

Surface Chemistry Matters. How Ligands Influence Excited State Interactions between CsPbBr ₃ and Methyl Viologen
journal, May 2020

Principles of Fluorescence Spectroscopy
book, January 2006

Perspectives on the Physical Chemistry of Semiconductor Nanocrystals
journal, January 1996

Metal Semiconductor Heterostructures for Photocatalytic Conversion of Light Energy
journal, March 2015

Core–Shell CsPbBr ₃ @CdS Quantum Dots with Enhanced Stability and Photoluminescence Quantum Yields for Optoelectronic Devices
journal, July 2020

Ultrafast Interfacial Electron and Hole Transfer from CsPbBr ₃ Perovskite Quantum Dots
journal, September 2015

State of the Art and Prospects for Halide Perovskite Nanocrystals
journal, June 2021

Effect of Surface Ligand on Charge Separation and Recombination at CsPbI ₃ Perovskite Quantum Dot/TiO ₂ Interfaces
journal, August 2019

The Surface Chemistry and Structure of Colloidal Lead Halide Perovskite Nanocrystals
journal, January 2021

New understanding on the different photocatalytic activity of wurtzite and zinc-blende CdS
journal, September 2016

Water resistant CsPbX ₃ nanocrystals coated with polyhedral oligomeric silsesquioxane and their use as solid state luminophores in all-perovskite white light-emitting devices
journal, January 2016

A Nanocrystal Catalyst Incorporating a Surface Bound Transition Metal to Induce Photocatalytic Sequential Electron Transfer Events
journal, July 2021

Complete ultrafast charge carrier dynamics in photo-excited all-inorganic perovskite nanocrystals (CsPbX ₃ )
journal, January 2017

Ultrafast Exciton Dynamics in Colloidal CsPbBr ₃ Perovskite Nanocrystals: Biexciton Effect and Auger Recombination
journal, February 2017

Perovskite Photocatalysis. Methyl Viologen Induces Unusually Long-Lived Charge Carrier Separation in CsPbBr ₃ Nanocrystals
journal, December 2019

CsPbBr ₃ /ZnS Core/Shell Type Nanocrystals for Enhancing Luminescence Lifetime and Water Stability
journal, May 2020

Photocatalysis with CdSe Nanoparticles in Confined Media: Mapping Charge Transfer Events in the Subpicosecond to Second Timescales
journal, February 2009

Highly stable, luminescent core–shell type methylammonium–octylammonium lead bromide layered perovskite nanoparticles
journal, January 2016

Probing Perovskite Photocatalysis. Interfacial Electron Transfer between CsPbBr ₃ and Ferrocene Redox Couple
journal, September 2019

Solar-Driven Metal Halide Perovskite Photocatalysis: Design, Stability, and Performance
journal, March 2020

On the crystal structure of colloidally prepared CsPbBr ₃ quantum dots
journal, January 2016

Photoelectrochemistry in particulate systems. 4. Photosensitization of a titanium dioxide semiconductor with a chlorophyll analog
journal, March 1986

Highly Luminescent Monodisperse CdSe and CdSe/ZnS Nanocrystals Synthesized in a Hexadecylamine−Trioctylphosphine Oxide−Trioctylphospine Mixture
journal, April 2001

Quantum Dot Sensitized Solar Cells. A Tale of Two Semiconductor Nanocrystals: CdSe and CdTe
journal, May 2009

Efficient and Stable Luminescence from Mn ²⁺ in Core and Core–Isocrystalline Shell CsPbCl ₃ Perovskite Nanocrystals
journal, May 2017

Metal halide perovskite nanomaterials: synthesis and applications
journal, January 2017

Photocatalytic and Photoelectrochemical Degradation of Organic Compounds with All-Inorganic Metal Halide Perovskite Quantum Dots
journal, January 2019

Enhanced Stability and Tunable Photoluminescence in Perovskite CsPbX ₃ /ZnS Quantum Dot Heterostructure
journal, April 2017

CdSe/CdS Nanorod Photocatalysts: Tuning the Interfacial Charge Transfer Process through Shell Length
journal, July 2015

Challenges and Opportunities in Designing Perovskite Nanocrystal Heterostructures
journal, June 2020

Efficient and Selective Photocatalytic Oxidation of Benzylic Alcohols with Hybrid Organic–Inorganic Perovskite Materials
journal, February 2018

All Inorganic Halide Perovskites Nanosystem: Synthesis, Structural Features, Optical Properties and Optoelectronic Applications
journal, January 2017

Synthesis and Micrometer-Scale Assembly of Colloidal CdSe/CdS Nanorods Prepared by a Seeded Growth Approach
journal, October 2007

Semiconductor Surface Chemistry as Holy Grail in Photocatalysis and Photovoltaics
journal, March 2017

Novel B-site Cd2+ doped CsPbBr3 quantum dot glass toward strong fluorescence and high stability for wLED
journal, September 2020

Strongly emissive perovskite nanocrystal inks for high-voltage solar cells
journal, December 2016

Switchable Anion Exchange in Polymer-Encapsulated APbX ₃ Nanocrystals Delivers Stable All-Perovskite White Emitters
journal, July 2021

Ultrafast Charge Separation in Two-Dimensional CsPbBr 3 Perovskite Nanoplatelets
journal, January 2019

Facile Synthesis of ZnS−AgInS ₂ Solid Solution Nanoparticles for a Color-Adjustable Luminophore
journal, October 2007

Mechanistic Understanding and Rational Design of Quantum Dot/Mediator Interfaces for Efficient Photon Upconversion
journal, November 2020

Metal Halide Perovskite Nanocrystals: Synthesis, Post-Synthesis Modifications, and Their Optical Properties
journal, February 2019

Synthesis and Properties of Biocompatible Water-Soluble Silica-Coated CdSe/ZnS Semiconductor Quantum Dots ^†
journal, September 2001

Mechanism of Efficient Viologen Radical Generation by Ultrafast Electron Transfer from CdS Quantum Dots
journal, March 2018

Nanocrystals of Cesium Lead Halide Perovskites (CsPbX ₃ , X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut
journal, February 2015

Synthesis of highly luminescent wurtzite CdSe/CdS giant-shell nanocrystals using a fast continuous injection route
journal, January 2014

Luminescence Photophysics in Semiconductor Nanocrystals
journal, November 1998